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161 results on '"Emmanuelle Deleporte"'

1. Unexpected Anisotropy of the Electron and Hole Landé g-Factors in Perovskite CH3NH3PbI3 Polycrystalline Films

Author

Guadalupe Garcia-Arellano, Gaëlle Trippé-Allard, Thomas Campos, Frédérick Bernardot, Laurent Legrand, Damien Garrot, Emmanuelle Deleporte, Christophe Testelin, and Maria Chamarro

Subjects
halide perovskite, CH3NH3PbI3, g-factor, polycrystalline film, photo-induced Faraday rotation, Chemistry, QD1-999
Abstract

In this work, we studied, at low temperature, the coherent evolution of the localized electron and hole spins in a polycrystalline film of CH3NH3PbI3 (MAPI) by using a picosecond-photo-induced Faraday rotation technique in an oblique magnetic field. We observed an unexpected anisotropy for the electron and hole spin. We determined the electron and hole Landé factors when the magnetic field was applied in the plane of the film and perpendicular to the exciting light, denoted as transverse ⊥ factors, and when the magnetic field was applied perpendicular to the film and parallel to the exciting light, denoted as parallel ∥ factors. We obtained |ge,⊥|=2.600 ± 0.004, |ge,∥|=1.604 ± 0.033 for the electron and |gh,⊥|=0.406 ± 0.002, |gh,∥|=0.299 ± 0.007 for the hole. Possible origins of this anisotropy are discussed herein.

Published
2022
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2. Photostability of 2D Organic-Inorganic Hybrid Perovskites

Author

Yi Wei, Pierre Audebert, Laurent Galmiche, Jean-Sébastien Lauret, and Emmanuelle Deleporte

Subjects
organic-inorganic hybrid perovskites, photostability, Technology, Electrical engineering. Electronics. Nuclear engineering, TK1-9971, Engineering (General). Civil engineering (General), TA1-2040, Microscopy, QH201-278.5, Descriptive and experimental mechanics, QC120-168.85
Abstract

We analyze the behavior of a series of newly synthesized (R-NH3)2PbX4 perovskites and, in particular, discuss the possible reasons which cause their degradation under UV illumination. Experimental results show that the degradation process depends a lot on their molecular components: not only the inorganic part, but also the chemical structure of the organic moieties play an important role in bleaching and photo-chemical reaction processes which tend to destroy perovskites luminescent framework. In addition, we find the spatial arrangement in crystal also influences the photostability course. Following these trends, we propose a plausible mechanism for the photodegradation of the films, and also introduced options for optimized stability.

Published
2014
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3. Preparations and Characterizations of Luminescent Two Dimensional Organic-inorganic Perovskite Semiconductors

Author

Sanjun Zhang, Pierre Audebert, Yi Wei, Antoine Al Choueiry, Gaëtan Lanty, Antoine Bréhier, Laurent Galmiche, Gilles Clavier, Cédric Boissière, Jean-Sébastien Lauret, and Emmanuelle Deleporte

Subjects
organic-inorganic perovskites, hybrid materials, multi-quantum wells, nanoparticles, spin coating, X-ray diffraction, absorption spectrum, photoluminescence, Technology, Electrical engineering. Electronics. Nuclear engineering, TK1-9971, Engineering (General). Civil engineering (General), TA1-2040, Microscopy, QH201-278.5, Descriptive and experimental mechanics, QC120-168.85
Abstract

This article reviews the synthesis, structural and optical characterizations of some novel luminescent two dimensional organic-inorganic perovskite (2DOIP) semiconductors. These 2DOIP semiconductors show a self-assembled nano-layered structure, having the electronic structure of multi-quantum wells. 2DOIP thin layers and nanoparticles have been prepared through different methods. The structures of the 2DOIP semiconductors are characterized by atomic force microscopy and X-ray diffraction. The optical properties of theb DOIP semiconductors are characterized from absorption and photoluminescence spectra measured at room and low temperatures. Influences of different components, in particular the organic parts, on the structural and optical properties of the 2DOIP semiconductors are discussed.

Published
2010
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4. Using Low Temperature Photoluminescence Spectroscopy to Investigate CH3NH3PbI3 Hybrid Perovskite Degradation

Author

Khaoula Jemli, Hiba Diab, Ferdinand Lédée, Gaelle Trippé-Allard, Damien Garrot, Bernard Geffroy, Jean-Sébastien Lauret, Pierre Audebert, and Emmanuelle Deleporte

Subjects
CH3NH3PbI3, hybrid perovskite, solar cells, optoelectronics, degradation, photoluminescence, Organic chemistry, QD241-441
Abstract

Investigating the stability and evaluating the quality of the CH3NH3PbI3 perovskite structures is quite critical both to the design and fabrication of high-performance perovskite devices and to fundamental studies of the photophysics of the excitons. In particular, it is known that, under ambient conditions, CH3NH3PbI3 degrades producing some PbI2. We show here that low temperature Photoluminescence (PL) spectroscopy is a powerful tool to detect PbI2 traces in hybrid perovskite layers and single crystals. Because PL spectroscopy is a signal detection method on a black background, small PbI2 traces can be detected, when other methods currently used at room temperature fail. Our study highlights the extremely high stability of the single crystals compared to the thin layers and defects and grain boundaries are thought to play an important role in the degradation mechanism.

Published
2016
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6. Third-order optical nonlinearity in nucleobase solid thin solid film and its application for ultrashort light pulse generation

Author

Reza Khazaeinezhad, Sahar Hosseinzadeh Kassani, Marjan Ghasemi, Yongjae Cho, Seong Il Im, Dong Il Yeom, Fabian Rotermund, James G Grote, Emmanuelle Deleporte, Isabelle Ledoux-Rak, and Kyunghwan Oh

Subjects
Materials Chemistry, General Chemistry
Abstract

Generating high stability ultrafast pulse laser using constituents of the most powerful biomolecules in nature (Adenine, Guanine, Cytosine, and Thymine).

Published
2022

7. Using chiral ammonium cations to modulate the structure of 1D hybrid lead bromide perovskites for linearly polarized broadband light emission at room temperature

Author

Joanna M. Urban, Abdelaziz Jouaiti, Nathalie Gruber, Géraud Delport, Gaëlle Trippé-Allard, Jean-François Guillemoles, Emmanuelle Deleporte, Sylvie Ferlay, and Damien Garrot

Subjects
Materials Chemistry, General Chemistry
Abstract

Low dimensional 1D enantiomerically pure and racemic lead bromide perovskite compounds have been structurally characterized. All compounds show broadband below-bandgap emission. They exhibit a significant degree of linear polarization at RT.

Published
2022

9. Synthesis of highly calibrated CsPbBr

Author

Cédric R, Mayer, Hugo, Levy-Falk, Maxime, Rémond, Gaëlle, Trippé-Allard, Frédéric, Fossard, Maxime, Vallet, Marc, Lepeltier, Nicolas, Guiblin, Jean-Sébastien, Lauret, Damien, Garrot, and Emmanuelle, Deleporte

Abstract

A new synthetic method for preparing highly calibrated CsPbBr

Published
2022

11. Electron Dynamics in Hybrid Perovskites Reveal the Role of Organic Cations on the Screening of Local Charges

Author

Marie Cherasse, Jingwei Dong, Gaëlle Trippé-Allard, Emmanuelle Deleporte, Damien Garrot, Sebastian F. Maehrlein, Martin Wolf, Zhesheng Chen, Evangelos Papalazarou, Marino Marsi, Jean-Pascal Rueff, Amina Taleb-Ibrahimi, Luca Perfetti, Laboratoire des Solides Irradiés (LSI), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Department of Inorganic Chemistry, Fritz Haber Institute of the Max Planck Society, Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Deutscher Akademischer Austauschdienst, DAAD: 20181832, 57507869, Deutsche Forschungsgemeinschaft, DFG: 490867834, Agence Nationale de la Recherche, ANR: ANR-21-CE30-0059, and We acknowledge financial support of the 2D-HYPE project from the Agence Nationale de la Recherche (ANR, Nr. ANR-21-CE30-0059), the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, Nr. 490867834), the DAAD Scholarship 57507869, and the SOLEIL Synchrotron for the provision of the beamtime (proposal 20181832). Valerie Veniard, Paolo Umari, Antonio Tejeda, and Catherine Corbel contributed to the data interpretation with enlightening discussions.

Subjects
Condensed Matter::Materials Science, Mechanical Engineering, screening, band alignment, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], General Materials Science, Bioengineering, General Chemistry, Condensed Matter Physics, time-resolved spectroscopy, hybrid perovskites
Abstract

International audience; The large tolerance of hybrid perovksites to the trapping of electrons by defects is a key asset in photovoltaic applications. Here, the ionic surface terminations of CH3NH3PbI3 are employed as a testbed to study the effect of electrostatic fields on the dynamics of excited carriers. We characterize the transition across the tetragonal to orthorhombic phase. The observed type II band offset and drift of the excited electrons highlight the important role that organic cations have on the screening of local electrostatic fields. When the orientation of organic cations is frozen in the orthorhombic phase, the positively charged termination induces a massive accumulation of excited electrons at the surface of the sample. Conversely, no electron accumulation is observed in the tetragonal phase. We conclude that the local fields cannot penetrate in the sample when the polarizability of freely moving cations boosts the dielectric constant up to ϵ = 120.

Published
2022

12. Taming Friedrich-Wintgen interference in resonant metasurface: vortex laser emitting at on-demand tilted-angle

Author

Raphael Mermet-Lyaudoz, Clémentine Symonds, Florian Berry, Emmanuel Drouard, Céline Chevalier, Gaëlle Trippé-Allard, Emmanuelle Deleporte, Joel Bellessa, Christian Seassal, and Hai Son Nguyen

Subjects
Mechanical Engineering, FOS: Physical sciences, General Materials Science, Bioengineering, General Chemistry, Condensed Matter Physics, Physics - Optics, Optics (physics.optics)
Abstract

Friedrich-Wintgen (FW) interference is an atypical coupling mechanism that grants loss exchange between leaky resonances in non-Hermitian classical and quantum systems. Intriguingly, such an mechanism makes it possible for destructive interference scenario in which a radiating wave becomes a bound state in the continuum (BIC) by giving away all of its losses. Here we propose and demonstrate experimentally an original concept to tailor FW-BICs as polarization singularity at on-demand wavevectors in optical metasurface. As a proof-of-concept, using hybrid organic-inorganic halide perovskite as active material, we empower this novel polarization singularity to obtain lasing emission exhibiting both highly directional emission at oblique angles and polarization vortex in momentum space. Our results pave the way to steerable coherent emission with tailored polarization pattern for applications in optical communication/manipulation in free-space, high-resolution imaging /focusing and data storage.

Published
2022
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13. Tetrazine molecules as an efficient electronic diversion channel in 2D organic-inorganic perovskites

Author

Jean-Sébastien Lauret, Gaëlle Trippé-Allard, Claudio Quarti, Laurent Galmiche, Jacky Even, Ferdinand Lédée, Damien Garrot, Pierre Audebert, Jérôme Marrot, Claudine Katan, Emmanuelle Deleporte, Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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), Université de Mons (UMons), J.E and J.S.L acknowledges the financial support from the Institut Universitaire de France. Computational investigations were conducted thanks to HPC resources provided by [TGCC/CINES/IDRIS] under the allocation 2020-A0010907682 made by GENCI., ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), ANR-18-CE24-0016,EMIPERO,Dispositifs émetteurs de lumière, pompés électriquement, à base de pérovskites hybrides(2018), European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016), 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
Materials science, 02 engineering and technology, Electronic structure, 010402 general chemistry, 01 natural sciences, 7. Clean energy, DFT, Electron transfer, Tetrazine, chemistry.chemical_compound, halide perovskites, Molecule, Moiety, General Materials Science, Electrical and Electronic Engineering, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], HOMO/LUMO, Perovskite (structure), energy transfer, Process Chemistry and Technology, band alignement, Heterojunction, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry, Mechanics of Materials, Chemical physics, tetrazine, 0210 nano-technology
Abstract

International audience; Taking advantage of an innovative design concept for layered halide perovskites with active chromophores acting as organic spacers, we present here the synthesis of two novel two-dimensional (2D) hybrid organic-inorganic halide perovskites incorporating for the first time 100% of a photoactive tetrazine derivative as organic component. Namely, the use of a heterocyclic ring containing a nitrogen proportion imparts a unique electronic structure to the organic component, with lowest energy optical absorption in the blue. The present compound, a tetrazine, presents several resonances between the organic and inorganic components, both in terms of single particle electronic levels and exciton states, providing the ideal playground to discuss charge and energy transfer mechanisms at the organic/inorganic interface. Photophysical studies along with hybrid Time-Dependent DFT simulations demonstrate partial energy transfer and rationalise the suppressed emission from the perovskite frame in terms of different energy-transfer diversion channels, potentially involving both singlet and triplet states of the organic spacer. Periodic DFT simulations also support the feasibility of electron transfers from the conduction band of the inorganic component to the LUMO of the spacer as potential quenching mechanism, suggesting the coexistence and competition of charge and energy transfer mechanisms in these heterostructure. Our work proves the feasibility of inserting photoactive small rings in a 2D perovskite structure, meanwhile providing a robust frame to rationalize the electronic interactions between the semiconducting inorganic layer and organic chromophores, with the prospects of optimizing the organic moiety according to the envisaged application.

Published
2021

14. Perovskite semiconductors for room-temperature exciton-polaritonics

Author

Hai Son Nguyen, Timothy Chi Hin Liew, Qihua Xiong, Zhanghai Chen, Emmanuelle Deleporte, Rui Su, Daniele Sanvitto, Qing Zhang, Antonio Fieramosca, Institut des Nanotechnologies de Lyon (INL), Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-École Centrale de Lyon (ECL), Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), and CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)

Subjects
Materials science, Exciton, Binding energy, Physics::Optics, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Condensed Matter::Materials Science, Polariton, Polaritonics, General Materials Science, ComputingMilieux_MISCELLANEOUS, Perovskite (structure), Condensed Matter::Quantum Gases, [PHYS]Physics [physics], Condensed Matter::Other, business.industry, Mechanical Engineering, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Semiconductor, Mechanics of Materials, Optoelectronics, 0210 nano-technology, business, Thermal energy
Abstract

Lead-halide perovskites are generally excellent light emitters and can have larger exciton binding energies than thermal energy at room temperature, exhibiting great promise for room-temperature exciton-polaritonics. Rapid progress has been made recently, although challenges and mysteries remain in lead-halide perovskite semiconductors to push polaritons to room-temperature operation. In this Perspective, we discuss fundamental aspects of perovskite semiconductors for exciton-polaritons and review the recent rapid experimental advances using lead-halide perovskites for room-temperature polaritonics, including the experimental realization of strong light–matter interaction using various types of microcavities as well as reaching the polariton condensation regime in planar microcavities and lattices. An outlook on the potential of lead-halide perovskites as a playground for exciton-polariton studies and for the development of polaritonic devices operating at room temperature is provided.

Published
2021

15. Energy Tuning of Electronic Spin Coherent Evolution in Methylammonium Lead Iodide Perovskites

Author

Laurent Legrand, Christophe Testelin, M. Chamarro, Emmanuelle Deleporte, Damien Garrot, Guadalupe Garcia-Arellano, Frédérick Bernardot, Gaëlle Trippé-Allard, Thierry Barisien, Institut des Nanosciences de Paris (INSP), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Photonique et cohérence de spin (INSP-E12), and Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Physics, Coherence time, Exciton, 02 engineering and technology, Electron, 021001 nanoscience & nanotechnology, 01 natural sciences, 3. Good health, symbols.namesake, Amplitude, 0103 physical sciences, Faraday effect, symbols, General Materials Science, Physical and Theoretical Chemistry, Atomic physics, 010306 general physics, 0210 nano-technology, Absorption (electromagnetic radiation), ComputingMilieux_MISCELLANEOUS, Perovskite (structure), Spin-½
Abstract

We investigated the coherent evolution of the electronic spin at low temperature in high-quality CH3NH3PbI3 polycrystalline films by picosecond-resolved photoinduced Faraday rotation. We show that this coherent evolution can be tuned by choosing the pump-probe energy within the lowest optical-absorption band, and we explain it as the result of two main contributions: the localized electron and the localized hole. Their corresponding amplitude ratios are not constant across the lowest absorption band-an observation which disqualifies a free exciton from being at the origin of the electronic spin coherent evolution. We measured a spin coherence time of localized electrons (holes) of 4.4 ns (3.7 ns) at 1.635 eV, which evolves to about 7 ns at 1.612 eV (the hole coherence time remains almost constant at lower energies). Finally, we provide a global image of the spin coherent evolution in bulk metal halide perovskite, which overcomes recent controversies.

Published
2021

16. Room-Temperature Cavity Polaritons with 3D Hybrid Perovskite: Toward Large-Surface Polaritonic Devices

Author

Fabien Bretenaker, Gaëlle Trippé-Allard, Hiba Diab, Hai Son Nguyen, Géraud Delport, Emmanuelle Deleporte, Paul Bouteyre, Ali Belarouci, Christian Seassal, Ferdinand Lédée, Jean-Sébastien Lauret, Damien Garrot, INL - Nanophotonique (INL - Photonique), Institut des Nanotechnologies de Lyon (INL), École Centrale de Lyon (ECL), Université de Lyon-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-École Centrale de Lyon (ECL), Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Photonique Quantique et Moléculaire (LPQM), École normale supérieure - Cachan (ENS Cachan)-CentraleSupélec-Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Laboratoire Aimé Cotton, CNRS, ENS Cachan, Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-École Centrale de Lyon (ECL), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Surface (mathematics), Materials science, Nanophotonics, Halide, 02 engineering and technology, bromide hybrid perovskite, 01 natural sciences, 7. Clean energy, polaritonic devices, 010309 optics, [SPI]Engineering Sciences [physics], Photovoltaics, strong coupling, 0103 physical sciences, Polariton, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Electrical and Electronic Engineering, ComputingMilieux_MISCELLANEOUS, Perovskite (structure), business.industry, 021001 nanoscience & nanotechnology, Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials, Solution processed, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Strong coupling, Optoelectronics, exciton−polaritons, 0210 nano-technology, business, Biotechnology
Abstract

International audience; Hybrid halide perovskites are now considered to be key materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining large-surface devices suited to a wide scale of wafers and large-scale integrated devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton−photon coupling with 3D bromide hybrid perovskite. Cavity polaritons are experimentally demonstrated from both reflectivity and photoluminescence experiments, at room temperature, in a 3λ/2 planar microcavity containing a large-surface spin-coated CH 3 NH 3 PbBr 3 thin film. A microcavity quality factor of 92 was found, and a large Rabi splitting of 70 meV was measured. This result paves the way to large-surface and low-cost polaritonic devices operating at room temperature, compatible with electrical injection

Published
2019

17. Tetrazine-incorporating layered halide perovskites featuring type II electronic interface: a small cation with several optical and electronic resonances

Author

Emmanuelle Deleporte, Ferdinand Ledee, Pierre Audebert, Gaëlle Trippé-Allard, Laurent Galmiche, Damien Garrot, Marrot Jérôme, Jean‐sébastien Lauret, Claudine Katan, Jacky Even, Claudio Quarti, Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-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), 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), University of Mons [Belgium] (UMONS), ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), ANR-18-CE24-0016,EMIPERO,Dispositifs émetteurs de lumière, pompés électriquement, à base de pérovskites hybrides(2018), European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016), Université Paris-Saclay, 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 Université de Mons (UMons)

Subjects
[PHYS]Physics [physics], [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract

J.E and J.S.L acknowledges the financial support from the InstitutUniversitaire de France. Computational investigations were conducted thanks to HPC resourcesprovided by [TGCC/CINES/IDRIS] under the allocation 2020-A0010907682 made by GENCI.; National audience; Layered halide perovskites are a class of semiconductors easily produced via chemical approaches and showing unique optical and electronic properties. These materials have a natural quantum-well electronic structure, that is, the band-gap of the inorganic frame is embedded into that of the organic spacers,[1] and feature effective light absorption, positive in-plane transport properties, effective narrow linewidth emission and improved stability against their 3D counterpart.[2] On the other hand, confinement of semiconducting properties in an inorganic is not ideal for applications where photogenerated species are required to effectively travel within the optically active component. This is the typical case of photovoltaics, where ineffective out-of-plane charge transport results in depleted performances for layered halide perovskites, as compared to 3D analogues.[3] In this frame, substituting the (usually) electronic inert organic spacer with organic chromophores featuring extended -conjugated core can pave the way for layered materials showing improved charge and energy transport properties.[4] Indeed, the band-gap closing due to extended -electronic conjugation can result in the (de)stabilization of the frontier orbitals of the spacer, compared to those of the inorganic frame, resulting in the formation of a type II heterojunction at the organic/inorganic interface. Here, we discuss the related charge/energy transfer processes on the basis of recently reported PbX4 (X=Cl,Br) layered perovskite frame incorporating tetrazine derivative as organic spacer.[5] Thanks to the various energy resonances between the inorganic and the organic component, both at the level of the single particle electronic states and at the level of many-body exciton states, this system represents the ideal test case to discuss in the detail charge and energy transfer processes at the type II interface. Furthermore, the incorporation of this novel chromophore as spacer is based on a new design concept, which exploits heterocycles with large fraction of nitrogen, rather than extending the size of carbon-based -core.[6] Photoluminescence (PL) and Photoluminescence Excitation (PLE) measurements indicate partial energy transfer from the inorganic frame to the organic component. Furthermore, cutting-edge, periodic DFT simulations suggest potential exciton ionization as potential responsible for the suppressed light emission from the perovskite frame. REFERENCES[1] C. Katan, et al. Chem. Rev. 2019, 119, 3140−3192[2] M. D. Smith, et al., Chem. Rev. 2019, 119, 3104−3139[3] H. Tsai, et al., Nature 2016, 536, 312–316[4] D. B. Mitzi, et al., Inorg. Chem. 1999, 38, 6246-6256[5] F. Ledée et al., revised manuscript submitted to Mater. Horiz.[6] Y. Gao, Nat. Chem. 2019, 11, 1151–1157

Published
2021

18. Resonant Metasurface for Halide Perovskite-Based Emitting Devices: Extraction Efficiency Enhancement and Radiation Pattern on-Demand

Author

Raphaël Mermet-Lyaudoz, Emmanuel Drouard, Johann Bouclé, Bernard Ratier, Pierre Combeau, Gaëlle Trippé-Allard, Emmanuelle Deleporte, Christian Seassal, Céline Chevalier, Hai Son Nguyen, Institut des Nanotechnologies de Lyon (INL), Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-École Centrale de Lyon (ECL), Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE), RF-ELITE : RF-Electronique Imprimée pour les Télécommunications et l'Energie (XLIM-RFEI), XLIM (XLIM), Université de Limoges (UNILIM)-Centre National de la Recherche Scientifique (CNRS)-Université de Limoges (UNILIM)-Centre National de la Recherche Scientifique (CNRS), Systèmes et Réseaux Intelligents (XLIM-SRI), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), and Bouclé, Johann

Subjects
[PHYS.PHYS.PHYS-OPTICS] Physics [physics]/Physics [physics]/Optics [physics.optics], [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], [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], [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], ComputingMilieux_MISCELLANEOUS
Abstract

National audience

Published
2021

19. Renormalization of the valence and conduction bands of (C6H5C2H4NH3)(2)PbI4 hybrid perovskite

Author

A Barragán, J.-M. Themlin, Hela Mrezguia, Maya N. Nair, J. Minár, Saleem Ayaz Khan, L. Giovanelli, Gaëlle Trippé-Allard, Antonio Tejeda, Hamza Khelidj, Ferdinand Lédée, Amina Taleb-Ibrahimi, Min-I Lee, Emmanuelle Deleporte, Younal Ksari, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), University of West Bohemia [Plzeň ], Institut des Matériaux, de Microélectronique et des Nanosciences de Provence (IM2NP), Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), and Aix Marseille Université (AMU)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS)

Subjects
spin–orbit coupling, (C6H5C2H4NH3)2PbI4, Materials science, Acoustics and Ultrasonics, Photoemission spectroscopy, Inverse photoemission spectroscopy, Angle-resolved photoemission spectroscopy, 02 engineering and technology, Electronic structure, 7. Clean energy, 01 natural sciences, Renormalization, inverse photoemission spectroscopy, Condensed Matter::Materials Science, Photovoltaics, Condensed Matter::Superconductivity, 2D hybrid organic-inorganic perovskites, 0103 physical sciences, angle-resolved photoemission spectroscopy, phenylethylammonium lead iodine, 010306 general physics, Perovskite (structure), Valence (chemistry), Condensed matter physics, business.industry, k-resolved band structures, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Condensed Matter::Strongly Correlated Electrons, 0210 nano-technology, business
Abstract

International audience; Quasi two-dimensional hybrid organic-inorganic perovskites (HOIPs) have been rediscovered recently for photovoltaics due to a higher stability than other HOIPs. We focus here on the electronic structure of the 2D perovskite (C6H5C2H4NH3)2PbI4. We perform an experimental k-resolved determination of the valence and conduction bands by angle-resolved photoemission spectroscopy (ARPES) and inverse photoemission spectroscopy (IPES). The experimental and theoretical dispersions are compared. The valence band width is in agreement with that of renormalized theoretical bands, while no significative renormalization is observed for the conduction band. The effect of the spin-orbit coupling in the conduction band is also experimentally observed.

Published
2021

20. Realization of Polaritonic Topological Charge at Room Temperature Using Polariton Bound States in the Continuum from Perovskite Metasurface (Advanced Optical Materials 6/2022)

Author

Nguyen Ha My Dang, Simone Zanotti, Emmanuel Drouard, Céline Chevalier, Gaëlle Trippé‐Allard, Mohamed Amara, Emmanuelle Deleporte, Vincenzo Ardizzone, Daniele Sanvitto, Lucio Claudio Andreani, Christian Seassal, Dario Gerace, and Hai Son Nguyen

Subjects
Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials
Published
2022

21. Revealing Excitonic Phonon Coupling in (PEA)

Author

Joanna M, Urban, Gabriel, Chehade, Mateusz, Dyksik, Matan, Menahem, Alessandro, Surrente, Gaëlle, Trippé-Allard, Duncan K, Maude, Damien, Garrot, Omer, Yaffe, Emmanuelle, Deleporte, Paulina, Plochocka, and Michal, Baranowski

Abstract

The family of 2D Ruddlesden-Popper perovskites is currently attracting great interest of the scientific community as highly promising materials for energy harvesting and light emission applications. Despite the fact that these materials are known for decades, only recently has it become apparent that their optical properties are driven by the exciton-phonon coupling, which is controlled by the organic spacers. However, the detailed mechanism of this coupling, which gives rise to complex absorption and emission spectra, is the subject of ongoing controversy. In this work we show that the particularly rich, absorption spectra of (PEA)

Published
2020

22. Tailoring Dispersion of Room-Temperature Exciton-Polaritons with Perovskite-Based Subwavelength Metasurfaces

Author

Nguyen Ha My Dang, Christian Seassal, Hai Son Nguyen, Emmanuelle Deleporte, Emmanuel Drouard, Dario Gerace, Radoslaw Mazurczyk, Gaëlle Trippé-Allard, Ferdinand Lédée, Institut des Nanotechnologies de Lyon (INL), Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-École Centrale de Lyon (ECL), Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Laboratoire Aimé Cotton (LAC), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), INL - Nanophotonique (INL - Photonique), and Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon)

Subjects
Quantum fluid, Photoluminescence, Materials science, Exciton, Nanophotonics, FOS: Physical sciences, Physics::Optics, Bioengineering, Applied Physics (physics.app-ph), 02 engineering and technology, Exciton-polaritons, 7. Clean energy, polaritonic devices, Condensed Matter::Materials Science, Lattice (order), Mesoscale and Nanoscale Physics (cond-mat.mes-hall), General Materials Science, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, Rigorous coupled-wave analysis, ComputingMilieux_MISCELLANEOUS, Condensed Matter::Quantum Gases, Condensed Matter - Mesoscale and Nanoscale Physics, business.industry, Condensed Matter::Other, Mechanical Engineering, General Chemistry, Physics - Applied Physics, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Condensed Matter::Mesoscopic Systems and Quantum Hall Effect, metasurfaces, Strong coupling regime, exciton-polaritons, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Optoelectronics, nanophotonics, Photonics, 0210 nano-technology, business, 2D layered perovskites, Optics (physics.optics), Physics - Optics
Abstract

Exciton-polaritons, elementary excitations arising from the strong coupling regime between photons and excitons in insulators or semiconductors, represent a promising platform for studying quantum fluids of light and realizing prospective all-optical devices. Among different materials for room temperature polaritonic devices, two-dimensional (2D) layered perovskites have recently emerged as one of the promising candidates thanks to their prominent excitonic features at room temperature. Here we report on the experimental demonstration of exciton-polaritons at room temperature in resonant metasurfaces made from a subwavelength 2D lattice of perovskite pillars. These metasurfaces are obtained via spincoating, followed by crystallization of the perovskite solution in a pre-patterned glass backbone. The strong coupling regime is revealed by both angular-resolved reflectivity and photoluminescence measurements, showing anticrossing between photonic modes and the exciton resonance with a Rabi splitting in the 200 meV range. Moreover, we show that the polaritonic dispersion can be engineered by tailoring the photonic Bloch mode to which perovskite excitons are coupled. Linear, parabolic, and multi-valley polaritonic dispersions are experimentally demonstrated. All of our results are perfectly reproduced by both numerical simulations based on a rigorous coupled wave analysis and an elementary model based on a quantum theory of radiation-matter interaction. Our results suggest a new approach to study exciton-polaritons and pave the way towards large-scale and low-cost integrated polaritonic devices operating at room temperature.

Published
2020

23. Directing random lasing emission using cavity exciton-polaritons

Author

Géraud Delport, Fabien Bretenaker, Jean-Sébastien Lauret, Emmanuelle Deleporte, Gaëlle Trippé-Allard, Hiba Diab, Hai Son Nguyen, Christian Seassal, Paul Bouteyre, Ferdinand Lédée, Damien Garrot, Ali Belarouci, Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Institut des Nanotechnologies de Lyon (INL), Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées de Lyon (INSA Lyon), Université de Lyon-Institut National des Sciences Appliquées (INSA)-Université de Lyon-Institut National des Sciences Appliquées (INSA)-École Centrale de Lyon (ECL), Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École supérieure de Chimie Physique Electronique de Lyon (CPE), Groupe d'Etude de la Matière Condensée (GEMAC), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)

Subjects
FOS: Physical sciences, Physics::Optics, 02 engineering and technology, Exciton-polaritons, Molecular physics, 01 natural sciences, Light scattering, law.invention, 010309 optics, Optics, [PHYS.QPHY]Physics [physics]/Quantum Physics [quant-ph], law, 0103 physical sciences, Spontaneous emission, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS, Photonic crystal, Physics, [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Random laser, business.industry, Resonance, 021001 nanoscience & nanotechnology, Laser, Atomic and Molecular Physics, and Optics, 3. Good health, Optoelectronics, 0210 nano-technology, business, Lasing threshold, Optics (physics.optics), Physics - Optics
Abstract

Random lasing is an intriguing phenomenon occurring in disordered structures with optical gain. In such lasers, the scattering of light provides the necessary feedback for lasing action. Because of the light scattering, the random lasing systems emit in all the directions in contrast with the directional emission of the conventional lasers. While this property can be desired in some cases, the control of the emission directionality remains required for most of the applications. Besides, it is well known that the excitation of cavity exciton-polaritons is intrinsically directional. Each wavelength (energy) of the cavity polariton, which is a superposition of an excitonic state and a cavity mode, corresponds to a well-defined propagation direction. We demonstrate in this article that coupling the emission of a 2D random laser with a cavity polaritonic resonance permits to control the direction of emission of the random laser. This results in a directional random lasing whose emission angle with respect to the microcavity axis can be tuned in a large range of angles by varying the cavity detuning. The emission angles reached experimentally in this work are 15.8$^\circ$ and 22.4$^\circ$., Article : 10 pages, 5 figures Supplementary : 11 pages, 14 figures

Published
2020

24. Hybrid perovskites for photovoltaics and optoelectronics

Author

Wallace C. H. Choy, Emmanuelle Deleporte, Michael Grätzel, Antonio Tejeda, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), The University of Hong Kong (HKU), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), and Ecole Polytechnique Fédérale de Lausanne (EPFL)

Subjects
Materials science, Acoustics and Ultrasonics, business.industry, Nanotechnology, 010402 general chemistry, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Photovoltaics, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], business, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2020

25. Revealing Excitonic Phonon Coupling in (PEA)2(MA)n-1PbnI3n+1 2D Layered Perovskites

Author

Damien Garrot, Omer Yaffe, Gabriel Chehade, Gaëlle Trippé-Allard, Alessandro Surrente, Mateusz Dyksik, Joanna Urban, Emmanuelle Deleporte, Matan Menahem, Paulina Plochocka, Duncan K. Maude, Michal Baranowski, Laboratoire national des champs magnétiques intenses - Toulouse (LNCMI-T), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), Laboratoire Lumière, Matière et Interfaces (LuMIn), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Nano Optique et Spectroscopy (NOOS), CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay)-CentraleSupélec-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Wroclaw University of Science and Technology, Weizmann Institute of Science [Rehovot, Israël], Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), ANR-11-IDEX-0002,UNITI,Université Fédérale de Toulouse(2011), ANR-18-CE24-0006,LEOPAR,Unité de pré-traitement pour systèmes intégrés à faible énergie(2018), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)

Subjects
Materials science, Absorption spectroscopy, Phonon, Metal halide perovskites, exciton-phonon coupling, magneto optical spectroscopy, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Condensed Matter::Materials Science, Coupling (physics), Chemical physics, General Materials Science, Light emission, Emission spectrum, Physical and Theoretical Chemistry, 0210 nano-technology, Absorption (electromagnetic radiation), Perovskite (structure)
Abstract

International audience; The family of 2D Ruddlesden-Popper perovskites is currently attracting great interest of the scientific community as highly promising materials for energy harvesting and light emission applications. Despite the fact that these materials are known for decades, only recently has it become apparent that their optical properties are driven by the exciton-phonon coupling, which is controlled by the organic spacers. However, the detailed mechanism of this coupling, which gives rise to complex absorption and emission spectra, is the subject of ongoing controversy. In this work we show that the particularly rich, absorption spectra of (PEA)2(CH3NH3)n-1PbnI3n+1 (where PEA stands for phenylethylammonium and n = 1, 2, 3), are related to a vibronic progression of excitonic transition. In contrast to other two-dimensional perovskites, we observe a coupling to a high-energy (40 meV) phonon mode probably related to the torsional motion of the NH3+ head of the organic space

Published
2020

26. Exciton Recombination and Annihilation in Pure-Phase Phenylethylammonium Based 2D-Layered Hybrid Perovskite Crystals

Author

Emmanuelle Deleporte, Geraud Delport, Gabriel Chehade, Ferdinand Lédée, Hiba Diab, Gaëlle Trippé-Allard, Jacky Even, Jean‐sébastien Lauret, Damien Garrot, Ecole Normale Supérieure Paris-Saclay (ENS Paris Saclay), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-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)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), 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)-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
2019

27. Les pérovskites hybrides : des excitons sur mesure pour l’optoélectronique

Author

Emmanuelle Deleporte

Abstract

Veritables stars des conferences d’optoelectronique depuis deja 5 ans, les perovskites hybrides apparaissent comme une nouvelle classe de semiconducteurs qui montrent des performances exceptionnelles, donnant l’espoir de produire des dispositifs photoniques efficaces a faible cout et flexibles. Le materiau ayant emerge il y a peu, ses declinaisons chimiques, sa qualite cristalline et ses proprietes photophysiques representent un grand champ d’investigation pour les physiciens et les chimistes.

Published
2017

28. Fast growth of monocrystalline thin films of 2D layered hybrid perovskite

Author

Ferdinand Lédée, Emmanuelle Deleporte, Damien Garrot, Pierre Audebert, Jean-Sébastien Lauret, Gaëlle Trippé-Allard, Hiba Diab, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Mineralogy, Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 7. Clean energy, 01 natural sciences, Aspect ratio (image), 0104 chemical sciences, law.invention, Monocrystalline silicon, Hybrid perovskites, law, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], monocrystalline film, General Materials Science, Crystallization, Thin film, 0210 nano-technology, Perovskite (structure)
Abstract

International audience; During the past few years hybrid organic-inorganic perovskites (HOIPs) have attracted much interest as solution-processed semiconductors with high potentialities in optoelectronics and photovoltaics. On the one hand 3D HOIPs such as CH3NH3PbI3 have shown their outstanding performances when incorporated in solar cells [1]. On the other hand their 2D layered counterparts such as (C6H5C2H4NH3)2PbI4 (PEPI) are promising materials for light emitting devices because of their strong emission at room temperature [2]. However, the optoelectronic properties of hybrid perovskite polycrystalline films suffer from a microscale grain structure. In order to take advantage of the great potential of these materials for both photovoltaics and emitting devices, the synthesis of large monocrystalline films is a key issue. Here we propose a fast crystallization method for the 2D layered hybrid perovskite PEPI. A vapor-assisted process coupled with a capping of the precursor solution allows to grow 2-dimensionnal thin films with millimetric monocrystalline grains, a high aspect ratio and a good surface quality (Fig.1). Moreover, this growth is several orders of magnitudes faster than the other reported techniques. In addition, we highlight the benefits of using γ-butyrolactone (GBL) for the growth of layered perovskites monocrystalline grains.

Published
2017

29. Exciton-Exciton Annihilation in Two-dimensional Halide Perovskites at Room Temperature

Author

Jacky Even, Emmanuelle Deleporte, Damien Garrot, Cosme Milesi-Brault, Jean-Sébastien Lauret, Gaëlle Trippé-Allard, Hiba Diab, Géraud Delport, Ferdinand Lédée, Gabriel Chehade, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), 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), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), ANR-10-04, Agence Nationale de la Recherche, 687008, H2020 Future and Emerging Technologies, ANR-18-CE24-0016,EMIPERO,Dispositifs émetteurs de lumière, pompés électriquement, à base de pérovskites hybrides(2018), European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), 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)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Exciton, Graphical TOC Entry Keywords Halide Perovskite, Halide, 02 engineering and technology, Exciton Dynamics, engineering.material, 010402 general chemistry, 7. Clean energy, 01 natural sciences, law.invention, Ruddlesden-Popper phase, law, Exciton-Exciton Annihilation, [CHIM]Chemical Sciences, General Materials Science, Physical and Theoretical Chemistry, Perovskite (structure), Diode, [PHYS]Physics [physics], Annihilation, Condensed matter physics, 021001 nanoscience & nanotechnology, 0104 chemical sciences, engineering, Ruddlesden-Popper Phase, Defect, 0210 nano-technology, Light-emitting diode
Abstract

International audience; Recently, Ruddlesden–Popper 2D perovskite (RPP) solar cells and light-emitting diodes (LEDs) have shown promising efficiencies and improved stability in comparison to 3D halide perovskites. Here, the exciton recombination dynamics is investigated at room temperature in pure-phase RPP crystals (C6H5C2H4NH3)2(CH3NH3)n−1PbnI3n+1 (n = 1, 2, 3, and 4) by time-resolved photoluminescence (TRPL) in a large range of power excitations. As the number of perovskite layers increases, we detect the presence of an increasing fraction of out-of-equilibrium free carriers just after photoexcitation, on a picosecond time scale, while the dynamics is characterized by the recombination of excitons with long lifetime spanning several tens of nanoseconds. At low excitation power, the TRPL decays are nonexponential because of defect-assisted recombination. At high fluence, defects are filled and many-body interactions become important. Similar to other 2D systems, exciton–exciton annihilation (EEA) is then the dominant recombination path in a high-density regime below the Mott transition.

Published
2019

30. New long-range sub-structure found in the tetragonal phase of CH3NH3PbI3 single crystals

Author

Olivier Plantevin, Damien Garrot, D. Le Bolloc'h, Pierre Fertey, Antonio Tejeda, Gaëlle Trippé-Allard, A Gallo-Frantz, Emmanuelle Deleporte, Ferdinand Lédée, Vincent Jacques, Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Centre de Sciences Nucléaires et de Sciences de la Matière (CSNSM), Centre National de la Recherche Scientifique (CNRS)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Université Paris-Sud - Paris 11 (UP11), and Université Paris-Sud - Paris 11 (UP11)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Diffraction, Materials science, Acoustics and Ultrasonics, Condensed matter physics, Scattering, business.industry, Phase (waves), 02 engineering and technology, Semiconductor device, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Monocrystalline silicon, Tetragonal crystal system, Semiconductor, 0103 physical sciences, X-ray crystallography, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 010306 general physics, 0210 nano-technology, business
Abstract

International audience; Hybrid organic-inorganic perovskites have become one of the most promising low-cost alternatives to traditional semiconductors in the field of photovoltaics and light emitting devices. It combines both attractive features of organic and inorganic materials within a single composite, for instance with excellent electronic properties. We used x-ray diffraction to reveal a sub-structure within CH 3 NH 3 PbI 3 single crystals. We could observe the presence of additional peaks with a square symmetry in several monocrystalline samples. We discuss these results in terms of two different models: a superstructure modulated in two in-plane orthogonal directions, and a model with tilted domains with a shallow angle of ~0.6°. In both cases, the modulated or tilted domains appear in regions with small lattice expansion. We show that this last model appears to be the most likely to explain our observations.

Published
2019

31. Photoluminescence Tuning Through Irradiation Defects in CH$_3$NH$_3$PbI$_3$ Perovskites

Author

Driffa Guerfa, Ferdinand Lédée, Gaëlle Trippé-Allard, Emmanuelle Deleporte, Olivier Plantevin, Damien Garrot, Stéphanie Valère, Centre de Sciences Nucléaires et de Sciences de la Matière (CSNSM), Université Paris-Sud - Paris 11 (UP11)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), and École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Photoluminescence, Materials science, FOS: Physical sciences, 02 engineering and technology, Applied Physics (physics.app-ph), 01 natural sciences, Tetragonal crystal system, 0103 physical sciences, [CHIM.CRIS]Chemical Sciences/Cristallography, Irradiation, Spectroscopy, defects, hybrid perovskites, 010302 applied physics, [PHYS]Physics [physics], Condensed Matter - Materials Science, business.industry, ion irradiation, Materials Science (cond-mat.mtrl-sci), Physics - Applied Physics, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Crystallographic defect, Electronic, Optical and Magnetic Materials, Semiconductor, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Optoelectronics, Light emission, photoluminescence, Crystallite, 0210 nano-technology, business
Abstract

International audience; Defect engineering is applied to hybrid (CH3NH3)PbI3 organic–inorganic perovskites. These materials have become one of the most promising low‐cost alternatives to traditional semiconductors in the field of photovoltaics and light emitting devices. Here Helium ion irradiation at low energy has been used as a tool for the controlled introduction of point defects in both single crystals and polycrystalline thin films. The irradiation defects modify the opto‐electronic properties as probed using photoluminescence (PL) spectroscopy from 10 K to room‐temperature. Contrary to usual semiconductors, a very good resilience of the PL properties with irradiation is observed, even associated to an enhancement of the optical emission at low temperature. These results are discussed in relation with the tetragonal to orthorhombic low‐temperature phase transition below T = 160 K. A comparison between spectra from single crystals and polycrystalline films, both with and without irradiation defects, allows a better understanding of the light emission mechanisms in both kinds of samples. The authors thereby evidence radiation hardness of these materials and the specificity of defects and their impact on light emission properties.

Published
2019

32. Multinuclear NMR as a tool for studying local order and dynamics in CH3NH3PbX3(X = Cl, Br, I) hybrid perovskites

Author

Thierry Bataille, Claudine Katan, Jean-Claude Ameline, Laurent Le Pollès, Emmanuelle Deleporte, Bruno Alonso, Khaoula Jemli, Régis Gautier, Claire Roiland, Gaëlle Trippé-Allard, Jacky Even, Institut des Sciences Chimiques de Rennes (ISCR), 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), Laboratoire Aimé Cotton (LAC), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Fonctions Optiques pour les Technologies de l'informatiON (FOTON), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Université européenne de Bretagne - European University of Brittany (UEB)-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)-Télécom Bretagne, Cellule Energie du CNRS (SOLHYBTRANS Project)University of Rennes 1 (Action Incitative, D ́efis Scientifiques Emergents 2015). Banque Populaire de l’Ouest for its financial support (Grant PEROPHOT 2015). Rennes Métropole and Région Betagne (FEDER), European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016), 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)-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)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), 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)-Télécom Bretagne-Centre National de la Recherche Scientifique (CNRS), 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 Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Université européenne de Bretagne - European University of Brittany (UEB)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Télécom Bretagne-Centre National de la Recherche Scientifique (CNRS)

Subjects
Deuterium NMR, Phase transition, Carbon-13 NMR satellite, Chemistry, Analytical chemistry, General Physics and Astronomy, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, Fluorine-19 NMR, Nuclear magnetic resonance spectroscopy, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, Carbon-13 NMR, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Transverse relaxation-optimized spectroscopy, Physical and Theoretical Chemistry, 0210 nano-technology, Perovskite (structure)
Abstract

We report on 207Pb, 79Br, 14N, 1H, 13C and 2H NMR experiments for studying the local order and dynamics in hybrid perovskite lattices. 207Pb NMR experiments conducted at room temperature on a series of MAPbX3 compounds (MA = CH3NH3+; X = Cl, Br and I) showed that the isotropic 207Pb NMR shift is strongly dependent on the nature of the halogen ions. Therefore 207Pb NMR appears to be a very promising tool for the characterisation of local order in mixed halogen hybrid perovskites. 207Pb NMR on MAPbBr2I served as a proof of concept. Proton, 13C and 14N NMR experiments confirmed the results previously reported in the literature. Low temperature deuterium NMR measurements, down to 25 K, were carried out to investigate the structural phase transitions of MAPbBr3. Spectral lineshapes allow following the successive phase transitions of MAPbBr3. Finally, quadrupolar NMR lineshapes recorded in the orthorhombic phase were compared with simulated spectra, using DFT calculated electric field gradients (EFG). Computed data do not take into account any temperature effect. Thus, the discrepancy between the calculated and experimental EFG evidences the fact that MA cations are still subject to significant dynamics, even at 25 K.

Published
2016

33. Exciton dynamics in 2D layered Hybrid Perovskites Crystals

Author

Géraud Delport, Ferdinand Lédée, Hiba Diab, Cosmes Milesi Brault, Gaëlle Trippé-Allard, Jean‐sébastien Lauret, Emmanuelle Deleporte, Damien Garrot, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Groupe d'Etude de la Matière Condensée (GEMAC), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract

International audience; Over the past few years, organic-inorganic halide 3D perovskites (3D-HOP) were found to present remarkable optoelectronic properties. A great attention has been paid to perovskites thin films, as an ideal building block for PV and LED devices. On the other hand, the study of single crystals has proven necessary to unveil some of the intrinsic properties of these semiconductors [1,2]. While the 2D perovskites have been known for decades, they are attracting growing interest, for their strong PL properties, their chemical versatility and their low sensitivity to external degradation mechanisms due to UV light and moisture. Monocrystalline thin films of phenylethylammonium-based 2D perovskites (C 6 H 5 C 2 H 4 NH 3) 2 PbI 4 and their 2D/3D derivatives are produced using the "Anti-solvent Vapor Assisted Capping Crystalllization [3]. A cryogenic micro-photoluminescence study of these samples will be presented (with a sub micrometer precision), allowing to extract the intrinsic properties of the perovskite crystals, such as electron-phonon coupling and the PL lifetimes. This technique allows in particular to finely correlate the optoelectronic properties of the produced films with their morphology. The optoelectronic properties of these monocrystalline thin films will be compared to the ones of spin-coated polycrystalline perovskites films. They will be also compared to the ones published on butylammonium-based 2D perovskites, that were recently used to create efficient and longed-lived solar cells [4].

Published
2018

34. Micro-photoluminescence study of 2D-layered hybrid perovskite monocrystalline thin films. Correlation between the structural and optoelectronics properties

Author

Géraud Delport, Ferdinand Lédée, Hiba Diab, Cosme Milesi Brault, Gaëlle Trippé-Allard, Jean‐sébastien Lauret, Emmanuelle Deleporte, Damien Garrot, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Groupe d'Etude de la Matière Condensée (GEMAC), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract

International audience; Over the past few years, organic-inorganic halide 3D perovskites (3D-HOP) were found to present remarkable optoelectronic properties. A great attention has been paid to perovskites thin films, as an ideal building block for PV and LED devices. On the other hand, the study of single crystals has proven necessary to unveil some of the intrinsic properties of these semiconductors [1,2]. While the 2D perovskites have been known for decades, they are attracting growing interest, for their strong PL properties, their chemical versatility and their low sensitivity to external degradation mechanisms due to UV light and moisture. Monocrystalline thin films of phenylethylammonium-based 2D perovskites (C 6 H 5 C 2 H 4 NH 3) 2 PbI 4 and their 2D/3D derivatives are produced using the "Anti-solvent Vapor Assisted Capping Crystalllization [3]. A cryogenic micro-photoluminescence study of these samples will be presented (with a sub micrometer precision), allowing to extract the intrinsic properties of the perovskite crystals, such as electron-phonon coupling and the PL lifetimes. This technique allows in particular to finely correlate the optoelectronic properties of the produced films with their morphology. The optoelectronic properties of these monocrystalline thin films will be compared to the ones of spin-coated polycrystalline perovskites films. They will be also compared to the ones published on butylammonium-based 2D perovskites, that were recently used to create efficient and longed-lived solar cells [4].

Published
2018

35. Time-resolved microphotoluminescence study of 2D layered hybrid perovskites crystals. Correlation between the structural and optical properties

Author

Géraud Delport, Ferdinand Lédée, Hiba Diab, Cosmes Milesi Brault, Gaëlle Trippé-Allard, Jean‐sébastien Lauret, Emmanuelle Deleporte, Damien Garrot, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), and DELEPORTE, Emmanuelle

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; Over the past few years, organic-inorganic halide 3D perovskites (3D-HOP) were found to present remarkable optoelectronic properties. In particular, the efficiency of perovskite solar cells rivals now with commercial silicon solar cells. However, their instability in presence of moisture and under irradiation hinders their practical applications. There is currently a renewed interest in 2D layered hybrid perovskites (2D-HOP) due to their chemical versatility and stability. They consist in natural self-assembled quantum well where the perovskite layers are separated by bulky organic cations. Recently, solar cells based on low-dimensional perovskites have demonstrated high efficiency and improved stability. [1] However, the fundamental photophysics of 2D-HOP is not fully understood. A great attention has been paid to thin films, which present generally multiple phases and grain boundaries, as an ideal building block for PV and LED devices. Nevertheless, the study of crystals has proven necessary to unveil some of the intrinsic properties of hybrid perovskites. [2,3] In this work, we have studied the optical properties of 2D layered perovskites crystals of (C 6 H 5 C 2 H 4 NH 3) 2 (CH 3 NH 3) n-1 Pb n I 3n+1 (n=1,2 and 3) (Fig. 1) using time-resolved microphotoluminescence as function of temperature. The emission properties are correlated with the material morphology. Analysis of the fluence and temperature dependence of the photoluminescence decay provides insight into the exciton recombination dynamics in low-dimensional perovskites.

Published
2018

36. Mode-Locked all-fiber laser using Two-Dimensional Perovskite in C and L band

Author

Jaedoek Park, Kyunghwan Oh, Sanggwon Song, Emmanuelle Deleporte, Dong-Il Yeom, Seongjing Hong, and Ferdinand Lédée

Subjects
Optical fiber, Materials science, business.industry, Soliton (optics), Saturable absorption, 02 engineering and technology, Laser, law.invention, 020210 optoelectronics & photonics, Mode-locking, law, Fiber laser, 0202 electrical engineering, electronic engineering, information engineering, Optoelectronics, business, Ultrashort pulse, Perovskite (structure)
Abstract

Using two-dimensional (2D) hybrid organic-inorganic (C 6 H 5 C 2 H 4 NH 3 ) 2 PbI 4 perovskite thin film as an in-line saturable absorber, we experimentally demonstrate an all-fiber mode-locked laser in both C and L band. We successfully generated self-started ultrafast pulses at the anomalous dispersion regime with a spectral bandwidth of 7 nm and a pulse duration of 381 fs at the center wavelength of 1565.9 nm. Moreover, by adjusting the optical gain, we also achieve a transform-limited soliton pulses with the spectral bandwidth of 6 nm at the center wavelength of 1604 nm.

Published
2018

37. Feature issue introduction : halide perovskites for optoelectronics

Author

Thomas P. White, Emmanuelle Deleporte, Tze Chien Sum, and School of Physical and Mathematical Sciences

Subjects
Photoluminescence, Materials science, Computer science, Semiconductor materials, Halide, Photodetector, 02 engineering and technology, 01 natural sciences, law.invention, 010309 optics, chemistry.chemical_compound, law, Physics [Science], Optical materials, 0103 physical sciences, Optoelectronics, Perovskite (structure), business.industry, Halide Perovskites, Nonlinear optics, Laser, 021001 nanoscience & nanotechnology, Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials, Perovskite, chemistry, Thin film solar cell, 0210 nano-technology, business, Light-emitting diode
Abstract

This joint Optics Express and Optical Materials Express feature issue presents a collection of nine papers on the topic of halide perovskites for optoelectronics. Perovskite materials have attracted significant attention over the past four years, initially for their outstanding performance in thin film solar cells, but more recently for applications in light-emitting devices (LEDs and lasers), photodetectors and nonlinear optics. At the same time, there is still much more to learn about the fundamental properties of these materials, and how these depend on composition, processing, and exposure to the environment. This feature issue provides a snapshot of some of the latest research in this rapidly-evolving multidisciplinary field. Published version

Published
2018

38. Solid-State Physics Perspective on Hybrid Perovskite Semiconductors

Author

Jacky Even, Mikael Kepenekian, Laurent Pedesseau, Jean-Sébastien Lauret, Emmanuelle Deleporte, Daniel Sapori, Claudine Katan, Fonctions Optiques pour les Technologies de l'informatiON (FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Université européenne de Bretagne - European University of Brittany (UEB)-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)-Télécom Bretagne-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), 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)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), This work was performed using HPC resources from GENCI-CINES/IDRIS grant 2014-c2012096724. The work is supported by Cellule Energie du CNRS (SOLHYBTRANS Project)., ANR-10-BLAN-1001,PEROCAI,Pérovskites en cavité(2010), Université de Rennes (UR)-Université européenne de Bretagne - European University of Brittany (UEB)-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)-Télécom Bretagne-Centre National de la Recherche Scientifique (CNRS), 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 École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Solid-state physics, Point reflection, 02 engineering and technology, Dielectric, 010402 general chemistry, 01 natural sciences, Condensed Matter::Materials Science, Lattice (order), Quantum mechanics, Physical and Theoretical Chemistry, Perovskite (structure), [PHYS]Physics [physics], Physics, Condensed matter physics, business.industry, Heterojunction, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, General Energy, Semiconductor, Condensed Matter::Strongly Correlated Electrons, Density functional theory, 0210 nano-technology, business
Abstract

International audience; In this review we examine recent theoretical investigations on 2D and 3D hybrid perovskites (HOP) that combine classical solid-state physics concepts and density functional theory (DFT) simulations as a tool for studying their optoelectronic properties. Such an approach allows one to define a new class of semiconductors, where the pseudocubic high temperature perovskite structure plays a central role. Bloch states and k.p Hamiltonians yield new insight into the influence of lattice distortions, including loss of inversion symmetry, as well as spin-orbit coupling. Electronic band folding and degeneracy, effective masses and optical absorption are analyzed. Concepts of Bloch and envelope functions, as well as confinement potential are discussed in the context of layered HOP and 3D HOP heterostructures. Screening and dielectric confinements are important for room temperature optical properties of 3D and layered HOP, respectively. Non-radiative Auger effects are analyzed for the first time close to the electronic band gap of 3D hybrid perovskites.

Published
2015

39. Photophysics of self-assembled luminophore-perovskite systems

Author

Ferdinand Lédée, Gaëlle Trippé-Allard, Géraud Delport, Jean‐sébastien Lauret, Damien Garrot, Emmanuelle Deleporte, Pierre Audebert, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), and École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.MATE]Chemical Sciences/Material chemistry
Abstract

International audience; During the past few years hybrid organic-inorganic perovskites (HOIPs) have attracted much interest as solution-processed semiconductors with high potentialities in optoelectronics. On the one hand “3D” HOIPs such as CH3NH3PbI3 have shown their outstanding performances when incorporated in solar cells [1]. On the other hand their “2D layered” counterparts (R-NH3)2PbI4, where R is an organic group, are promising materials for light emitting devices such as LEDs [2] and Lasers [3]. Indeed their self-assembled, multilayered structure allows strong excitonic emission at room temperature (fig. 1). They offer moreover much flexibility with respect to the organic group R. While most of the reported 2D layered perovskites have optically inactive organic moieties, a huge improvement of the performances could be done by introducing functional organic groups. This is why we propose in the present work two innovative luminophore-perovskite systems. First by introducing 2,3-naphthalimide-ethylammonium (NAAB) fluorescent molecules in the perovskite structure we efficiently improved its excitonic emission [4]. Secondly thanks to the perovskite self-assembling we succesfully templated tetrazine molecules into the perovskite structure and changed their optical properties (fig. 2).

Published
2017

40. Experimental valence band dispersion of CH3NH3PbI3 hybrid organic-inorganic perovskite

Author

Min-I Lee, Barragán, A. N., Nair, M. N., Jacques, V., D. Le Bolloc'H, Fertey, P., Jemli, K., Lédée, F., Gaëlle Trippé-Allard, Emmanuelle Deleporte, Taleb-Ibrahimi, A., Tejeda, A. N., Laboratoire de Physique des Solides (LPS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), and Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan)

Subjects
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract

International audience; Organic-inorganic hybrid perovskites are promising absorber materials for low-cost photovoltaic solar cells or optoelectronic devices [1-4]. Among these perovskites, methylammonium triiodideplumbate (CH 3 NH 3 PbI 3 , MAPbI 3 or MAPI) exhibits currently the highest efficiency. Here we have analyzed the structural transition in MAPI by X-ray diffraction at the β phase and we have correlated it to its electronic properties. Despite all the extensive work on hybrid organic-inorganic halide perovskites, their experimental band structure measured with k-resolution has remained elusive. Such an experimental determination is a necessary requirement for an accurate theoretical description and understanding of the system. The impact of the structural phase transitions on the band structure in the operation temperature range of solar cells needed also to be elucidated. Herein, we present the experimental determination of the band structure of MAPI with k resolution by angle-resolved photoemission at 170 K [5]. Our results show that the spectral weight is strongly affected by the cubic symmetry although traces of the tetragonal band structure are appreciated. Some deviations with respect to theoretical calculations are observed, which may help to reach a more precise description of this paradigmatic system of the hybrid perovskite family. The project leading to this application has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 687008 (GOTSolar).

Published
2017

41. Excitonic emission of hybrid lead iodide perovskite single crystals

Author

Emmanuelle Deleporte, Hiba Diab, Gaëlle Trippé-Allard, Ferdinand Lédée, Guillaume Bouchez, Christèle Vilard, Jacques, Vincent L. R., Antonio Tejeda, Pierre Audebert, Jean‐sébastien Lauret, Damien Garrot, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), and DELEPORTE, Emmanuelle

Subjects
excitons, Hybrid perovskites, [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; Since 2012, the 3D Hybrid Organic Perovskites of formula CH3NH3PbI3 and their derivatives represent a “material breakthrough” for photovoltaïcs: in only 3 years, the efficiency of 3D HOP-based solar cells has progressed from 12% to more than 20%. These HOP molecules appear also very attractive for light-emitting devices such as electroluminescent diodes and lasers.Improvement of the performance of perovskite solar cells and optoelectronic devices may benefit from a better understanding of the intrinsic photophysics of materials. However, the properties of films are very dependent of the grain structure. We will focus here on the synthesis of HOP single crystals and we will study their optical properties. The optical properties of a millimetric CH3NH3PbI3 single crystal are compared to those of thin polycrystalline films. In particular, the main feature in single crystals is the appearance, in the low temperature luminescence spectra, of a sharp emission line (FWHM ~ 5 meV) at high energy which is attributed to the free exciton signature (figure 1). Experiments performed as a function of temperature confirm the existence of a strong electron-phonon coupling. We highlight the extremely high stability of the single crystals compared to the thin layers: defects and grain boundaries are then thought to play an important role in the degradation mechanism.

Published
2017

42. Excitonic emission of hybrid lead iodide perovskite single crystals

Author

Hiba Diab, Gaëlle Trippé-Allard, Ferdinand Lédée, Khaoula Jemli, Guillaume Bouchez, Christèle Vilard, Jacques, Vincent L. R., Antonio Tejeda, Pierre Audebert, Jean‐sébastien Lauret, Damien Garrot, Emmanuelle Deleporte, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), and École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Abstract

International audience; Since 2012, hybrid organic perovskites (HOPs) represent a “material breakthrough” for photovoltaïcs and more broadly, HOPs have also high potentialities for light-emitting devices such as electroluminescent diodes and lasers. Improvement of the performance of perovskite solar cells and optoelectronic devices may benefit from a better understanding of the intrinsic photophysics of materials. However, the properties of films are very dependent of the grain structure. We will discuss here about the optical properties of HOPs single crystals and compare them to those of thin polycrystalline films. In particular, the main feature in CH3NH3PbI3 crystals is the appearance, in the low temperature luminescence spectra, of a sharp emission line (FWHM ~ 5 meV) at high energy which is attributed to the free exciton signature (figure 1). Experiments performed as a function of temperature confirm the existence of a strong electron-phonon coupling. A critical point for the design and fabrication of high-performance perovskite devices is related to the moisture sensitivity of HOPs. In particular, it is known that, under ambient conditions, CH3NH3PbI3 degrades producing some PbI2. Using the low temperature photoluminescence spectroscopy as a powerful tool to detect small PbI2 traces in hybrid perovskite thin layers and single crystals, we highlight the extremely high stability of the single crystals compared to the thin layers. Defects and grain boundaries are then thought to play an important role in the degradation mechanism.These results highlight the importance of single crystals as a reference material for the study of hybrid organic-inorganic perovskites.

Published
2017

43. First determination of the valence band dispersion of CH3NH3PbI3 hybrid organic-inorganic perovskite

Author

Min-I Lee, Barragán, A., Nair, M. N., Jacques, V., D. Le Bolloc'H, Fertey, P., Jemli, K., Lédée, F., Gaëlle Trippé-Allard, Emmanuelle Deleporte, Taleb-Ibrahimi, A., Tejeda, A., Laboratoire de Physique des Solides (LPS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), and Tejeda, Antonio

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; Organic-inorganic hybrid perovskites are promising absorber materials for low-cost photovoltaic solar cells or optoelectronic devices [1-5]. Among these perovskites, methylammonium triiodideplumbate (CH 3 NH 3 PbI 3 , MAPbI 3 or MAPI) exhibits currently the highest efficiency. Here we have analyzed the structural transition in MAPI by X-ray diffraction at the β phase and we have correlated it to its electronic properties. Despite all the extensive work on hybrid organic-inorganic halide perovskites, their experimental band structure measured with k-resolution has remained elusive. Such an experimental determination is a necessary requirement for an accurate theoretical description and understanding of the system. The impact of the structural phase transitions on the band structure in the operation temperature range of solar cells needed also to be elucidated. Herein, we present the experimental determination of the band structure of MAPI with k resolution by angle-resolved photoemission at 170 K [6]. Our results show that the spectral weight is strongly affected by the cubic symmetry although traces of the tetragonal band structure are appreciated. Some deviations with respect to theoretical calculations are observed, which may help to reach a more precise description of this paradigmatic system of the hybrid perovskite family. The project leading to this application has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 687008 (GOTSolar).

Published
2017

44. Effet de la transition de phase structurelle sur la structure de bande résolue en k de la pérovskite hybride organique-inorganique CH3NH3PbI3

Author

Min-I Lee, Barragan, A., Nair, M. N., Vincent Jacques, D. Le Bolloc'H, Fertey, P., Jemli, K., Ferdinand Lédée, Gaëlle Trippé-Allard, Emmanuelle Deleporte, Taleb-Ibrahimi, A., Tejeda, A., Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), DELEPORTE, Emmanuelle, Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), and École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)

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

National audience; Les pérovskites hybrides organiques-inorganiques d'halogénure de plomb sont devenues des matériaux prometteurs pour le photovoltaïque en raison de leur rendement élevé de conversion d’énergie solaire, ainsi que de leur fabrication à basse température et à bas coût en solution.Une des performances la plus remarquables (22%4) est celle des pérovskites d’halogénure de plomb méthylammonium (CH3NH3PbI3, MAPI). L’optimisation des performances au-delà nécessiterait d’une meilleure compréhension de la structure de bande électronique, qui est demeurée jusqu'à présent difficile à déterminer expérimentale. De plus, l'effet de la transition de phase structurelle sur la structure de bande dans la plage de température de fonctionnement des cellules solaires doit être éclairci. Ici, nous présentons la première détermination expérimentale de la structure de bande de MAPI avec résolution en k. Nos résultats montrent que la périodicité électronique dans la phase tétragonale de MAPI (inférieure à 50 ° C) correspond à celle de la phase cubique au haute température. Cela explique l'insensibilité des cellules solaires dans la gamme habituelle des températures de fonctionnement malgré la transition structurelle de tétragonale-cubique.

Published
2017

45. Electronic structure and dynamics of CH3NH3PbI3 hybrid organic-inorganic perovskite

Author

Min-I Lee, Zhesheng Chen, Ana Barragan, Zailan Zhang, Lédée, F., Maya Narayanan Nair, Jemli, K., Gaëlle Trippé-Allard, Hiba Diab, Pierre Fertey, Garrot, D., Papalazarou, E., Carlito Ponseca, Jacques, V., David Le Bolloc'H, Marsi, M., Emmanuelle Deleporte, Luca Perfetti, Taleb-Ibrahimi, A., Antonio Tejeda, Tejeda, Antonio, Laboratoire de Physique des Solides (LPS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Solides Irradiés (LSI), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Centre National de la Recherche Scientifique (CNRS), Laboratoire Aimé Cotton (LAC), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Lund University [Lund], Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de recherche pour le développement [IRD] : UR206-Muséum national d'Histoire naturelle (MNHN)-Centre National de la Recherche Scientifique (CNRS)

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; Organic-inorganic hybrid perovskites are promising absorber materials for low-cost photovoltaic solar cells or optoelectronic devices [1-4]. Among these perovskites, methylammonium triiodideplumbate (CH 3 NH 3 PbI 3 , MAPbI 3 or MAPI) exhibits currently the highest efficiency. Here we have analyzed the structural transition in MAPI by X-ray diffraction at the β phase and we have correlated it to its electronic properties. Despite all the extensive work on hybrid organic-inorganic halide perovskites, their experimental band structure measured with k-resolution has remained elusive. Such an experimental determination is a necessary requirement for an accurate theoretical description and understanding of the system. The impact of the structural phase transitions on the band structure in the operation temperature range of solar cells needed also to be elucidated. Herein, we present the experimental determination of the band structure of MAPI with k resolution by angle-resolved photoemission at 170 K [5]. Our results show that the spectral weight is strongly affected by the cubic symmetry although traces of the tetragonal band structure are appreciated. Some deviations with respect to theoretical calculations are observed, which may help to reach a more precise description of this paradigmatic system of the hybrid perovskite family. On a second step, we have studied the relaxation dynamics after photoexcitation, particularly important in a photovoltaic material. Time-resolved two-photon photoemission spectroscopy allows to directly visualize the electronic cooling at early delay times. It follows that photoexcited carriers thermalize on a subpicosecond timescale, presumably because of the coupling to the vibrations of organic cations [6]. The project leading to this application has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 687008 (GOTSolar). [1] S.D. Stranks and H.J. Snaith, Nature Nanotech 10, 391 (2015).[2] M. Grätzel, Nature Materials 13, 838 (2014).[3] Y. Wei et al., J. Phys. D: Appl. Phys. 46, 135105 (2013).[4] H. Diab, G. Trippé-Allard, F. Ledee, K. Jemli, C. Vilar, G. Bouchez, V. L. R. Jacques, A. Tejeda, J. Even, J.S. Lauret, E. Deleporte, and D. Garrot, J. Phys. Chem. Lett. 7, 5093 (2016). [5] M.-I. Lee, A. Barragán, M. N. Nair, V. L. R. Jacques, D. Le Bolloc’h, P. Fertey, K. Jemli, F. Ledee, G. Trippé-Allard, E. Deleporte, A. Taleb-Ibrahimi, and A. Tejeda, J. Phys. D: Appl. Phys. 50, 26LT02 (2017). [6] Z. Chen, M.-I. Lee, Z. Zhang, H. Diab, D. Garrot, F. Ledee, P. Fertey, E. Papalazarou, M. Marsi, C. Ponseca, E. Deleporte, A. Tejeda, and L. Perfetti, Phys. Rev. Mat. 1, 045402 (2017).

Published
2017

48. Using Low Temperature Photoluminescence Spectroscopy to Investigate CH3NH3PbI3 Hybrid Perovskite Degradation

Author

Bernard Geffroy, Gaëlle Trippé-Allard, Hiba Diab, Khaoula Jemli, Damien Garrot, Ferdinand Lédée, Pierre Audebert, Emmanuelle Deleporte, Jean-Sébastien Lauret, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Innovation en Chimie des Surfaces et NanoSciences (LICSEN UMR 3685), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), This work is supported by DIM Nano-K (grant PEROVOLT- IDF), and European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016)

Subjects
Fabrication, Materials science, optoelectronics, Exciton, hybrid perovskite, Pharmaceutical Science, Mineralogy, 02 engineering and technology, CH$_3$ NH$_3$ PbI$_3$, 010402 general chemistry, 01 natural sciences, Analytical Chemistry, lcsh:QD241-441, Quality (physics), lcsh:Organic chemistry, CH3NH3PbI3, solar cells, degradation, photoluminescence, Drug Discovery, Physical and Theoretical Chemistry, Spectroscopy, Perovskite (structure), hybrid perovskites, Thin layers, business.industry, Organic Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemistry (miscellaneous), [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Molecular Medicine, Optoelectronics, Degradation (geology), Grain boundary, 0210 nano-technology, business
Abstract

International audience; Investigating the stability and evaluating the quality of the CH$_3$NH$_3$PbI$_3$ perovskite structures is quite critical both to the design and fabrication of high-performance perovskite devices and to fundamental studies of the photophysics of the excitons. In particular, it is known that, under ambient conditions, CH$_3$NH$_3$PbI$_3$ degrades producing some PbI$_2$. We show here that low temperature Photoluminescence (PL) spectroscopy is a powerful tool to detect PbI$_2$ traces in hybrid perovskite layers and single crystals. Because PL spectroscopy is a signal detection method on a black background, small PbI$_2$ traces can be detected, when other methods currently used at room temperature fail. Our study highlights the extremely high stability of the single crystals compared to the thin layers and defects and grain boundaries are thought to play an important role in the degradation mechanism.

Published
2016

49. Optical properties of 3D hybrid organic perovskites monocrystals

Author

Hiba Diab, Gaëlle Trippé-Allard, Ferdinand Lédée, Khaoula Jemli, Guillaume Bouchez, Christèle Vilard, Vincent Jacques, Antonio Tejeda, Jean‐sébastien Lauret, Emmanuelle Deleporte, Damien Garrot, Laboratoire Aimé Cotton (LAC), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Laboratoire de Photophysique et Photochimie Supramoléculaires et Macromoléculaires (PPSM), École normale supérieure - Cachan (ENS Cachan)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), and DELEPORTE, Emmanuelle

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; Since 2012, the 3D hybrid organic perovskite CH3NH3PbI3 causes an incredible enthusiasm due to its application as absorbant material in solar cells, acheiving efficiency as large as 21%. It is now well established that this hybrid perovskite is a semiconductor whose band structure can be calculated using solid state physics methods such as DFT or tight-bending calculations. At this date, the origin of their remarkable performances is still quite unknown, so fundamental studies about the photophysics of these compounds are quite necessary. Until now, the fundamental studies are usually performed on spin-coated hybrid organic perovskite thin layers. These thin layers are highly polycristalline and the quality of the layers depend strongly on the synthesis conditions and on the substrates. As a consequence, the studies show a great variability of the electronic properties as a function of the morphology of the polycristalline thin layers, since the optical properties are dominated by the defects at low temperature. In particular, the size of the crystallites, varying between several 100 nanometers to several micrometers, has a great impact on the gap energy, the lifetimes and the excitonic properties. In this context, the recent possibility to synthesize 3D hybrid organic perovskite monocrystals having millimetric sizes allows to study the intrinsic properties of the material. We report here the emission and absorption properties of 3D hybrid organic perovskites at low temperature around the orthorhombic-tetragonal phase transition. We observe a hysteresis cycle related to the phase transition in these monocrystals and we show that the emission is dominated by the free excitons from time-resolved photoluminescence experiments. In particular, an important narrowing of the excitonic emission line as a function of temperature is observed in the orthorhombic phase, in contrast with previous studies.

Published
2016

50. Magic Angle Spinning 207 Pb and low temperature deuterium NMR as a tool for studying local order and dynamics in CH 3 NH 3 PbX 3 (X=Cl, Br, I) hybrid perovskites

Author

Claire Roiland, Gaëlle Trippé-Allard, Jemli, K., Alonso, C., Jean-Claude Ameline, Regis Gautier, Laurent Le Pollès, Emmanuelle Deleporte, Jacky Even, Claudine Katan, 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), Laboratoire Aimé Cotton (LAC), École normale supérieure - Cachan (ENS Cachan)-Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Fonctions Optiques pour les Technologies de l'informatiON (FOTON), Université de Rennes (UR)-Université européenne de Bretagne - European University of Brittany (UEB)-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)-Télécom Bretagne-Centre National de la Recherche Scientifique (CNRS), European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016), 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), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École normale supérieure - Cachan (ENS Cachan), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Université européenne de Bretagne - European University of Brittany (UEB)-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)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-Télécom Bretagne

Subjects
[CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS
Abstract

National audience

Published
2016

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