Author: "KATAN, Claudine" / Publisher: hal ccsd - Searchworks@Jio Institute Digital Library Search Results

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210 results on '"KATAN, Claudine"'

1. Tight-binding modelling of layered halide perovskites

Author: Thébaud, Simon, Cucco, Bruno, Quarti, Claudio, Volonakis, George, Pedesseau, Laurent, Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), and ANR-22-MER3-0006,PHANTASTIC,PHysics- and dAta-driven multiscale modelling desigN of layered lead halide perovskiTe mAterials for Stable phoTovoltaICs(2022)
Subjects: [PHYS]Physics [physics]
Abstract: International audience; In recent years, layered heterostructures of halide perovskites have emerged as promising optoelectronic systems due to their tunability and to the presence of strong excitonic effects [1], with potential applications for efficient light emission, spintronics, single-photon emission and photonic logic. This last technology is being developped by the H2020 POLLOC (polariton logic) consortium using exciton-polariton devices. From the theoretical point of view, first-principles studies of exciton physics in layered halide pervoskites are possible [2] but severely constrained by system size. To go beyond this limitation, symmetry-based semi-empirical tight-binding models have provided an efficient description of the electronic structure and optical properties of bulk halide perovskites [3-5]. In this talk, we will discuss such models and their extension to the case of layered perovskites, a stepping stone towards a robust description of excitons in these compounds within the tight-binding framework [6,7].[1] J.-C. Blancon et al., Nature Comm. 9, 2254 (2018) [2] C. Quarti et al., Adv. Optical Mater. 2023, 2202801[3] S. Boyer-Richard et al., J. Phys. Chem. Lett. 7, 3833 (2016)[4] A. Marronnier et al., ACS Nano 12, 3477 (2018)[5] Z. Wei et al., Nature Comm. 10, 5342 (2019) [6] R. Benchamekh et al., Phys. Rev. B 91, 045118 (2015)[7] Y. Cho et al., Phys. Chem. Lett. 10, 6189 (2019)This work was supported by the M-ERANET grant PHANTASTIC Call 2021.
Published: 2023

2. Towards deeper and more complete theoretical understanding of optical properties of perovskite nanocrystals

Author: Nguyen, Thi Phuc Tan, Katan, Claudine, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA), and European Project: 899141,PoLLoC
Subjects: Nanoparticle NP, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Perovskites
Abstract: International audience
Published: 2023

3. Halide perovskites beyond methylammonium lead iodide for more than optoelectronics

Author: Cucco, Bruno, Katan, Claudine, Volonakis, George, Even, Jacky, Kepenekian, Mikaël, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018)
Subjects: [CHIM]Chemical Sciences
Abstract: International audience
Published: 2023

4. Symmetry-informed tight-binding modeling of disordered hybrid perovskites

Author: Thébaud, Simon, Quarti, Claudio, Volonakis, George, Kepenekian, Mikaël, Pedesseau, Laurent, Katan, Claudine, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and ANR-22-MER3-0006,PHANTASTIC,PHysics- and dAta-driven multiscale modelling desigN of layered lead halide perovskiTe mAterials for Stable phoTovoltaICs(2022)
Subjects: [PHYS]Physics [physics]
Abstract: International audience; In the past decade, hybrid halide perovskites have generated tremendous interest as optoelectronic materials, particularly for photovoltaïc applications due to impressive conversion efficiency values reaching over 25% in only a few years. Their large-scale industrial application, however, depends on subsequent improvements of their stability and tunability that can be achieved in both halide solid solutions (in which I, Br and Cl anions are mixed on a disordered sublattice) and two-dimensional halide perovskites (in which charge carriers are confined within inorganic atomic layers separated by organic spacers) [1,2]. Thus, it is crucial to gain an understanding of the electronic properties and carrier transport in these systems. In this talk, I will describe how a model tight-binding Hamiltonian can be extended from the archetypal CH3NH3PbI3 bulk perovskite [3-5] to mixed halide perovskites and two-dimensional perovskites using a combination of symmetry considerations and DFT calculations. This will pave the way towards a robust theoretical treatment of halide clustering effects in the former, and towards a proper description of the excitonic fine structure in the latter.[1] V Diez-Cabanes et al., Adv. Optical Mater 2001832 (2021).[2] S. Sidhik et al., Science 377, 1425 (2022)[3] S. Boyer-Richard et al., J. Phys. Chem. Lett. 7, 3833 (2016)[4] A. Marronnier et al., ACS Nano 12, 3477 (2018)[5] Z. Wei et al., Nature Communications 10, 5342 (2019)This work was supported by the M-ERANET grant PHANTASTIC Call 2021.
Published: 2023

5. Metal halide perovskites and their interfaces: current issues and recent advances

Author: Even, Jacky, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges financial support from the Institute Universitaire de France. This research received funding from the European Union’s Horizon 2020 research and innovation program, through an Innovation Action under the grant agreement No. 861985 (PeroCUBE) and a FET Open action under the grant agreement No. 899141 (PoLLoC)., European Project: 899141,PoLLoC, European Project: PeroCUBE, KATAN, Claudine, Polariton logic - PoLLoC - 899141 - INCOMING, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, solar cells, LED, perovskites, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], DFT, [PHYS.COND] Physics [physics]/Condensed Matter [cond-mat]
Abstract: The considerable attention paid to metal halide perovskites (MHP) in recent years led to several scientific and technological advances, among which the creation of a new photovoltaic (PV) technology that competes with the most widespread ones[1]. With the ever-increasing diversity of applications explored, the need for fundamental understanding persists and may be gained either by smart and simple experimental protocols or models, or else via complex set-ups and computationally expensive ab-initio calculations.At present, MHP materials used in devices are frequently far from their ideal bulk structure, which hinders the use of state-of-the-art first principles simulations including many-body effects and calls for the design of dedicated models. For PV and LEDs, they are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability and/or defectiveness as well as assembled with carrier selective layers. On the other hand, colloidal MHP nanocrystals are promising for devices exploiting both weak and strong light-matter interactions, such as lasers, single photon emitters if not all-optical logic gates. After a general introduction on MHPs, the talk will bring up some of the hot topics in the field and will summarize recent results obtained by the group in Rennes in collaboration with our partners from France and abroad[2-6]. References : [1] https://www.nrel.gov/pv/cell-efficiency.html and https://www.nrel.gov/pv/module-efficiency.html.[2] W. Li et al., Light-activated interlayer contraction in two-dimensional perovskites for high-efficiency solar cells, Nature Nanotechnology, 17, 45 (2022)[3] B. Traore et al., A theoretical framework for microscopic surface and interface dipoles, work functions and valence band alignments in 2D and 3D halide perovskite heterostructures, ACS Energy Lett. 7, 349 (2022) [4] B. Traore et al., Band gap and energy level alignment of 2D and 3D halide perovskites using DFT-1/2, Phys. Rev. Materials, 6, 014604 (2022)[5] S. Sidhik et al., Deterministic fabrication of 3D|2D 1 perovskite bilayer 2 stacks for durable and efficient solar cells, accepted. [6] Q. Akkerman, et al., Taming the nucleation and growth kinetics of lead halide perovskite quantum dots, https://doi.org/10.21203/rs.3.rs-1236393/v1
Published: 2022

6. 2D multilayered perovskites and 2D/3D bilayers for stable solar cells

Author: Even, Jacky, Sidhik, Siraj, Katan, Claudine, Kanatzidis, Mercouri, Mohite, Aditya, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Northwestern University [Evanston]
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: International audience
Published: 2023

7. Interfacial engineering to modulate surface dipoles, work functions and dielectric confinement of halide perovskites

Author: Basera, Pooja, Traore, Boubacar, Even, Jacky, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledgesthe financial support from the Institut Universitaire de France. This work was granted access tothe HPC resources of TGCC under the allocations 2021-A0110907682 and 2022-A0110907682made by GENCI., European Project: 899141,PoLLoC, and European Project: PeroCUBE
Subjects: [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: Authors are grateful to Maksym Kovalenko and Andriy Stelmakh for useful discussions and providing the MD snapshots.; International audience; The interfacial properties between perovskite photoactive and charge transport layers are critical for device performance and operational stability. Therefore, an accurate theoretical description of the link between surface dipoles and work functions is of scientific and practical interest. We show that for a CsPbBr 3 perovskite surface functionalized by dipolar ligand molecules, the interplay between surface dipoles, charge transfers, and local strain effects leads to upward or downward shifts of the valence level. We further demonstrate that the contribution of individual molecular entities to the surface dipoles and electric susceptibilities are essentially additive. Finally, we compare our results to those predicted from conventional classical approaches based on a capacitor model that links the induced vacuum level shift and the molecular dipole moment. Our findings identify recipes to fine-tune materials work functions that provide valuable insights into the interfacial engineering of this family of semiconductors.
Published: 2023
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8. Surfaces/interfaces in atomic-scale semiconductor devices: structural and electronic properties of Pb-free perovskites and charge transport materials

Author: Pedesseau, Laurent, Jiang, Pingping, Traore, Boubacar, Kepenekian, Mikaël, Katan, Claudine, Volonakis, George, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and European Project: 862656,DROP-IT
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: International audience; Halide perovskites have captivated the research community over the past decade mainly in the photovoltaic field as a new generation of absorber materials for high-efficiency and low-cost solar cells. Nowadays, the power conversion efficiency (PCE) is reaching 25.7% for single cells and 31.3% for Perovskite/Si tandem cells. Moreover, halide perovskites exhibit attractive potential for Lasers, LEDs, Photodetectors, Photocatalysis. Nevertheless, despite promising low manufacturing costs, short payback time and abundant material resources, the potential industrial use of halide perovskites is still be hampered by toxicity issues, device stability and upscaling. Researchers are also looking for alternative materials related to the substitution of Pb by Sn in standard halide perovskite structures, double perovskite structures, perovskite-like structures or even non-perovskite structures such as rudorfittes. Importantly, the low-bandgap Pb-Sn alloyed perovskite allows the building of all-perovskite tandem solar cells that shall overcome the performances of single-junction perovskite cells. In fact, of all possible means to improve perovskite film quality and suppress nonradiative recombination in optoelectronic devices for a high photo conversion efficiency purpose, the surface and interface functionalizations after the assembly with charge transport layer (CTL) are one of the most critical parameters . In view of the sophisticated chemical and physical properties of Sn-based perovskites, theoretical calculations based on density functional theory (DFT) may provide a useful insight into the interplay between absorbers and CTLs. Here, FASnI3 is chosen as a benchmark material. We thoroughly investigate the influence of its surface termination on structural and electronic properties when interfacing with organic C60 (100) and inorganic SnO2 (100) and (110), including the intermediate work function calculations on the free-standing slabs. Based on the theoretical methology developed in our team, we have evidenced the proportionality between work function shifts and surface dipoles, providing an additional microscopic insight into interfacial properties in lead-free heterostructures.
Published: 2022
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9. Recent results on metal halide perovskites and their interfaces*

Author: Traore, Boubacar, Quarti, Claudio, Jiang, Junke, Pedesseau, Laurent, Volonakis, George, Kepenekian, Mikael, Even, Jacky, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Mons [Belgium] (UMONS), This research received funding from the European Union’s Horizon 2020 program, through and Innovation Action under the grant agreement No. 861985 (PeroCUBE). J.E. acknowledges the Institut Universitaire de France., European Project: PeroCUBE, KATAN, Claudine, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], [PHYS.COND] Physics [physics]/Condensed Matter [cond-mat]
Abstract: International audience; The considerable attention paid to metal halide perovskites (MHP) in recent years led to several scientific and technological advances. This in turn raised important questions that currently challenge the limits of available theoretical techniques and atomistic models. At present, perovskite materials are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability and/or defectiveness as well as assembled with carrier selective layers, other materials and components to turn them into devices. Considering the target applications, ambient conditions predominate with additional issues related, for example, to the intrinsic dynamics in action in the MHP structure that may not be well captured using static averaged structures.Based on a set of customized examples, this talk will summarize recent theoretical results obtained by our group that aimed at answering questions such as: i) How do these engineering strategies impact the work function and absolute valence band energy of the MHP material? ii) Is it correlated with surface/interface dipoles? iii) Can one quantitatively assess energy level alignments of MHP semiconductors based on first-principles electronic structure calculations? How can one get rid of the stochastic dynamics of organic cations and further include cation and anion alloying while computing materials properties? iv) Is it possible to extract semi-empirical formula for molecular passivation at surface or transitivity rules for interface dipoles? Special attention will be paid on newly discovered phases and compositions and opportunities to further engineer MHP properties in connection with their use in devices under working conditions.*This research received funding from the European Union’s Horizon 2020 program, through and Innovation Action under the grant agreement No. 861985 (PeroCUBE). J.E. acknowledges the Institut Universitaire de France.
Published: 2022

10. Excitonic Properties of Vacancy Ordered Halide Double Perovskites: From Wannier to Frenkel excitons

Author: Cucco, Bruno, Katan, Claudine, Even, Jacky, Kepenekian, Mikaël, Volonakis, George, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and European Project: 862656,DROP-IT
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Over the past decade ABX3 halide perovskites based on Pb have emerged as a most-promising class of materials. To-date they have been employed for record-breaking solar-cells, highly-efficient lightemitters, new photo-catalysts and even as X-ray detectors. A2BX6 vacancy ordered doubleperovskites (VODP) are air-stable and environmentally friendly (Pb-free) that have been proposed as alternatives, to halide perovskites. Yet, VODP materials have not achieve the high performance of their Pb-based counterparts. In this work, we thoroughly analyze the properties of the VODP family of materials by employing state-of-art ab initio calculations to unveil the key details of the electronic structure and the effects of electron-hole coupling on the optical properties.
Published: 2022

11. Non-Equilibrium Lattice Dynamics in Photo-Excited Two-Dimensional Perovskites

Author: Cuthriell, Shelby, Panuganti, Shobhana, Laing, Craig, Quintero, Michael, Guzelturk, Burak, Yazdani, Nuri, Traore, Boubacar, Brumberg, Alexandra, Malliakas, Christos, Lindenberg, Aaron, Wood, Vanessa, Katan, Claudine, Even, Jacky, Zhang, Xiaoyi, Kanatzidis, Mercouri, Schaller, Richard, Department of Chemistry [Northwestern University], Northwestern University [Evanston], Argonne National Laboratory [Lemont] (ANL), SLAC National Accelerator Laboratory (SLAC), Stanford University, Department of Information Technology and Electrical Engineering, ETH Zurich, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges financial support from the Institute Universitaire de France. This work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2020-A0100911434 and 2020-A0090907682 made by GENCI., and European Project: PeroCUBE
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, lead halide perovskites, transient structures, optical excitation
Abstract: International audience; Interplay between structural and photophysical properties of metal halide perovskites is critical to their utility in optoelectronics, but there is limited understanding of lattice response upon photoexcitation. Here, 2D perovskites butylammonium lead iodide, (BA) PbI , and phenethylammonium lead iodide, (PEA) PbI , are investigated using ultrafast transient X-ray diffraction as a function of optical excitation fluence to discern structural dynamics. Both powder X-ray diffraction and time-resolved photoluminescence linewidths narrow over 1 ns following optical excitation for the fluence range studied, concurrent with slight redshifting of the optical bandgaps. These observations are attributed to transient relaxation and ordering of distorted lead iodide octahedra stimulated mainly by electron-hole pair creation. The c axis expands up to 0.37% over hundreds of picoseconds; reflections sampling the a and b axes undergo one tenth of this expansion with the same timescale. Post-photoexcitation appearance of the (110) reflection in (BA) PbI would suggest a transient phase transition, however, through new single-crystal XRD, reflections are found that violate glide plane conditions in the reported Pbca structure. The static structure space group is reassigned as P2 2 2 . With this, a nonequilibrium phase transition is ruled out. These findings offer increased understanding of remarkable lattice response in 2D perovskites upon excitation.
Published: 2022
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12. Unusual anharmonicity and pseudospin-phonon dynamics in 3D halide perovskites

Author: Even, Jacky, Hehlen, Bernard, Bourges, Philippe, Rufflé, Benoit, Létoublon, Antoine, Zacharias, Marios, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Charles Coulomb (L2C), Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and European Project: 899141,PoLLoC
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: International audience; 3D halide perovskites used in light emitters and PV systems exhibit an unusual anharmonicity, which is not accounted for in nowadays descriptions of phonons and electron-phonon coupling. Therefore, the low frequency lattice vibrations and relaxations were investigated in single crystals of the four 3D hybrid organolead perovskites, MAPbBr3, FAPbBr3, MAPbI3, and FAPbI3, at the Brillouin zone center using Raman and Brillouin scattering and at the zone boundary using inelastic neutron scattering. The temperature dependence of the PbX6 lattice modes in the four compounds can berenormalized into universal curves and no soft vibration is observed excluding a displacive-like transitional dynamics related to structural phase transitions. The reorientational (pseudospin) motions of the molecular cations exhibit a seemingly order-disorder character recalling that of plastic crystals, but attributed to a secondary order-parameter. At ultra-low frequency, a quasi-elastic component evidenced by Brillouin scattering and associated to the unresolved central peak observed in neutron scattering, is attributed to center of mass anharmonic motions and rattling of the molecular cations in the perovskite cavities. 3D halide perovskites are therefore in a very unusualsituation where anharmonicity prevails. It is leading to partial, extensive and ultraslow critical and stochatic dynamics connected to structural instabilities. The extensive disorder of the lattice at normal operation temperatures for devices is similar to premelting where only long-range acoustic normal modes survive.
Published: 2022

13. Controlling the nucleation and growth kinetics of lead halide perovskite quantum dots

Author: Akkerman, Quinten A., Nguyen, Tan P. T., Boehme, Simon C., Montanarella, Federico, Dirin, Dmitry N., Wechsler, Philipp, Beiglböck, Finn, Rainò, Gabriele, Erni, Rolf, Katan, Claudine, Even, Jacky, Kovalenko, Maksym V., Department of Chemistry and Applied Biosciences [ETH Zürich] (D-CHAB), Eidgenössische Technische Hochschule - Swiss Federal Institute of Technology [Zürich] (ETH Zürich), Swiss Federal Laboratories for Materials Science and Technology [Dübendorf] (EMPA), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Swiss Federal Laboratories for Materials Science and Technology [St Gallen] (EMPA), Electron Microscopy Center, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges financial support from the Institute Universitaire de France., and European Project: 899141,PoLLoC
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Multidisciplinary
Abstract: Colloidal lead halide perovskite nanocrystals are of interest as photoluminescent quantum dots (QDs) whose properties depend on the size and shape. They are normally synthesized on subsecond time scales through hard-to-control ionic metathesis reactions. We report a room-temperature synthesis of monodisperse, isolable, spheroidal APbBr 3 QDs (“A” indicates cesium, formamidinium, and methylammonium) that are size tunable from 3 to >13 nanometers. The kinetics of both nucleation and growth are temporally separated and substantially slowed down by the intricate equilibrium between the precursor (PbBr 2 ) and the A[PbBr 3 ] solute, with the latter serving as a monomer. QDs of all these compositions exhibit up to four excitonic transitions in their linear absorption spectra, and we demonstrate that the size-dependent confinement energy for all transitions is independent of the A-site cation.
Published: 2022
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14. Lattice dynamics in 3D lead halide hybrid perovskites

Author: Even, Jacky, Hehlen, Bernard, Bourges, Philippe, Létoublon, Antoine, Rufflé, Benoit, Ecolivet, Claude, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Charles Coulomb (L2C), Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Technical University of Munich - Institute for Advanced Study, European Project: PeroCUBE, and European Project: 899141,PoLLoC
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: International audience; Lattice dynamics in 3D lead halide hybrid perovskites is analyzed together with the possible consequences for device applications
Published: 2022

15. Synergic experimental and theoretical study of the ss-NMR response of halide perovskites: mixed and layered halide perovskites as test bed

Author: Quarti, Claudio, Dittmer, Jens, Mercier, Nicolas, Furet, Eric, Katan, Claudine, KATAN, Claudine, APPEL À PROJETS GÉNÉRIQUE 2018 - Cellules solaires perovskite plus stables et à teneur réduite en plomb. - - MORELESS2018 - ANR-18-CE05-0026 - AAPG2018 - VALID, University of Mons [Belgium] (UMONS), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), MOLTECH-Anjou, Université d'Angers (UA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: Computational investigations were conducted thanks to HPC resources provided by [TGCC/CINES/IDRIS] under the allocation 2020-A0010907682 made by GENCI.; International audience; Halide perovskites and related nanostructures show complex structural interplay between well-defined long-range structural order, associated to their corner-shared MX6 organization, and short-range dynamic disorder, due to the soft nature of the lattice, libration motion and conformational freedom of the organic component. The structural characterization of these materials reveals therefore challenging, as it calls for an appropriate description of both short-range and long-range structural features, then requiring a smart combination of different structural investigation techniques. In this frame, solid state Nuclear Magnetic Resonance (ss-NMR) emerges as unique technique to complement long-range description routinely addressed via X-ray diffraction, to probe the material structure at different scales[1].We perform ss-NMR characterization of halide perovskites adopting synergic experimental and theoretical tools. The ss-NMR of 3D methylammonium lead halide perovskites is investigated, first, via periodic Density Functional Theory (DFT) simulations, with good match between the theoretical results for 1H and 13C nuclei and the experimental literature data. Theoretical/experimental agreement is comparably less accurate for 207Pb nuclei, due to lack of Spin-Orbit-Coupling (SOC) in our computational set-up, but still provides correct trends with respect to the PbX6 octahedra halide composition, hence making the NMR signature of 207Pb the ideal marker for characterizing halide segregation down to the atomic scale.[2] Further investigations involve a recently synthesized terminated, m=3 halide perovskite. Again, ssNMR of 207Pb nicely distinguishes between the lead atoms in the inner and outer layers.[3] Further efforts in the directions of incorporation of SOC in the computational set-up and better framing of thermal narrowing is needed but the present results highlight the potential of joint theoretical/experimental NMR simulations in the field of halide perovskites for energy conversion applications.[1] Dahlman C. J., Kubicki D. J., Reddy G. N. M., Interfaces in metal halide perovskites probed by solid-state NMR spectroscopy, J. Mater. Chem. A, 2021,9, 19206[2] Quarti C., Furet E., Katan C., DFT simulations as valuable tool to support NMR characterization of halide perovskites: the case of pure and mixed halide perovskites, Helv. Chim. Acta 2021, 104, e2000231.[3] M. Ben Haj Salah, N. Mercier, M. Allain, A. Leblanc, J. Dittmer, C. Botta, C. Quarti, C. Katan, Synthesis and characterization of (FA)3(HEA)2Pb3I11: a rare example of -oriented multilayered halide perovskite, accepted in Chemistry of Materials.
Published: 2022

16. Are Styrylpyrimidines dyes promising candidates for TADF ?

Author: Hodée, Maxime, Massue, Julien, Achelle, Sylvain, Fihey, Arnaud, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Hodée, Maxime
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: International audience
Published: 2022

17. Synthesis and Characterization of (FA)3(HEA)2Pb3I11: A Rare Example of <1 1 0>-Oriented Multilayered Halide Perovskites

Author: Ben Haj Salah, Maroua, Mercier, Nicolas, Allain, Magali, Leblanc, Antonin, Dittmer, Jens, Botta, Chiara, Quarti, Claudio, Katan, Claudine, MOLTECH-Anjou, Université d'Angers (UA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Istituto di Scienze e Tecnologie Chimiche 'Giulio Natta' (SCITEC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), and ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: For DFT calculations, this work was granted access to the HPC resources of TGCC/CINES/IDRIS under the allocation 2020-A0090907682 made by GENCI; International audience; Metal-halide perovskites have recently demonstrated great potential for a wide variety of optoelectronic applications, with their layered subfamily offering improved stability as compared to their 3D analogs. Among the layered compounds, subclass of terminated compounds are currently dominating the field, while subclass is comparably much less explored. Here we report on the synthesis of (FA) 3 (HEA) 2 Pb 3 I 11 obtained by room-temperature liquid-gas diffusion involving the intermediate-size cation hydroxyethylammonium (HEA +), formamidinium (FA +) and PbI 2 dissolved in an acidic solution. This multilayered hybrid perovskite is a rare example of a m= 3 member of the -oriented series (A') 2 (A) m B m X 3m+2. Structural characterization based on X-ray diffraction and NMR investigations reveals that the small size cation FA + is located both in the inner layer of the perovskite sheet, but also in the interlayer space, while the intermediate-size cation HEA + is situated in the outer cavities of the perovskite sheet. (FA) 3 (HEA) 2 Pb 3 I 11 exhibits a broad absorption band in the visible region (400-650 nm) leading to an optical band gap of 1.96 eV. Electronic structure calculations confirm the direct nature of the band gap and evidence sizeable inter layer electronic coupling related to short I…I distances. These features are reminiscent of those observed for -oriented Pb 3 I 10 analogs that have shown photovoltaic efficiencies over 18%. These findings should prompt further investigations for the design of other -oriented multilayered (m= 3, 4,…) metal halide perovskites.
Published: 2022
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18. Tuning the properties of multilayered perovskites and their interfaces for optoelectronic applications

Author: Even, Jacky, Traore, Boubacar, Quarti, Claudio, Jiang, Junke, Pedesseau, Laurent, Volonakis, Yorgos, Kepenekian, Mikaël, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), and European Project: PeroCUBE
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; The presentation will focus on the interplay between structural, interfacial and optoelectronic properties in 2D multilayered halide perovskites, either in Ruddlesden Popper (RP) or Dion Jacobson (DJ) structure. At present, perovskite materials are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability and/or defectiveness as well as assembled with carrier selective layers, other materials and components to turn them into devices. Considering the target applications, ambient conditions predominate with additional issues related, for example, to the intrinsic dynamics in action in the MHP structure that may not be well captured using static averaged structures.Based on a set of customized examples, this talk will summarize recent theoretical results obtained by our group that aimed at answering questions such as: i) How do these engineering strategies impact the work function and absolute valence band energy of the MHP material? ii) Is it correlated with surface/interface dipoles? iii) Can one quantitatively assess energy level alignments of MHP semiconductors based on first-principles electronic structure calculations? How can one get rid of the stochastic dynamics of organic cations and further include cation and anion alloying while computing materials properties? iv) Is it possible to extract semi-empirical formula for molecular passivation at surface or transitivity rules for interface dipoles?Special attention will be paid on newly discovered phases and compositions and opportunities to further engineer MHP properties in connection with their use in devices under working conditions. We will see that in practical cases the funneling of electronic carriers to the 2D crystal edges, important for ionization of electron-hole pairs in 2D RP phases, is also at work in bromide perovskites. Continuous and ultrafast photodoping will be further discussed, demonstrating their strong impact on the structural and carrier transport properties of DJ perovskites
Published: 2022

19. Unveiling surface and interface properties of Pb-free perovskites from atomicscale simulation for thin-film device applications

Author: Pedesseau, Laurent, Jiang, Pingping, Traore, Boubacar, Kepenekian, Mikaël, Katan, Claudine, Volonakis, George, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and PEDESSEAU, Laurent
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.PHYS]Physics [physics]/Physics [physics], [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [PHYS.PHYS] Physics [physics]/Physics [physics], [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract: International audience
Published: 2022

20. Pseudospin-phonon dynamics in lead halide hybrid perovskites

Author: Even, Jacky, Hehlen, Bernard, Bourges, Philippe, Ruffle, Benoit, Katan, Claudine, Létoublon, Antoine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA), Laboratoire Charles Coulomb (L2C), Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM), LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], Condensed Matter::Materials Science, [CHIM]Chemical Sciences, Condensed Matter::Strongly Correlated Electrons
Abstract: International audience; The low frequency lattice vibrations and relaxations are investigated in single crystals of the four 3Dhybrid organolead perovskites, MAPbBr3, FAPbBr3, MAPbI3, and FAPbI3, at the Brillouin zone centerusing Raman and Brillouin scattering and at the zone boundary using inelastic neutron scattering. Thetemperature dependence of the PbX6 lattice modes in the four compounds can be renormalized intouniversal curves and no soft vibration is observed excluding a displacive-like transitional dynamics. Thereorientational (pseudospin) motions of the molecular cations exhibit a seemingly order-disordercharacter recalling that of plastic crystals, but attributed to a secondary order-parameter. At ultra-lowfrequency, a quasi-elastic component evidenced by Brillouin scattering and associated to the unresolvedcentral peak observed in neutron scattering, is attributed to center of mass anharmonic motions andrattling of the molecular cations in the perovskite cavities.
Published: 2022

21. A theoretical framework for microscopic surface and interface dipoles, work functions and valence band alignments in 2D and 3D halide perovskite heterostructures

Author: Traoré, Boubacar, Basera, Pooja, Ramadan, Alexandra J., Snaith, Henry J., Katan, Claudine, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Oxford, Clarendon Laboratory [Oxford], J.E. acknowledges financial support from the Institute Universitaire de France., European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), and University of Oxford [Oxford]
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Fuel Technology, Renewable Energy, Sustainability and the Environment, Chemistry (miscellaneous), Materials Chemistry, Energy Engineering and Power Technology, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 0210 nano-technology, 01 natural sciences, 0104 chemical sciences
Abstract: The work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2020-A0100911434 and 2020-A0090907682 made by GENCI.; International audience; We propose a computational methodology that highlights the intimate connection between surface and interface dipoles and work functions or valence band alignments. We apply the methodology to inspect the energy level alignments of halide perovskites and explore various situations relevant to perovskite-based heterostructures: i) the effect of surface termination, the ability to fine-tune and interpret the shift in energy alignments via ii) surface coating and iii) surface functionalization and/or passivation with molecules. We highlight the importance of local strain relaxation at the surfaces or interfaces, and revisit classical approaches based on capacitor models. Finally, we show that surface dipoles are additive in heterostructures and illustrate it through a 2D/3D perovskite interface. This provides a handy tool to interpret band alignments in complex perovskite-based heterostructures and buried interfaces. The scope of our work goes far beyond halide perovskites and can be useful to scrutinize the surfacial and interfacial behaviors of other semiconductors and heterojunctions. It allows bridging results from atomistic ab initio calculations and classical simulation approaches for multilayered thin film devices.
Published: 2022
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22. From bulk, to surface and interface properties of unusual semiconductors at the atomic scale to promising devices

Author: Pedesseau, Laurent, Jiang, Pingping, Traore, Boubacar, Kepenekian, Mikaël, Katan, Claudine, Volonakis, George, Even, Jacky, PEDESSEAU, Laurent, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.PHYS]Physics [physics]/Physics [physics], [SPI.NANO] Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [PHYS.PHYS] Physics [physics]/Physics [physics], [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract: International audience
Published: 2022

23. Importance of disorder and lattice anharmonicity on the exciton fine structure and exciton-phonon coupling in halide perovskite nanocrystals for light emission

Author: Even, Jacky, Tamarat, Philippe, Bourges, Philippe, Roma, Guido, Zacharias, Marios, Nguyen, Tan, Katan, Claudine, Rainò, Gabriele, Bodnarchuk, Maryna, Lounis, Brahim, Kovalenko, Maksym, even, jacky, Polariton logic - PoLLoC - 899141 - INCOMING, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Photonique, Numérique et Nanosciences (LP2N), Université de Bordeaux (UB)-Institut d'Optique Graduate School (IOGS)-Centre National de la Recherche Scientifique (CNRS), CEA- Saclay (CEA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Swiss Federal Laboratories for Materials Science and Technology [Dübendorf] (EMPA), Institute of Inorganic Chemistry, ETH Zürich, and European Project: 899141,PoLLoC
Subjects: [PHYS]Physics [physics], [PHYS] Physics [physics]
Abstract: National audience; Halide perovskite nanocrystals are a promising route to efficient light emitting devices, and more recently as potential single photon emitters. Their radiative recombinations are governed by excitons. The bright or dark character of the ground state is debated. A Rashba effect correlated with a local polarization was proposed in 2018 as a general mechanism for inversion of bright and dark level ordering. But direct spectroscopic signatures of the dark exciton emission in the low-temperature photoluminescence of single FAPbBr3 and CsPbI3 nanocrystals under magnetic fields rather yield a dark singlet below the bright triplet. The dark-bright splitting values are in fair agreement with numerical estimations of the long-range electron–hole exchange interaction. The intense luminescence of perovskite nanocrystals is alternatively attributed to a reduced bright-to-dark phonon-assisted relaxation. The phonon side bands in nanocrystals match neutron scattering phonon spectroscopy results obtained at low temperature. More, a recent classification of 3D perovskites into ferroelectric or hyperferroelectric materials, points toward the role of the depolarization effect for the reduction of a spontaneous polarization in nanocrystals. The role of lattice disorder and the strong anharmonicity of the lattice is however far from being well-understood.[1] P. Tamarat, J.-B. Trebbia, M. I. Bodnarchuk, R. Erni, M. V. Kovalenko, J. Even & B. Lounis, The ground exciton state of formamidinium lead bromide perovskite nanocrystals is a singlet dark state. Nature Materials 18, 717–724 (2019).[2] P. Tamarat, L. Hou, J.-B. Trebbia, A. Swarnkar, L. Biadala, Y. Louyer, M. I. Bodnarchuk, M. V. Kovalenko, J. Even, B. Lounis, The dark exciton ground state promotes photon-pair emission in individual perovskite nanocrystals, Nature Comm. 11, 6001 (2020)[3] A. Ferreira, S. Paofai, A. Létoublon, J. Ollivier, S. Raymond, B. Hehlen, B. Rufflé, S. Cordier, C. Katan, J. Even & P. Bourges, Direct evidence of weakly dispersed and strongly anharmonic optical phonons in hybrid perovskites, Comm. Phys. 3, 48 (2020).[4] G. Roma, A. Marronnier & J. Even, From latent ferroelectricity to hyperferroelectricity in alkali lead halide perovskites, Phys Rev. Mat. 4, 092402(R) (2020).
Published: 2022

24. Atomistic studies of surface and interface properties in lead-free halide perovskite semiconductor devices

Author: Pedesseau, Laurent, Jiang, Pingping, Traore, Boubacar, Kepenekian, Mikaël, Katan, Claudine, Volonakis, George, Even, Jacky, PEDESSEAU, Laurent, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.INOR] Chemical Sciences/Inorganic chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.PHYS]Physics [physics]/Physics [physics], [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [PHYS.PHYS] Physics [physics]/Physics [physics], [INFO.INFO-MO] Computer Science [cs]/Modeling and Simulation, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, [INFO.INFO-MO]Computer Science [cs]/Modeling and Simulation, [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract: International audience
Published: 2022

25. Perovskite nanocrystal quantum dots: theoretical exploration profoundly inspired by synthesis and spectroscopy

Author: Nguyen, Thi Phuc Tan, Katan, Claudine, Even, Jacky, Nguyen, Thi Phuc Tan, Polariton logic - PoLLoC - 899141 - INCOMING, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and European Project: 899141,PoLLoC
Subjects: [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract: International audience
Published: 2022

26. Many-body calculations for perovskite nanocrystals

Author: Nguyen, Thi Phuc Tan, Katan, Claudine, Even, Jacky, Nguyen, Thi Phuc Tan, Polariton logic - PoLLoC - 899141 - INCOMING, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA), This project has received funding from the European Union’s Horizon 2020 program, through a FET Openresearch and innovation action under the grant agreement No 899141 (POLLOC), and European Project: 899141,PoLLoC
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: National audience; Perovskite nanocrystals (NCs) are among the most fashionable names nowadays in the field of colloidalsynthesis owing to their superior photoluminescence quantum yield and blinking-free properties, whichmake them promising materials for both classical [1,2] and quantum light sources [3,4]. Their brightnessand sub-nanosecond radiative decay originates from the inherent correlation effects [5,6]. The manybodyCoulomb interaction has generally been studied for semiconductor quantum dots [7,8]. Perovskites,as a consequence of the unique properties of their dielectric functions, possess enhanced Coulombinteraction between the charge carriers [9]. This leads to large binding energies of multi-exciton systemssuch as trion and biexciton in these NCs or the sizable splitting in the fine structure of single excitonstates. Considering each NC as an artificial atom under the envelope function approximation, thisproblem of correlation effects can be approached at first by using second-order many-body techniquesas outlined in Ref. [10]. This offers an elegant and efficient method that provides qualitative results forthe trion and biexciton binding energies [11]. In going beyond the second-order description, configurationinteraction can be employed to include the correlation energies between the various charge carriers in amore holistic manner.REFERENCES:[1] Kovalenko et al., Properties and potential optoelectronic applications of lead halide perovskitenanocrystals. Science 358, 6364, 745-750, 2017.[2] Raino et al., Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure. ACS Nano 10, 2, 2485–2490, 2016.[3] Utzat et al., Coherent single-photon emission from colloidal lead halide perovskite quantum dots.Science, 363(6431):1068–1072, 2019.[4] Tamarat et al., The dark exciton ground state promotes photon-pair emission in individual perovskitenanocrystals. Nature Communications. 11, 6001, 2020.[5] Becker et al., Bright triplet excitons in caesium lead halide perovskites. Nature, 553(1):189–193,2018.[6] Tamarat et al., The ground exciton state of formamidinium lead bromide perovskite nanocrystals is asinglet dark state. Nature Materials 18, 717–724, 2019.[7] M. Combescot and R. Combescot, Optical stark effect of the exciton: Biexcitonic origin of the shift.Phys. Rev. B, 40:3788–3801, 1989.[8] Rontani et al., Coulomb correlation effects in semiconductor quantum dots: The role of dimensionality.Phys. Rev. B 59, 10165, 1999.[9] Even et al., Analysis of Multivalley and Multibandgap Absorption and Enhancement of Free CarriersRelated to Exciton Screening in Hybrid Perovskites. J. Phys. Chem. C, 118, 11566−11572, 2014.[10] I. Lindgren and J. Morrison, Atomic Many-Body Theory. Springer-Verlag, 1982.[11] Nguyen et al., Calculation of the biexciton shift in nanocrystals of inorganic perovskites. Phys. Rev.B, 101. 125424, 2020.
Published: 2022

27. Physics of 2D perovskites

Author: Even, Jacky, Blancon, Jean Christophe, Sidhik, Siraj, li, weibin, Zhang, Hao, Li, Wei, Traore, Boubacar, Pedesseau, Laurent, Volonakis, George, Kepenekian, Mikael, Stoumpos, Constantinos, Kanatzidis, Mercouri, Mohite, Aditya, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Nankai University (NKU), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), University of Crete [Heraklion] (UOC), Northwestern University [Evanston], European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics]
Abstract: International audience; In the past years, solution-processed organometallic perovskite based solar cells have emerged as a promising low-cost thin-film photovoltaic technology. 3D halide perovskite semiconductors and their 2D or OD nanostructures present specific symmetry and electronic properties, including giant spin-orbit coupling (SOC) effects. The ultrahigh softness of the halide perovskite lattice is also characteristic, and the role of the electron-phonon coupling, especially at temperatures relevant for device operation, is not fully understood. The presentation will focus on 2D perovskites, composed of perovskites layers sandwiched between two layers of large organic cations, described in the 90’s as self-assembled quantum and dielectric well systems.
Published: 2021

28. Solid state NMR structural characterization of halide perovskites: the potential contribution of atomistic DFT modeling

Author: Quarti, Claudio, Furet, Eric, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Mons [Belgium] (UMONS), ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), KATAN, Claudine, and APPEL À PROJETS GÉNÉRIQUE 2018 - Cellules solaires perovskite plus stables et à teneur réduite en plomb. - - MORELESS2018 - ANR-18-CE05-0026 - AAPG2018 - VALID
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: International audience; Halide perovskites are a complex class of semiconductors whose structure features two apparently contradictory properties: long-range order associated to the regular crystalline structure,[1] and short-range dynamic disorder, related to the soft nature of the lattice and the libration motion of the organic cations.[2] While the former feature is routinely addressed via X-ray diffraction techniques, the latter requires more local “probes”, with solid state Nuclear Magnetic Resonance (NMR) being an ideal method-of-choice, in light of its sensitivity to local chemical composition and environment, as demonstrated in the recent literature [3-6]. However, the complex line-shapes of solid state NMR measurements, as due to the inherent anisotropic response of this technique, make their interpretation usually a delicate task, hence calling for additional supportive tools.Here we show how periodic DFT simulations can ease the interpretation of the NMR spectroscopic features, providing a complementary perspective to experiments. Targeting nuclei with spin-quantum number I=1/2 for 3D methylammonium lead iodide, bromide and mixed halide systems, we demonstrate the reliability of DFT in reproducing experimental signatures of 13C and 1H light-atoms, with prospects in supporting the characterization of dimensionally confined or hollow perovskite architectures, where the organic component has more important structural/templating role. Quantitative prediction of 207Pb nuclei is more challenging but the different response from pure phase iodide and bromide lead perovskites is well reproduced by DFT simulations. This motivated us to investigate on mixed halide compositions, confirming the sensitivity of NMR to the halide composition,[6-7] and segregation, already at the scale of the individual PbX6 octahedron.[8] Our results open the prospect for joint theoretical-experimental investigations of halide perovskite materials, that combine solid state NMR and periodic DFT simulations. [1] Weller, M. T.; Weber, O. J.; Frost, J. M.; Walsh, A. Cubic Perovskite Structure of Black Formamidinium Lead Iodide, α‐[HC(NH2)2]PbI3, at 298 K, J. Phys. Chem. Lett. 2015, 6, 3209-3212.[2] Quarti, C.; Mosconi, E.; De Angelis, F. Structural and electronic properties of organo-halide hybrid perovskites from ab initio molecular dynamics, Phys. Chem. Chem. Phys., 2015, 17, 9394-9409. [3] Piveteau, L.; Morad, V.; Kovalenko, M. V. Solid-State NMR and NQR spectroscopy of lead-halide perovskite materials, J. Am. Chem. Soc. 2020, 142, 19413-19437.[4] Kubicki, D. J.; Prochowicz, D.; Hofstetter, A.; Zakeeruddin, S. M.; Grätzel, M.; Emsley, L.; Phase Segregation in Cs‐, Rb- and K‐Doped Mixed-Cation (MA)x(FA)1−xPbI3 Hybrid Perovskites from Solid-State NMR’, J. Am. Chem. Soc. 2017, 139, 14173–14180.[5] Milic, J. V.; Im, J.-H.; Kubicki, D. J.; Ummadisingu, A.; Seo, J.-Y.; Li, Y. Ruiz-Preciado, M. A.; Ibrahim Bar, M.; Zakeeruddin, S. M.; Emsley, L.; Grätzel, M. Supramolecular Engineering for Formamidinium-Based Layered 2D Perovskite Solar Cells: Structural Complexity and Dynamics Revealed by Solid-State NMR Spectroscopy, Adv. Energy Mater. 2019, 9, 1900284.[6] Rosales, B. A.; Men, L.; Cady, S.; Hanrahan, M. P.; Rossini, A. J.; Vela, J. Persistent Dopants and Phase Segregation in Organolead Mixed- Halide Perovskites, Chem. Mater. 2016, 28, 6848–6859.[7] Roiland, C.; Trippé-Allard, G.; Jemli, K.; Alonso, B.; Ameline, J.-C.; Gautier, R.; Bataille, T.; Le Pollès, L.; Deleporte, E.; Even, J.; Katan, C. Multinuclear NMR as a tool for studying local order and dynamics in CH3NH3PbX3 (X = Cl, Br, I) hybrid perovskites, Phys. Chem. Chem. Phys. 2016, 18, 27133–27142.[8] Quarti C., Furet E., Katan C., DFT simulations as valuable tool to support NMR characterization of halide perovskites: the case of pure and mixed halide perovskites, submitted under invitation to Helvetica Chimica ActaAcknowledgements This work has been supported by Agence Nationale de la Recherche, project ANR-18-CE05-0026 (MORELESS).
Published: 2021

29. Multi-excitons and correlation effects in perovskite nanocrystals

Author: Nguyen, Tan, Katan, Claudine, Even, Jacky, KATAN, Claudine, Polariton logic - PoLLoC - 899141 - INCOMING, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), European Project: 899141,PoLLoC, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: National audience; Up to date, perovskites have remained to be one of the most fashionable names in the research ofphotovoltaic materials, achieving an efficiency reaching over 25% without the use of tandem structure[1]. Apart from being excellent materials for solar cells, perovskites have also shown to be an extremelypromising candidate for both classical and quantum light sources [2, 3]. Recent advancements insynthesis and surface treatment have allowed a more precise control of emission from nanostructures[4, 5]. In this context, our theoretical work aims to investigate the electronic and optical properties ofthe systems of single exciton and beyond. Previous calculations on nanocubes or spherical nanocrystalshave demonstrated the correlation origin of exciton fine-structure [6] and biexciton/trion emission [7].In this talk, we will present the configuration interaction approach to take into account the correlationeffects in these systems in a more systematic and complete manner.REFERENCES[1] Kim et al., High-Efficiency Perovskite Solar Cells, Chem. Rev. 2020, 120, 7867-7918, 2020[2] Protesescu et al., Nanocrystals of cesium lead halide perovskites (cspbx3, x = cl, br, and i): Novel optoelectronicmaterials showing bright emission with wide color gamut. Nano Letters, 15(6):3692–3696, 2015[3] Utzat et al., Coherent single-photon emission from colloidal lead halide perovskite quantum dots. Science,363(6431):1068–1072, 2019[4] Huo et al., Optical Spectroscopy of Single Colloidal CsPbBr3 Perovskite Nanoplatelets, Nano Lett. 2020, 20,5, 3673–3680[5] Bertolloti et al., Crystal Structure, Morphology, and Surface Termination of Cyan-Emissive, Six-Monolayers-Thick CsPbBr3 Nanoplatelets from X-ray Total Scattering, ACS Nano 2019, 13, 12, 14294–14307[6] Tamarat et al., The dark exciton ground state promotes photon-pair emission in individual perovskitenanocrystals, Nature Communications, vol 11, 6001, 2020[7] Nguyen et al., Calculation of the biexciton shift in nanocrystals of inorganic perovskites. Phys. Rev. B, 101.125424, 2020
Published: 2021

30. Using Time-Resolved Photoconductivity Measurements to Reveal the Urbach Tail and Two Photon Absorption in MHPs

Author: Savenije, Tom, Thieme, Jos, Wei, Zimu, Caselli, Valentina, Guo, Dengyang, Even, Jacky, Katan, Claudine, Delft University of Technology (TU Delft), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), and KATAN, Claudine
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, perovskites, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], photoconductivity, optoelectronic, [PHYS.COND.CM-MS] Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract: International audience; The unprecedented rise in power conversion efficiency of solar cells based on metal halide perovskites (MHPs) has led to an enormously growing research effort over the last 6 years. In this paper, we report how the electrodeless transient microwave photoconductivity technique (TRMC) can reveal detailed information, regarding the interesting photo-physical properties of MHPs. First, we recorded two photon absorption (2PA) spectra of MHP thin films over a wavelength regime between 0.5Eg and Eg, from which the 2PA coefficients have been calculated. A two-step upward trend is observed in the 2PA coefficient spectrum for CH3NH3PbI3. Using a parameterized tight binding model, spectra were calculated by integration over all Brillouin zones showing compelling similarity with experimental results. We conclude that the second upward trend in the 2PA spectrum originates from additional optical transitions to the heavy and light electron bands formed by the strong spin-orbit coupling. Next, we performed TRMC measurements using optical excitation above and below the band-gap on pristine MAPbI3, MAPbI3/C60, and MAPbI3/Spiro-OMeTAD thin films. In pristine MAPbI3 we have observed a band-like charge transport for photon energies down to 1.40eV, from which we calculated an Urbach energy of approximately 16 meV, indicative of a relatively low structural disorder. Our TRMC measurements on the bilayers revealed that electrons in defect states close to the VB can be excited by photons with an energy as low as 1.30 eV. Their excitation leads to free electrons in the CB that undergo charge injection into the C60 yielding long-lived charge separation. In contrast, excitation of MAPbI3/Spiro-OMeTAD at 1.3 eV shows a rapidly decaying signal implying that holes are localized and cannot be transferred over the interface to the Spiro-OMeTAD.
Published: 2020

31. Insight into the Versatility of Layered Metal Halide Perovskites Based on Atomic Scale Modeling

Author: Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), KATAN, Claudine, APPEL À PROJETS GÉNÉRIQUE 2018 - Cellules solaires perovskite plus stables et à teneur réduite en plomb. - - MORELESS2018 - ANR-18-CE05-0026 - AAPG2018 - VALID, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: the work was granted access to the HPC resources of TGCC/CINES/IDRIS under the allocation A0060906724 and A0010907682 between 2016 to 2020 made by GENCI.; International audience
Published: 2020

32. From Bulk Metal Halide Perovskites to Lower Dimensions: Few Representative Examples

Author: Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Giacomo Giorgi and Linn Leppert, ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), KATAN, Claudine, APPEL À PROJETS GÉNÉRIQUE 2018 - Cellules solaires perovskite plus stables et à teneur réduite en plomb. - - MORELESS2018 - ANR-18-CE05-0026 - AAPG2018 - VALID, Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Rennes-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES), ANR-18-CE05-0026,MORELESS,MORE STABLE AND LESS LEAD FOR PEROVSKITE SOLAR CELLS(2018), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], [PHYS.COND] Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2020

33. Using large scale scattering facilities to study structural and optoelectronic properties of 2D and 3D perovskites

Author: Even, Jacky, Sidhik, Siraj, li, weibin, Zhang, Hao, Traoré, Boubacar, Bourges, Philippe, Kanatzidis, Mercouri, Blancon, Jean Christophe, Mohite, Aditya, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Northwestern University [Evanston], Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), J. Even acknowledges the financial support from the Institut Universitaire de France., European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, even, jacky, Polariton logic - PoLLoC - 899141 - INCOMING, High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING, and DRop-on demand flexible Optoelectronics & Photovoltaics by means of Lead-Free halide perovskITes - DROPIT - 862656 - INCOMING
Subjects: [PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract: National audience; The presentation will describe a few recent results on the structural and optoelectronic properties in 2D and 3D halide perovskites, focusing on some possibilities offered by nowadays neutron, X-rays and electron large scale scattering facilities.
Published: 2021

34. Light-activated interlayer contraction leads to high-efficiency in 2D perovskite solarcells

Author: Traoré, Boubacar, Li, Wenbin, Sidhik, Siraj, Asadpour, Reza, Hou, Jin, Zhang, Hao, Fehr, Austin, Essman, Joseph, Wang, Yafei, Hoffman, Justin, Spanopoulos, Ioannis, Crochet, Jared, Tsai, Esther, Strzalka, Joseph, Alam, Muhammad, Kanatzidis, Mercouri, Katan, Claudine, Blancon, Jean Christophe, Mohite, Aditya, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Rice University [Houston], Purdue University [West Lafayette], Northwestern University [Evanston], Los Alamos National Laboratory (LANL), Brookhaven National Laboratory [Upton, NY] (BNL), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE), Argonne National Laboratory [Lemont] (ANL), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J. Even acknowledges the financial support from the Institut Universitaire de France. DFT calculations were performed at Institut FOTON as well as Institut des Sciences Chimiques de Rennes, and the work was granted access to the HPC resources of Très Grand Centre de Calcul du CEA (TGCC), the Centre Informatique National de I’Enseignement Supérieur (CINES) and Institut du développement et des ressources en informatique scientifique (IDRIS) under allocations 2019-A0060906724 and 2019-A0070907682 made by Grand Équipement National de Calcul Intensif (GENCI)., CNRS Israeli French scientific cooperation (Joint Research Projects 2019-2021 ALLPOA)., European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), even, jacky, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING
Subjects: [PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract: National audience; Despite their improved stability and versatility, 2D layered perovskites’ solar cell efficiencies lag behind those of their 3D counterparts, which currently exceed 25%. Through a proper selection of the organic spacer, 2D perovskites can be synthetized in different configurations adopting various phases such as the Ruddlesden-Popper (RP), the Alternating Cation Interlayer (ACI) or the Dion-Jacobson ones. Tailoring the organic spacer type has been shown to enhance the electronic coupling along the layered perovskite stacking axis and thereby enhance carrier transport resulting in improved efficiencies.
Published: 2021

35. Microscopic connection between absolute valence energy alignment and surface dipoles in halide perovskite heterostructures

Author: Traoré, Boubacar, Basera, Pooja, Ramadan, Alexandra, Snaith, Henry, Katan, Claudine, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Oxford, European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), and University of Oxford [Oxford]
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; In recent years, hybrid organic-inorganic perovskites (HOP) have undergone extensive research due to their excellent photovoltaic and optoelectronic properties. To further improve their device performance, there is a considerable ongoing research effort on their surface passivation and/or functionalization. This stems from the fact that surface passivation and/or functionalization, including the combination of 2D and 3D perovskites, directly influences the surface dipoles between adjacent layers in a device stack, which in turn changes materials' work functions and absolute energy level alignments. However, the link between the two lacks a general framework bridging classical electromagnetism and modern atomistic approaches. Shedding more light on this link is of great technological importance to fully exploit the potentials of these semiconductors. Hence, this contribution presents a theoretical methodology thatclearly shows the relationship between surface dipoles and work functions. We rely on a semiclassical approach, that will allow scientists not specialized in DFT computation, to make use of their chemical or physical intuitions. We demonstrate the potentials of the methodology through a variety of cases to clearly show i) the effect of surface termination on the absolute energy level alignments, the ability to modulate the work function via ii) surface coating and iii) surface functionalization and/or passivationwith molecules. Finally, we demonstrate the additivity of surface dipoles in heterostructures, which is analogous to the additivity of the dielectric susceptibility in these compounds. Our methodology transcends the limits of halide perovskites and provides a computational strategy to fine-tune the absolute energy level alignments for optimizing the performance of broader families of optoelectronic devices
Published: 2021

36. Theoretical insights to tune the surface dipoles and work functions of halide perovskites

Author: basera, pooja, Traoré, Boubacar, Even, Jacky, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Israeli-French scientific cooperation (Joint Research Projects 2019-2021 ALLPOA) CNRS., European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Lead halide perovskites have attracted considerable interest owing to their rich physics and rapidly burgeoning applications in the field of optoelectronic devices. Therefore, an accurate theoretical description of the link between surface dipoles and the work functions, especially to understand the interface effects in this class of materials is of scientific and practical interest. Herein, we briefly introduce our methodology that accentuates the relation between the surface dipoles and the work functions using concepts from classical physics combined with the state-of-the-art first-principles calculations.
Published: 2021

37. DFT study of the optoelectronic properties of 2D multilayered perovskites

Author: Bergonzoni, Ashanti, Li, Xiaotong, Pillet, Sébastien, Boukheddaden, Kamel, Yangui, Aymen, Pedesseau, Laurent, Traore, Boubacar, Katan, Claudine, Kanatzidis, Mercouri, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Northwestern University [Evanston], Cristallographie, Résonance Magnétique et Modélisations (CRM2), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay, Lund University [Lund], Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Israeli-French scientific cooperation (Joint Research Projects 2019-2021 ALLPOA) CNRS, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Used alone or associated with a 3D structure in a 2D/3D heterojunction, two-dimensional (2D) halide perovskites have recently emerged as a game changer in the field of perovskites solar cells thanks to their excellent optoelectronic properties combined with an enhanced material stability.
Published: 2021

38. Ag-Bi-I rudorffites for solar-cell applications: Insights on their structures, electronic and optical properties from first-principles

Author: Cucco, Bruno, Pedesseau, Laurent, Katan, Claudine, Even, Jacky, Kepenekian, Mikael, Volonakis, George, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), European Project: 862656,DROPIT, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), and Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Lead halide perovskites exhibit excellent photovoltaic properties and over the past years have revolutionized the field of solution processed photovoltaics, achieving record power conversion efficiencies (PCE) of above 25.5%. Yet, due to concerns raised regarding the presence of the nonenvironmentally friendly Pb-atoms, the quest for stable non-toxic materials with high photo-conversion efficiency remains an active topic of research. In 2017, silver bismuth halides with an AaBbXx (x = a+3b) lattice, were shown to be highly stable and promising candidate materials for solar cell applications. These compounds, also called rudorffites, exhibit optical band gaps ranging between 1.4 eV to 2.0 eV, impressive high short-circuit current [4,5] and have achieved PCE of up to 5.6%.
Published: 2021

39. Challenges and opportunities for bismuth-based low-dimension halide perovskites

Author: Kepenekian, Mikaël, Katan, Claudine, Manceau, Matthieu, Mercier, Nicolas, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018)
Subjects: [CHIM]Chemical Sciences
Abstract: International audience
Published: 2021

40. White-light emitting Ruddlesden-Popper perovskites

Author: Bergonzoni, Ashanti, Pillet, Sébastien, Boukheddaden, Kamel, Yangui, Aymen, Pedesseau, Laurent, Traoré, Boubacar, Katan, Claudine, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Cristallographie, Résonance Magnétique et Modélisations (CRM2), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay, Lund University [Lund], Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and even, jacky
Subjects: [PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract: International audience; Recently, owing to their excellent optoelectronic properties combined with an enhancedmaterial stability, two-dimensional (2D) organic halide perovskites have emerged as an attractive alternative to 3D perovskites for photovoltaics . More, their ability to emit white-light at room temperature with a good color rendering projected this family of materials into the spotlight of potential future low-cost white LED components .
Published: 2021

41. Towards lead-free perovskite device architectures: interface simulations of tin-based heterostructures

Author: Pedesseau, Laurent, Jiang, Pingping, Traore, Boubacar, Kepenekian, Mika��l, Volonakis, George, Katan, Claudine, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), European Project: 862656,DROPIT, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS
Abstract: Following the emergence of lead halide perovskites as record-breaking materials for emerging photovoltaic applications, lead-free perovskites are gaining interest as novel materials which are compatible with inkjet-printing based technologies1,2,3. Bulk properties are of the prime importance, but charge transport can be rapidly altered across the interface of perovskite/ (hole or electron) transport layer (HTL or ETL). Yet, due to the size and complexity of the interface systems, a thorough ab initio modeling of the interfaces remains elusive to-date. Within this work, to explore the atomic-scale details of the structural and electronic properties of these materials, we employ state-of-the-art density functional theory (DFT) based calculations of model tin-based heterostructures. We investigate in particular three-dimensional corner-sharing Sn-based perovskites, their surface and interface properties and calculate the interaction of the materials with charge transport layers (CTLs). Our approach reveals the electronic band alignments and dielectric mismatches between perovskite layers and the most important hole and electron transport layers that have been used in prototype thin film device architectures4,5. In an effort to understand the fundamental physico-chemical mechanisms that govern the interactions between the photo-active absorber material and CTLs, we also probe the influence of surface termination on structural and electronic properties at FASnI3/C60 (as ETL) interfaces and FASnI3/NiOx (as ETL) interfaces. Our findings give a detailed insight into the interface engineering necessary for optimizing the next generation of environmental-friendly high-performing opto-electronic devices. This DROP-IT project1 has received funding from the European Union’s Horizon 2020 research and innovation Program under the grant agreement No 862656. The information and views set out in the abstracts and presentations are those of the authors and do not necessarily reflect the official opinion of the European Union. Neither the European Union institutions and bodies nor any person acting on their behalf may be held responsible for the use which may be made of the information contained herein. References: (1) DROPIT https://www.uv.es/dropit/ (accessed June 22, 2021). (2) Volonakis, G.; Filip, M. R.; Haghighirad, A. A.; Sakai, N.; Wenger, B.; Snaith, H. J.; Giustino, F. Lead-Free Halide Double Perovskites via Heterovalent Substitution of Noble Metals. J. Phys. Chem. Lett. 2016, 7 (7), 1254–1259. https://doi.org/10.1021/acs.jpclett.6b00376. (3) Volonakis, G.; Haghighirad, A. A.; Milot, R. L.; Sio, W. H.; Filip, M. R.; Wenger, B.; Johnston, M. B.; Herz, L. M.; Snaith, H. J.; Giustino, F. Cs2InAgCl6: A New Lead-Free Halide Double Perovskite with Direct Band Gap. J. Phys. Chem. Lett. 2017, 8 (4), 772–778. https://doi.org/10.1021/acs.jpclett.6b02682. (4) Traore, B.; Pedesseau, L.; Blancon, J.-C.; Tretiak, S.; Mohite, A. D.; Even, J.; Katan, C.; Kepenekian, M. Importance of Vacancies and Doping in Hole Transporting Nickel Oxide Interface with Halide Perovskites. ACS Appl. Mater. Interfaces 2020. https://doi.org/10.1021/acsami.9b19457. (5) Canicoba, N. D.; Zagni, N.; Liu, F.; McCuistian, G.; Fernando, K.; Bellezza, H.; Traoré, B.; Rogel, R.; Tsai, H.; Le Brizoual, L.; et al. Halide Perovskite High-k Field Effect Transistors with Dynamically Reconfigurable Ambipolarity. ACS Materials Lett. 2019, 1 (6), 633–640. https://doi.org/10.1021/acsmaterialslett.9b00357.
Published: 2021

42. Nonadiabatic molecular dynamics analysis of hybrid Dion–Jacobson 2D leads iodide perovskites: A Nonadiabatic Molecular Dynamics Study

Author: Wang, Ying, Pedesseau, Laurent, Katan, Claudine, Even, Jacky, Prezhdo, Oleg, Tretiak, Sergei, Ghosh, Dibyajyoti, Neukirch, Amanda, University of Southern California (USC), Los Alamos National Laboratory (LANL), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Indian Institute of Technology Delhi (IIT Delhi), The work at Los Alamos National Laboratory (LANL) wassupported by the LANL LDRD program (S.G.L., F.L., W.N., A.J.N.,and S.T.). This work was done in part at Center for NonlinearStudies (CNLS) and the Center for Integrated Nanotechnologies(CINT), a U.S. Department of Energy and Office of Basic EnergySciences user facility, at LANL. This research used resourcesprovided by the LANL Institutional Computing Program. LANL isoperated by Triad National Security, LLC, for the National NuclearSecurity Administration of the U.S. Department of Energy underContract No. 89233218NCA000001. J.E. acknowledges the financialsupport from the Institut Universitaire de France. Y.W. and O.V.P.acknowledge support of the U. S. Department of Energy, Grant No.DE-SC0014429., Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry
Abstract: International audience; The past six years have witnessed the rapid growth of interest in Dion–Jacobson (DJ) phase two-dimensional (2D) hybrid halide perovskitesas optoelectronic materials with considerable intrinsic stability. The precise relationships between structural variations and the resultingcharge carrier dynamics at finite temperature in these materials are keys to practical applications and are not yet completely understood.Here, we study 3-(aminomethyl) piperidinium (3AMP) and 4-(aminomethyl) piperidinium (4AMP) spacer cation-based lead iodide DJphase systems and find these spacer cations to have a profound impact on the structural dynamics. Particularly, large conformational dynamicsof the 3AMP-based perovskite compared to that of the 4AMP at room temperature leads to pronounced state energy fluctuation nearband edges and further results in a shorter quantum coherence. The faster quantum decoherence of the 3AMP spacer-based perovskiteunderpins a longer nonradiative lifetime, offering insight into its superior performance as an optoelectronic material. This work sheds lighton the relationship between structural fluctuations and charge carrier dynamics that can help in designing 2D perovskites with superior photophysicalproperties.
Published: 2021
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43. Theoretical and experimental study of the influence of (de)protonation of phenol-substituted diazine for White OLEDs

Author: Hodée, Maxime, Lenne, Augustin, Rodríguez-López, Julián, Guen, Françoise Robin-Le, Achelle, Sylvain, Katan, Claudine, Fihey, Arnaud, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Universidad de Castilla-La Mancha = University of Castilla-La Mancha (UCLM)
Subjects: [CHIM]Chemical Sciences
Abstract: International audience; In recent years, lighting has become more and more energy consuming, now reaching 20% of the global electricity consumption. Thus, there is need to properly design new environment friendly lighting devices and organic light emitting devices (OLEDs), in particular White OLEDs (WOLEDs), are more relevant than ever.[1] The major issue is that obtaining white light is not an easy task, and is in most cases achieved by using multilayer devices or a combination of different emissive molecules.[1,2] In this contribution, we present an innovative way of obtaining white light emission by modulating the protonation[3,4] and deprotonation of organic fluorophores. To this end, a series of 8 push-pull phenol substituted hydroxystyrildiazines has been designed by varying the nature of the acceptor diazinic heterocycle (pyrimidine/pyrazine) to be protonatedand of the linker moieties (thiophene, vinylene, thienylenevinylene, vinylphenylene). The photo-physical investigation of this series of compounds in solution showed a systematic bathochromic shift of the emission compared to the neutral form, not only upon the protonation, but also after deprotonation. Extensive Density Functional Theory (DFT) and TD-DFT calculations were performed to rationalize this behavior and understand the impact of (de)protonation on the different optical transitions characteristic of this family of fluorophores. Such computations showed that the (de)protonation impacts not only the energies of the vertical transitions, but also the nature of these transitions, with a significant increase in the Intramolecular Charge Transfer (ICT) character of the (de)excitations. Furthermore, playing with the nature of the diazinic moiety and the linker in the push-pull skeleton allows to fine tune the emission wavelength of the two forms and reach a complementary emission in solution.To the best of our knowledge, modulation of the emission by deprotonation has not yet been reported as an alternative strategy for obtaining WOLEDs. Our experimental and theoretical results on the phenol-substituted diazinic chromophores demonstrate that this approach proves successful, at least in solution. Thus, it opens a new route for the design of efficient WOLEDs and shall prompt further investigations up to device fabrication.
Published: 2021

44. Theoretical and experimental study of the influence of (de)protonation of phenol-substituted diazine for White OLEDs

Author: Hodée, Maxime, Lenne, Augustin, Rodríguez-López, Julián, Guen, Françoise Robin-le, Achelle, Sylvain, Katan, Claudine, Fihey, Arnaud, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), and Universidad de Castilla-La Mancha (UCLM)
Subjects: [CHIM]Chemical Sciences
Abstract: International audience; In recent years, lighting has become more and more energy consuming, now reaching 20% of the global electricity consumption. Thus, there is need to properly design new environment friendly lighting devices and organic light emitting devices (OLEDs), in particular White OLEDs (WOLEDs), are more relevant than ever.[1] The major issue is that obtaining white light is not an easy task, and is in most cases achieved by using multilayer devices or a combination of different emissive molecules.[1,2] In this contribution, we present an innovative way of obtaining white light emission by modulating the protonation[3,4] and deprotonation of organic fluorophores. To this end, a series of 8 push-pull phenol substituted hydroxystyrildiazines has been designed by varying the nature of the acceptor diazinic heterocycle (pyrimidine/pyrazine) to be protonatedand of the linker moieties (thiophene, vinylene, thienylenevinylene, vinylphenylene). The photo-physical investigation of this series of compounds in solution showed a systematic bathochromic shift of the emission compared to the neutral form, not only upon the protonation, but also after deprotonation. Extensive Density Functional Theory (DFT) and TD-DFT calculations were performed to rationalize this behavior and understand the impact of (de)protonation on the different optical transitions characteristic of this family of fluorophores. Such computations showed that the (de)protonation impacts not only the energies of the vertical transitions, but also the nature of these transitions, with a significant increase in the Intramolecular Charge Transfer (ICT) character of the (de)excitations. Furthermore, playing with the nature of the diazinic moiety and the linker in the push-pull skeleton allows to fine tune the emission wavelength of the two forms and reach a complementary emission in solution.To the best of our knowledge, modulation of the emission by deprotonation has not yet been reported as an alternative strategy for obtaining WOLEDs. Our experimental and theoretical results on the phenol-substituted diazinic chromophores demonstrate that this approach proves successful, at least in solution. Thus, it opens a new route for the design of efficient WOLEDs and shall prompt further investigations up to device fabrication.
Published: 2021

45. Interfacial engineering to modulate surface dipoles, work functions and dielectric confinement of halide perovskites via surface passivation

Author: basera, pooja, Traoré, Boubacar, Katan, Claudine, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Lead halide perovskites have attracted considerable interest owing to their rich physics and rapidly burgeoning applications in the field of optoelectronic devices. Therefore, an accurate theoretical description of the link between surface dipoles and the work functions, especially to understand the interface effects in this class of materials is of scientific and practical interest.
Published: 2021

46. Theoretical and experimental study of the influence of (de)protonation of phenol-substituted diazine for White OLEDs

Author: Hodée, Maxime, Lenne, Augustin, Rodríguez-López, Julián, Guen, Françoise Robin-le, Achelle, Sylvain, Katan, Claudine, Fihey, Arnaud, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), and Universidad de Castilla-La Mancha (UCLM)
Subjects: [CHIM]Chemical Sciences
Abstract: International audience; In recent years, lighting has become more and more energy consuming, now reaching 20% of the global electricity consumption. Thus, there is need to properly design new environment friendly lighting devices and organic light emitting devices (OLEDs), in particular White OLEDs (WOLEDs), are more relevant than ever.[1] The major issue is that obtaining white light is not an easy task, and is in most cases achieved by using multilayer devices or a combination of different emissive molecules.[1,2] In this contribution, we present an innovative way of obtaining white light emission by modulating the protonation[3,4] and deprotonation of organic fluorophores. To this end, a series of 8 push-pull phenol substituted hydroxystyrildiazines has been designed by varying the nature of the acceptor diazinic heterocycle (pyrimidine/pyrazine) to be protonatedand of the linker moieties (thiophene, vinylene, thienylenevinylene, vinylphenylene). The photo-physical investigation of this series of compounds in solution showed a systematic bathochromic shift of the emission compared to the neutral form, not only upon the protonation, but also after deprotonation. Extensive Density Functional Theory (DFT) and TD-DFT calculations were performed to rationalize this behavior and understand the impact of (de)protonation on the different optical transitions characteristic of this family of fluorophores. Such computations showed that the (de)protonation impacts not only the energies of the vertical transitions, but also the nature of these transitions, with a significant increase in the Intramolecular Charge Transfer (ICT) character of the (de)excitations. Furthermore, playing with the nature of the diazinic moiety and the linker in the push-pull skeleton allows to fine tune the emission wavelength of the two forms and reach a complementary emission in solution.To the best of our knowledge, modulation of the emission by deprotonation has not yet been reported as an alternative strategy for obtaining WOLEDs. Our experimental and theoretical results on the phenol-substituted diazinic chromophores demonstrate that this approach proves successful, at least in solution. Thus, it opens a new route for the design of efficient WOLEDs and shall prompt further investigations up to device fabrication.
Published: 2021

47. Electronic Structure and Stability of Cs2TiX6 and Cs2ZrX6 (X = Br, I) Vacancy Ordered Double Perovskites

Author: Cucco, Bruno, Bouder, Gaëlle, Pedesseau, Laurent, Katan, Claudine, Even, Jacky, Kepenekian, Mikaël, Volonakis, George, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), and European Project: 862656,DROPIT
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2021
Full Text: View/download PDF

48. Importance of lattice softness and phonon anharmonicity for the optoelectronic properties of 3D, 2D and 0D halide perovskites

Author: Even, Jacky, Da Cunha Ferreira, Afonso, Paofai, Serge, Létoublon, Antoine, Ollivier, Jacques, Raymond, stéphane, Sébastien, Clément, VIALLA, Remy, HEHLEN, Bernard, RUFFLE, Benoit, Cordier, Stéphane, Katan, Claudine, Bourges, Philippe, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Laue-Langevin (ILL), Magnétisme et Diffusion Neutronique (MDN ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Laboratoire Charles Coulomb (L2C), Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), ILL, and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: National audience
Published: 2021

49. Propriétés optoélectroniques et structurales des pérovskites halogénées 3D, 2D and 0D : quelques résultats récents

Author: Even, Jacky, Pedesseau, Laurent, Kepenekian, Mikael, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: National audience
Published: 2021

50. Lead Iodide Hybrids with Aromatic Diammonium Cations—From 2D Dion-Jacobson Perovskites to 3D Hybrid Structures

Author: Li, Xiaotong, Ke, Weijun, He, Yihui, Guo, Peijun, Kepenekian, Mikael, Traoré, Boubacar, Even, Jacky, Katan, Claudine, Schaller, Richard, Stoumpos, Constantinos, Kanatzidis, Mercouri, Northwestern University [Evanston], Argonne National Laboratory [Lemont] (ANL), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Department of Chemistry [Heraklion], University of Crete [Heraklion] (UOC), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2021

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