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2. Inorganic Tin Perovskites with Tunable Conductivity Enabled by Organic Modifiers

Author

Haque, Md Azimul, Zhu, Tong, Hernandez, Luis Huerta, Tounesi, Roba, Combe, Craig, Davaasuren, Bambar, Emwas, Abdul-Hamid, de Arquer, F. Pelayo García, Sargent, Edward H., and Baran, Derya

Subjects
Physics - Applied Physics
Abstract

Achieving control over the transport properties of charge-carriers is a crucial aspect of realizing high-performance electronic materials. In metal-halide perovskites, which offer convenient manufacturing traits and tunability for certain optoelectronic applications, this is challenging: The perovskite structure itself, poses fundamental limits to maximum dopant incorporation. Here, we demonstrate an organic modifier incorporation strategy capable of modulating the electronic density of states in halide tin perovskites without altering the perovskite lattice, in a similar fashion to substitutional doping in traditional semiconductors. By incorporating organic small molecules and conjugated polymers into cesium tin iodide (CsSnI3) perovskites, we achieve carrier density tunability over 2.7 decades, transition from a semiconducting to a metallic nature, and high electrical conductivity exceeding 200 S/cm. We leverage these tunable and enhanced electronic properties to achieve a thin-film, lead free, thermoelectric material with a near room-temperature figure-of-merit (ZT) of 0.21, the highest amongst all halide perovskite thermoelectrics. Our strategy provides an additional degree of freedom in the design of halide perovskites for optoelectronic and energy applications.

Published
2023

3. Closed-loop Error Correction Learning Accelerates Experimental Discovery of Thermoelectric Materials

Author

Choubisa, Hitarth, Haque, Md Azimul, Zhu, Tong, Zeng, Lewei, Vafaie, Maral, Baran, Derya, and Sargent, Edward H

Subjects
Condensed Matter - Materials Science, Computer Science - Machine Learning
Abstract

The exploration of thermoelectric materials is challenging considering the large materials space, combined with added exponential degrees of freedom coming from doping and the diversity of synthetic pathways. Here we seek to incorporate historical data and update and refine it using experimental feedback by employing error-correction learning (ECL). We thus learn from prior datasets and then adapt the model to differences in synthesis and characterization that are otherwise difficult to parameterize. We then apply this strategy to discovering thermoelectric materials where we prioritize synthesis at temperatures < 300{\deg}C. We document a previously unreported chemical family of thermoelectric materials, PbSe:SnSb, finding that the best candidate in this chemical family, 2 wt% SnSb doped PbSe, exhibits a power factor more than 2x that of PbSe. Our investigations show that our closed-loop experimentation strategy reduces the required number of experiments to find an optimized material by as much as 3x compared to high-throughput searches powered by state-of-the-art machine learning models. We also observe that this improvement is dependent on the accuracy of prior in a manner that exhibits diminishing returns, and after a certain accuracy is reached, it is factors associated with experimental pathways that dictate the trends.

Published
2023
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5. Impact of the valence band energy alignment at the hole-collecting interface on the photostability of wide band-gap perovskite solar cells

Author

Torres Merino, Luis Victor, Petoukhoff, Christopher E., Matiash, Oleksandr, Subbiah, Anand Selvin, Franco, Carolina Villamil, Dally, Pia, Vishal, Badri, Kosar, Sofiia, Rosas Villalva, Diego, Hnapovskyi, Vladyslav, Ugur, Esma, Shah, Sahil, Peña Camargo, Francisco, Karalis, Orestis, Hempel, Hannes, Levine, Igal, Pradhan, Rakesh R., Kralj, Suzana, Kalasariya, Nikhil, Babics, Maxime, Yildirim, Bumin Kagan, Said, Ahmed A., Aydin, Erkan, Bristow, Helen, Mannar, Subhashri, Raja, Waseem, Pininti, Anil Reddy, Prasetio, Adi, Razzaq, Arsalan, Al Nasser, Hamza, Allen, Thomas G., Isikgor, Furkan H., Baran, Derya, Anthopoulos, Thomas D., Masis, Monica Morales, Schwingenschlögl, Udo, Unold, Thomas, Stolterfoht, Martin, Laquai, Frédéric, and De Wolf, Stefaan

Published
2024
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7. Rationalizing the influence of tunable energy levels on quantum efficiency to design optimal non-fullerene acceptor-based ternary organic solar cells

Author

Karuthedath, Safakath, Paleti, Sri H. K ., Sharma, Anirudh, Yin, Hang, De Castro, Catherine S. P., Chen, Si, Xi, Han, Alshehri, Nisreen, Ramos, Nicolas, Khan, Jafar I., Martin, Jaime, Li, Gang, Laquai, Frédéric, Baran, Derya, and Gorenflot, Julien

Subjects
Physics - Applied Physics, Condensed Matter - Materials Science
Abstract

Non-fullerene acceptor (NFA)-based ternary bulk heterojunction solar cells (TSC) are the most efficient organic solar cells (OSCs) today due to their broader absorption and quantum efficiencies (QE) often surpassing those of corresponding binary blends. We study how the energetics driving charge transfer at the electron donor:electron acceptor (D/A) interfaces impact the QE in blends of PBDB-T-2F donor with several pairs of lower bandgap NFAs. As in binary blends, the ionization energy offset between donor and acceptor ({\Delta}IE) controls the QE and maximizes for {\Delta}IE > 0.5 eV. However, {\Delta}IE is not controlled by the individual NFAs IEs but by their average, weighted for their blending ratio. Using this property, we improved the QE of a PBDB-T-2F:IEICO binary blend that had an insufficient {\Delta}IE for charge generation by adding a deep IE third component: IT-4F. Combining two NFAs enables to optimize the D/A energy alignment and cells' QE without molecular engineering., Comment: S Karuthedath and S H K Paleti contributed equally. MS: 35 pages, 9 figures. SI: 21 pages, 23 figures - updates: added a model scheme as Fig1, updated T1 EQE and blends PL in Fig 2 (former 1). Added Figure (5): charge generation upon acceptor excitation. Corrected {\Delta}IEs in fig7 and 9 (a few tens of meV off). Added more blends to show generality (2 groups, 10 blends compositions)

Published
2021
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11. Dissecting the structure-stability relationship of Y-series electron acceptors for real-world solar cell applications

Author

Xu, Han, Han, Jianhua, Chen, Si, Liu, Ye, Huerta Hernandez, Luis, Bertrandie, Jules, Babics, Maxime, Alam, Shahidul, Villalva, Diego Rosas, Paleti, Sri Harish Kumar, Gorenflot, Julien, Herok, Christoph, Ramos, Nicolas, Troughton, Joel, Sharma, Anirudh, Marder, Todd B., Engels, Bernd, Martin, Jaime, De Wolf, Stefaan, Laquai, Frédéric, and Baran, Derya

Published
2023
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17. Concurrent cationic and anionic perovskite defect passivation enables 27.4% perovskite/silicon tandems with suppression of halide segregation

Author

Isikgor, Furkan H., Furlan, Francesco, Liu, Jiang, Ugur, Esma, Eswaran, Mathan K., Subbiah, Anand S., Yengel, Emre, De Bastiani, Michele, Harrison, George T., Zhumagali, Shynggys, Howells, Calvyn T., Aydin, Erkan, Wang, Mingcong, Gasparini, Nicola, Allen, Thomas G., Rehman, Atteq ur, Van Kerschaver, Emmanuel, Baran, Derya, McCulloch, Iain, Anthopoulos, Thomas D., Schwingenschlögl, Udo, Laquai, Frédéric, and De Wolf, Stefaan

Published
2021
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18. Nanoscale Morphology of Doctor Bladed versus Spin‐Coated Organic Photovoltaic Films

Author

Pokuri, Balaji Sesha Sarath, Sit, Joseph, Wodo, Olga, Baran, Derya, Ameri, Tayebeh, Brabec, Christoph J, Moule, Adam J, and Ganapathysubramanian, Baskar

Subjects
Bioengineering, blade spin as-cast anneal, internal morphology analysis, organic photovoltaic cells, reconstruction, tortuosity connectivity fraction, Macromolecular and Materials Chemistry, Materials Engineering, Interdisciplinary Engineering
Abstract

Recent advances in efficiency of organic photovoltaics are driven by judicious selection of processing conditions that result in a “desired” morphology. An important theme of morphology research is quantifying the effect of processing conditions on morphology and relating it to device efficiency. State-of-the-art morphology quantification methods provide film-averaged or 2D-projected features that only indirectly correlate with performance, making causal reasoning nontrivial. Accessing the 3D distribution of material, however, provides a means of directly mapping processing to performance. In this paper, two recently developed techniques are integrated—reconstruction of 3D morphology and subsequent conversion into intuitive morphology descriptors —to comprehensively image and quantify morphology. These techniques are applied on films generated by doctor blading and spin coating, additionally investigating the effect of thermal annealing. It is found that morphology of all samples exhibits very high connectivity to electrodes. Not surprisingly, thermal annealing consistently increases the average domain size in the samples, aiding exciton generation. Furthermore, annealing also improves the balance of interfaces, enhancing exciton dissociation. A comparison of morphology descriptors impacting each stage of photophysics (exciton generation, dissociation, and charge transport) reveals that spin-annealed sample exhibits superior morphology-based performance indicators. This suggests substantial room for improvement of blade-based methods (process optimization) for morphology tuning to enhance performance of large area devices.

Published
2017

19. In situformation of thermoset matrices for improved stability in organic photovoltaics

Author

Han, Jianhua, Xu, Han, Sharma, Anirudh, Babics, Maxime, Bertrandie, Jules, Wang, Xunchang, Huerta Hernandez, Luis, Zhang, Yongcao, Wen, Yuanfan, Rosas Villalva, Diego, Ramos, Nicolas, Paleti, Sri Harish K., Martin, Jaime, Xu, Fuzong, Troughton, Joel, Yang, Renqiang, Gorenflot, Julien, Laquai, Frédéric, De Wolf, Stefaan, and Baran, Derya

Abstract

The performance of organic photovoltaics (OPVs) has rapidly increased. Yet, achieving long-term stability in the nano-morphology and thereby sustaining device performance remains challenging. Herein, we show that incorporating in-situ-forming cross-linked thermoset (CLT) matrices into the bulk heterojunction blends is a simple, general, and efficient strategy for high-performing and resilient OPVs. Our simulations and experimental data prove that these high-modulus CLT matrices featuring hydrogen-bonding interactions can freeze the nano-morphology, resulting in long-term thermal and photostable OPV devices. We demonstrate that this approach works efficiently with eight different blends and show that OPV devices can withstand 85°C for 1,000 h without losing performance. Blends with CLT matrices double the energy generated from OPV devices, showing an energy density output of 4,054 mW⋅h cm−2over an 11-week operating period under outdoor conditions. This methodology opens avenues for both developing new thermoset networks for OPV and their use in other optoelectronic applications.

Published
2024
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20. Intrinsic efficiency limits in low-bandgap non-fullerene acceptor organic solar cells

Author

Karuthedath, Safakath, Gorenflot, Julien, Firdaus, Yuliar, Chaturvedi, Neha, De Castro, Catherine S. P., Harrison, George T., Khan, Jafar I., Markina, Anastasia, Balawi, Ahmed H., Peña, Top Archie Dela, Liu, Wenlan, Liang, Ru-Ze, Sharma, Anirudh, Paleti, Sri H. K., Zhang, Weimin, Lin, Yuanbao, Alarousu, Erkki, Lopatin, Sergei, Anjum, Dalaver H., Beaujuge, Pierre M., De Wolf, Stefaan, McCulloch, Iain, Anthopoulos, Thomas D., Baran, Derya, Andrienko, Denis, and Laquai, Frédéric

Published
2021
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23. Understanding photochemical degradation mechanisms in photoactive layer materials for organic solar cells.

Author

Han, Jianhua, Xu, Han, Paleti, Sri Harish Kumar, Sharma, Anirudh, and Baran, Derya

Subjects
SOLAR cells, CHEMICAL stability, ELECTRON donors, LIGHT absorption, ELECTROPHILES, PHOTODEGRADATION
Abstract

Over the past decades, the field of organic solar cells (OSCs) has witnessed a significant evolution in materials chemistry, which has resulted in a remarkable enhancement of device performance, achieving efficiencies of over 19%. The photoactive layer materials in OSCs play a crucial role in light absorption, charge generation, transport and stability. To facilitate the scale-up of OSCs, it is imperative to address the photostability of these electron acceptor and donor materials, as their photochemical degradation process remains a challenge during the photo-to-electric conversion. In this review, we present an overview of the development of electron acceptor and donor materials, emphasizing the crucial aspects of their chemical stability behavior that are linked to the photostability of OSCs. Throughout each section, we highlight the photochemical degradation pathways for electron acceptor and donor materials, and their link to device degradation. We also discuss the existing interdisciplinary challenges and obstacles that impede the development of photostable materials. Finally, we offer insights into strategies aimed at enhancing photochemical stability and discuss future directions for developing photostable photo-active layers, facilitating the commercialization of OSCs. [ABSTRACT FROM AUTHOR]

Published
2024
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26. Nanoscale Morphology of PTB7 Based Organic Photovoltaics as a Function of Fullerene Size.

Author

Roehling, John D, Baran, Derya, Sit, Joseph, Kassar, Thaer, Ameri, Tayebeh, Unruh, Tobias, Brabec, Christoph J, and Moulé, Adam J

Subjects
Bioengineering, Biochemistry and Cell Biology, Other Physical Sciences
Abstract

High efficiency polymer:fullerene photovoltaic device layers self-assemble with hierarchical features from ångströms to 100's of nanometers. The feature size, shape, composition, orientation, and order all contribute to device efficiency and are simultaneously difficult to study due to poor contrast between carbon based materials. This study seeks to increase device efficiency and simplify morphology measurements by replacing the typical fullerene acceptor with endohedral fullerene Lu3N@PC80BEH. The metal atoms give excellent scattering contrast for electron beam and x-ray experiments. Additionally, Lu3N@PC80BEH has a lower electron affinity than standard fullerenes, which can raise the open circuit voltage of photovoltaic devices. Electron microscopy techniques are used to produce a detailed account of morphology evolution in mixtures of Lu3N@PC80BEH with the record breaking donor polymer, PTB7 and coated using solvent mixtures. We demonstrate that common solvent additives like 1,8-diiodooctane or chloronapthalene do not improve the morphology of endohedral fullerene devices as expected. The poor device performance is attributed to the lack of mutual miscibility between this particular polymer:fullerene combination and to co-crystallization of Lu3N@PC80BEH with 1,8-diiodooctane. This negative result explains why solvent additives mixtures are not necessarily a morphology cure-all.

Published
2016

30. Managing grains and interfaces via ligand anchoring enables 22.3%-efficiency inverted perovskite solar cells

Author

Zheng, Xiaopeng, Hou, Yi, Bao, Chunxiong, Yin, Jun, Yuan, Fanglong, Huang, Ziru, Song, Kepeng, Liu, Jiakai, Troughton, Joel, Gasparini, Nicola, Zhou, Chun, Lin, Yuanbao, Xue, Ding-Jiang, Chen, Bin, Johnston, Andrew K., Wei, Nini, Hedhili, Mohamed Nejib, Wei, Mingyang, Alsalloum, Abdullah Y., Maity, Partha, Turedi, Bekir, Yang, Chen, Baran, Derya, Anthopoulos, Thomas D., Han, Yu, Lu, Zheng-Hong, Mohammed, Omar F., Gao, Feng, Sargent, Edward H., and Bakr, Osman M.

Published
2020
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36. Photo‐Chemical Stimulation of Neurons with Organic Semiconductors (Adv. Sci. 31/2023)

Author

Savva, Achilleas, primary, Hama, Adel, additional, Herrera‐López, Gabriel, additional, Schmidt, Tony, additional, Migliaccio, Ludovico, additional, Steiner, Nadia, additional, Kawan, Malak, additional, Fiumelli, Hubert, additional, Magistretti, Pierre J., additional, McCulloch, Iain, additional, Baran, Derya, additional, Gasparini, Nicola, additional, Schindl, Rainer, additional, Głowacki, Eric D., additional, and Inal, Sahika, additional

Published
2023
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37. Author Correction: Intrinsic efficiency limits in low-bandgap non-fullerene acceptor organic solar cells

Author

Karuthedath, Safakath, Gorenflot, Julien, Firdaus, Yuliar, Chaturvedi, Neha, De Castro, Catherine S. P., Harrison, George T., Khan, Jafar I., Markina, Anastasia, Balawi, Ahmed H., Peña, Top Archie Dela, Liu, Wenlan, Liang, Ru-Ze, Sharma, Anirudh, Paleti, Sri H. K., Zhang, Weimin, Lin, Yuanbao, Alarousu, Erkki, Lopatin, Sergei, Anjum, Dalaver H., Beaujuge, Pierre M., De Wolf, Stefaan, McCulloch, Iain, Anthopoulos, Thomas D., Baran, Derya, Andrienko, Denis, and Laquai, Frédéric

Published
2022
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44. Hexanary Blends: A Strategy Towards Thermally Stable Organic Photovoltaics

Author

Paleti, Sri Harish Kumar, primary, Baran, Derya, additional, Han, Jianhua, additional, Xu, Han, additional, Wen, Yuanfan, additional, Chen, Si, additional, jarsvall, emmy, additional, Jalan, ishita, additional, Villalva, Diego Rosas, additional, Hultmark, Sandra, additional, Khan, Jafar.I., additional, Moons, Ellen, additional, Li, Ruipeng, additional, Yu, Liyang, additional, Gorenflot, Julien, additional, Laquai, Frederic, additional, Muller, Christian, additional, and Sharma, Anirudh, additional

Published
2023
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46. N-type organic thermoelectrics: demonstration of ZT > 0.3

Author

Liu, Jian, van der Zee, Bas, Alessandri, Riccardo, Sami, Selim, Dong, Jingjin, Nugraha, Mohamad I., Barker, Alex J., Rousseva, Sylvia, Qiu, Li, Qiu, Xinkai, Klasen, Nathalie, Chiechi, Ryan C., Baran, Derya, Caironi, Mario, Anthopoulos, Thomas D., Portale, Giuseppe, Havenith, Remco W. A., Marrink, Siewert J., Hummelen, Jan C., and Koster, L. Jan Anton

Published
2020
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49. Rationalizing the Influence of Tunable Energy Levels on Quantum Efficiency to Design Optimal Non‐Fullerene Acceptor‐Based Ternary Organic Solar Cells

Author

Karuthedath, Safakath, primary, Paleti, Sri H. K., additional, Sharma, Anirudh, additional, Yin, Hang, additional, P. De Castro, Catherine S., additional, Chen, Si, additional, Xu, Han, additional, Alshehri, Nisreen, additional, Ramos, Nicolas, additional, Khan, Jafar I., additional, Martin, Jaime, additional, Li, Gang, additional, Laquai, Frédéric, additional, Baran, Derya, additional, and Gorenflot, Julien, additional

Published
2023
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50. Device Performance of Emerging Photovoltaic Materials (Version 3)

Author

Almora, Osbel, Baran, Derya, Bazan, Guillermo C., Cabrera, Carlos I., Erten-Ela, Sule, Forberich, Karen, Guo, Fei, Hauch, Jens, Ho-Baillie, Anita W.Y., Jacobsson, T. Jesper, Janssen, Rene A.J., Kirchartz, Thomas, Kopidakis, Nikos, Loi, Maria A., Lunt, Richard R., Mathew, Xavier, McGehee, Michael D., Min, Jie, Mitzi, David B., Nazeeruddin, Mohammad K., Nelson, Jenny, Nogueira, Ana F., Paetzold, Ulrich W., Rand, Barry P., Rau, Uwe, Snaith, Henry J., Unger, Eva, Vaillant-Roca, Lídice, Yang, Chenchen, Yip, Hin Lap, Brabec, Christoph J., Almora, Osbel, Baran, Derya, Bazan, Guillermo C., Cabrera, Carlos I., Erten-Ela, Sule, Forberich, Karen, Guo, Fei, Hauch, Jens, Ho-Baillie, Anita W.Y., Jacobsson, T. Jesper, Janssen, Rene A.J., Kirchartz, Thomas, Kopidakis, Nikos, Loi, Maria A., Lunt, Richard R., Mathew, Xavier, McGehee, Michael D., Min, Jie, Mitzi, David B., Nazeeruddin, Mohammad K., Nelson, Jenny, Nogueira, Ana F., Paetzold, Ulrich W., Rand, Barry P., Rau, Uwe, Snaith, Henry J., Unger, Eva, Vaillant-Roca, Lídice, Yang, Chenchen, Yip, Hin Lap, and Brabec, Christoph J.

Abstract

Following the 2nd release of the “Emerging PV reports,” the best achievements in the performance of emerging photovoltaic devices in diverse emerging photovoltaic research subjects are summarized, as reported in peer-reviewed articles in academic journals since August 2021. Updated graphs, tables, and analyses are provided with several performance parameters, e.g., power conversion efficiency, open-circuit voltage, short-circuit current density, fill factor, light utilization efficiency, and stability test energy yield. These parameters are presented as a function of the photovoltaic bandgap energy and the average visible transmittance for each technology and application, and are put into perspective using, e.g., the detailed balance efficiency limit. The 3rd installment of the “Emerging PV reports” extends the scope toward triple junction solar cells.

Published
2023

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