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1. Light-activated interlayer contraction in two-dimensional perovskites for high-efficiency solar cells

Author

Mercouri G. Kanatzidis, Boubacar Traore, Yafei Wang, Hao Zhang, Jean-Christophe Blancon, Joseph Strzalka, Justin M. Hoffman, Aditya D. Mohite, Wenbin Li, Joseph Essman, Claudine Katan, Ioannis Spanopoulos, Jared Crochet, Jacky Even, Austin Fehr, Jin Hou, Muhammad A. Alam, Siraj Sidhik, Reza Asadpour, Esther H. R. Tsai, Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), 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), Purdue University [West Lafayette], Northwestern University [Evanston], Los Alamos National Laboratory (LANL), Brookhaven National Laboratory [Upton, NY] (BNL), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY), Argonne National Laboratory [Lemont] (ANL), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE), NSF 20-587, National Science Foundation, N00014-20-1-2725, United States Department of Defense | United States Navy | ONR | Office of Naval Research Global, DE-SC0012704, U.S. Department of Energy, N00014-20-1-2725, United States Department of Defense | United States Navy | Office of Naval Research, and U.S. Department of Defense

Subjects
[PHYS]Physics [physics], Electron mobility, Materials science, Superlattice, Photovoltaic system, Biomedical Engineering, Bioengineering, 02 engineering and technology, Conductivity, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 7. Clean energy, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, X-ray photoelectron spectroscopy, Chemical physics, [CHIM]Chemical Sciences, General Materials Science, Electrical and Electronic Engineering, 0210 nano-technology, Dispersion (chemistry), Perovskite (structure), Voltage
Abstract

Understanding and tailoring the physical behaviour of halide perovskites under practical environments is critical for designing efficient and durable optoelectronic devices. Here, we report that continuous light illumination leads to >1% contraction in the out-of-plane direction in two-dimensional hybrid perovskites, which is reversible and strongly dependent on the specific superlattice packing. X-ray photoelectron spectroscopy measurements show that constant light illumination results in the accumulation of positive charges in the terminal iodine atoms, thereby enhancing the bonding character of inter-slab I–I interactions across the organic barrier and activating out-of-plane contraction. Correlated charge transport, structural and photovoltaic measurements confirm that the onset of the light-induced contraction is synchronized to a threefold increase in carrier mobility and conductivity, which is consistent with an increase in the electronic band dispersion predicted by first-principles calculations. Flux-dependent space-charge-limited current measurement reveals that light-induced interlayer contraction activates interlayer charge transport. The enhanced charge transport boosts the photovoltaic efficiency of two-dimensional perovskite solar cells up to 18.3% by increasing the device’s fill factor and open-circuit voltage. Light-induced contraction in the out-of-plane direction in two-dimensional (2D) hybrid perovskites enables the realization of high-efficiency 2D perovskite solar cells.

Published
2021
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2. Highly efficient photoelectric effect in halide perovskites for regenerative electron sources

Author

Jared Crochet, Vitaly Pavlenko, Mark A. Hoffbauer, Amanda Neukirch, Sina G. Lewis, Sergei Tretiak, Siraj Sidhik, Jacky Even, Aditya D. Mohite, Jean-Christophe Blancon, Fangze Liu, Nathan A. Moody, Wanyi Nie, Hsinhan Tsai, Mercouri G. Kanatzidis, Pulickel M. Ajayan, Los Alamos National Laboratory (LANL), Rice University [Houston], 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), Northwestern University [Evanston], Argonne National Laboratory [Lemont] (ANL), The work at Rice University was supported by ARO STIR project N-mensional interfaces, grant W911NF-19-1-0353. The work at Los Alamos National Laboratory (LANL) was supported by the LANL Laboratory Directed Research and Development Funds (LDRD) program. This work was done in part at the Center for Nonlinear Studies (CNLS) and the Center for Integrated Nanotechnologies (CINT), a U.S. Department of Energy and Office of Basic Energy Sciences user facility, at LANL. This research used resources provided by the LANL Institutional Computing Program. Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy (Contract No. 89233218NCA000001). J.E. acknowledges the financial support from the Institut Universitaire de France. Work at Northwestern was supported by the U.S. Department of Energy, Office of Science (Grant No. SC0012541, structure characterization)., 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 for devices, Photomultiplier, Materials science, Band gap, Science, General Physics and Astronomy, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Article, General Biochemistry, Genetics and Molecular Biology, Night vision, [CHIM]Chemical Sciences, Thin film, [PHYS]Physics [physics], Multidisciplinary, business.industry, Electronics, photonics and device physics, General Chemistry, Photoelectric effect, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Semiconductor, Semiconductors, Optoelectronics, Quantum efficiency, Vacuum level, 0210 nano-technology, business
Abstract

Electron sources are a critical component in a wide range of applications such as electron-beam accelerator facilities, photomultipliers, and image intensifiers for night vision. We report efficient, regenerative and low-cost electron sources based on solution-processed halide perovskites thin films when they are excited with light with energy equal to or above their bandgap. We measure a quantum efficiency up to 2.2% and a lifetime of more than 25 h. Importantly, even after degradation, the electron emission can be completely regenerated to its maximum efficiency by deposition of a monolayer of Cs. The electron emission from halide perovskites can be tuned over the visible and ultraviolet spectrum, and operates at vacuum levels with pressures at least two-orders higher than in state-of-the-art semiconductor electron sources., Electron sources play as important component in a wide range of applications. Here, the authors demonstrate efficient, regenerative, and low-cost electron sources based on solution-processed halide perovskite thin films with quantum efficiency up to 2.2% and a lifetime of more than 25 h.

Published
2021
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3. Cation Alloying Delocalizes Polarons in Lead-halide Perovskites

Author

Jared Crochet, Laurent Pedesseau, Liujiang Zhou, Sergei Tretiak, Amanda Neukirch, Claudine Katan, Wanyi Nie, Hsinhan Tsai, Jacky Even, Aditya D. Mohite, Los Alamos National Laboratory (LANL), University of Electronic Science and Technology of China [Chengdu] (UESTC), 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), Rice University [Houston], Agence Nationale de la Recherche, Laboratory Directed Research and Development, Institut Universitaire de France, ANR-15-CE05-0018,TRANSHYPERO,Vers une compréhension des propriétés de transport électronique des cellules solaires basées sur les pérovskites hybrides(2015), University of Electronic Science and Technology of China (UESTC), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), and Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)

Subjects
[PHYS]Physics [physics], Materials science, Band gap, Binding energy, 02 engineering and technology, Crystal structure, 010402 general chemistry, 021001 nanoscience & nanotechnology, Polaron, 01 natural sciences, 0104 chemical sciences, Delocalized electron, Formamidinium, Chemical physics, First principle, [CHIM]Chemical Sciences, General Materials Science, Physical and Theoretical Chemistry, 0210 nano-technology, Perovskite (structure)
Abstract

International audience; Recently, mixed-cation perovskites have promised enhanced performances concerning stability and efficiency in optoelectronic devices. Here, we report a systematic study on the effects of cation alloying on polaronic properties in cation-alloyed perovskites using first principle calculations. We find that cation alloying significantly reduces the polaron binding energies for both electrons and holes compared to pure methylammonium lead iodide (MAPbI3). This is rationalized in terms of crystal symmetry reduction that causes polarons to be more delocalized. Electron polarons undergo large Jahn-Teller distortions (~15−30%) while hole polarons tend to shrink lattice by ~5%. Such different lattice distortion footprints could be utilized to distinguish the type of polarons. Finally, our simulations show that a Cs, formamidinium (FA) and MA mixture can effectively minimize polaron binding energy while weakly affecting band gap, in a good agreement with experimental findings. These modeling results can guide future development of halide perovskite materials compositions for optoelectronic applications.

Published
2019
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4. Stable Light-Emitting Diodes Using Phase-Pure Ruddlesden-Popper Layered Perovskites

Author

Roberto Brenes, Richard H. Friend, Wanyi Nie, Vladimir Bulovic, Constantinos C. Stoumpos, Jared Crochet, Sergei Tretiak, Chan Myae Myae Soe, Samuel D. Stranks, Giovanni Azzellino, Jacky Even, Jean-Christophe Blancon, Aditya Sadhanala, Aditya D. Mohite, Mercouri G. Kanatzidis, Hsinhan Tsai, Pulickel M. Ajayan, Jinkyoung Yoo, Los Alamos National Laboratory (LANL), Rice University [Houston], Northwestern University [Evanston], 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)-Université Bretagne Loire (UBL)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Cavendish Laboratory, University of Cambridge [UK] (CAM), Massachusetts Institute of Technology (MIT), 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), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-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), N00014-17-1-2231, Office of Naval Research, DE-AC02-06CH11357, U.S. Department of Energy, and PIOF-GA-2013-622630, Seventh Framework Programme

Subjects
Fabrication, Materials science, LEDs, 02 engineering and technology, Electroluminescence, 010402 general chemistry, 01 natural sciences, law.invention, Crystal, crystal orientation, law, Phase (matter), color tunability, [CHIM]Chemical Sciences, General Materials Science, Voltage droop, [PHYS]Physics [physics], business.industry, Mechanical Engineering, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Semiconductor, Mechanics of Materials, Optoelectronics, 0210 nano-technology, business, Voltage, Ruddlesden-Popper layered perovskites, Light-emitting diode
Abstract

International audience; State-of-the-art light emitting diodes (LEDs) are made from high-purity alloys of III-V semiconductors or small molecules, but high fabrication cost and conplicated synthetic process have limited their widespread use for large area solid-state lighting applications. Here we report efficient and stable LEDs processed from solution with tunable color enabled by using phase-pure two-dimensional (2D) Ruddlesden-Popper (RP) layered perovskites with a formula (CH3(CH2)3NH3)2(CH3NH3)n-1PbnI3n+1 (n=3-5 in this report). By using controlled vertically oriented of crystal in the thin-films that facilitate efficient charge injection and transport, we obtain efficient electroluminescence with a radiance of 35 W Sr-1 cm-2 at 744 nm with an ultra-low turn-on voltage of 1V. Finally, operational stability tests suggest that phase purity is strongly correlated to stability. Phase-pure 2D perovskites exhibit >14 hours of stable operation at peak operating conditions with no droop at current-densities of several Amperes/cm2 in comparison to mixtures of 2D/3D mixture or 3D perovskites, which degrade within minutes.

Published
2018
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5. Geometry Distortion and Small Polaron Binding Energy Changes with Ionic Substitution in Halide Perovskites

Author

Claudine Katan, Jacky Even, Hsinhan Tsai, Iwnetim Abate, Sergei Tretiak, Jared Crochet, Wanyi Nie, Liujiang Zhou, Amanda Neukirch, Laurent Pedesseau, Aditya D. Mohite, Los Alamos National Laboratory (LANL), Stanford University, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Agence Nationale de la Recherche, Laboratory Directed Research and Development, Institut Universitaire de France, ANR-15-CE05-0018,TRANSHYPERO,Vers une compréhension des propriétés de transport électronique des cellules solaires basées sur les pérovskites hybrides(2015), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Materials science, Binding energy, Substitution (logic), Ionic bonding, Halide, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Polaron, 01 natural sciences, 0104 chemical sciences, Chemical physics, Distortion, [CHIM]Chemical Sciences, General Materials Science, Physical and Theoretical Chemistry, 0210 nano-technology
Abstract

International audience; Halide perovskites have demonstrated remarkable performance in optoelectronic applications. Despite extraordinary progress, questions remain about device stability. We report an in-depth computational study of small polaron formation, electronic structure, charge density, and reorganization energies of several experimentally relevant halide perovskites using isolated clusters. Local lattice symmetry, electronic structure, and electron-phonon coupling are interrelated in polaron formation in these materials. To illustrate this, first principles calculations are performed on (MA/Cs/FA)Pb(I/Br)3 and MASnI3. Across the materials studied, electron small polaron formation is manifested by Jahn-Teller like distortions in the central octahedron, with apical PbI bonds expanding significantly more than the equatorial bonds. In contrast, hole polarons cause the central octahedron to uniformly contract. This difference in manifestation of electron and hole polaron formation can be a tool to determine what is taking place in individual systems to systematically control performance. Other trends as the anion and cations are changed, are established for optimization in specific optoelectronic applications.

Published
2018
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6. Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites

Author

Costas C. Stoumpos, Pulickel M. Ajayan, Mikael Kepenekian, Claudine Katan, Hsinhan Tsai, Laurent Pedesseau, Sergei Tretiak, Chan Myae Myae Soe, Aditya D. Mohite, John Jared Crochet, Jacky Even, Jean-Christophe Blancon, Wanyi Nie, Mercouri G. Kanatzidis, Matthew Y. Sfeir, Kannatassen Appavoo, Los Alamos National Laboratory (LANL), Northwestern University [Evanston], Rice University [Houston], 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), Institut des Sciences Chimiques de Rennes (ISCR), 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)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Brookhaven National Laboratory [Upton, NY] (BNL), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY), The work in France was supported by Cellule Energie du CNRS (SOLHYBTRANS Project) and University of Rennes 1 (Action Incitative, Défis Scientifique Emergents 2015)., CINT/LANL contract DE-AC52-06NA25396, SOLHYBTRANS, 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), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), and State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE)

Subjects
[PHYS]Physics [physics], Multidisciplinary, Condensed matter physics, Chemistry, Band gap, Exciton, 02 engineering and technology, Electronic structure, Electron, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Condensed Matter::Materials Science, [SPI]Engineering Sciences [physics], [PHYS.QPHY]Physics [physics]/Quantum Physics [quant-ph], Coulomb, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Thin film, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], 0210 nano-technology, Quantum well, Perovskite (structure)
Abstract

How perovskites have the edge Two-dimensional Ruddlesden-Popper perovskites form quantum wells by sandwiching inorganic-organic perovskite layers used in photovoltaic devices between organic layers. Blancon et al. show that if the perovskite layer is more than two unit cells thick, photogenerated excitons undergo an unusual but highly efficient process for creating free carriers that can be harvested in photovoltaic devices (see the Perspective by Bakr and Mohammed). Lower-energy local states at the edges of the perovskite layer facilitate dissociation into electrons and holes that are well protected from recombination. Science , this issue p. 1288 ; see also p. 1260

Published
2017
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7. Polaron stabilization by cooperative lattice distortion and cation rotations in hybrid perovskite materials

Author

Hsinhan Tsai, Amanda Neukirch, Laurent Pedesseau, Sergei Tretiak, Wanyi Nie, Jacky Even, Matthew Y. Sfeir, Gautam Gupta, Jean-Christophe Blancon, Aditya D. Mohite, Kannatassen Appavoo, Jared Crochet, Claudine Katan, Los Alamos National Laboratory (LANL), Brookhaven National Laboratory [Upton, NY] (BNL), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), 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), The work in France was supported by Cellule Energie du CNRS (SOLHYBTRANS Project) and University of Rennes 1 (Action Incitative, Défis Scientifique Emergents 2015). J.E. work was supported by the Fondation d’entreprises banque Populaire de l’Ouest under Grant PEROPHOT 2015.The work at Los Alamos National Laboratory (LANL) was supported by the LANL LDRD program (A.J.N., A.D.M, G.G., and S.T.). This work was done in part at Center for Nonlinear Studies (CNLS) and the Center for Integrated Nano- technologies CINT), a U.S. Department of Energy and Office of Basic Energy Sciences user facility, at LANL. This research used resources provided by the LANL Institutional Computing Program. LANL is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract DE-AC52- 06NA25396.This research used resources of the Center for Functional Nanomaterials, which is a US DOE Office of Science Facility, at Brookhaven National Laboratory under Contract No. DE- SC0012704., 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), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de 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), and even, jacky

Subjects
Materials science, [SPI] Engineering Sciences [physics], Inorganic chemistry, Ionic bonding, Bioengineering, 02 engineering and technology, Electronic structure, 010402 general chemistry, Polaron, 7. Clean energy, 01 natural sciences, [PHYS] Physics [physics], photovoltaic, [SPI]Engineering Sciences [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, General Materials Science, ComputingMilieux_MISCELLANEOUS, Perovskite (structure), Photocurrent, [PHYS]Physics [physics], polaron, Mechanical Engineering, Charge density, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, cation rotations, Chemical physics, Organic−inorganic perovskite, Density functional theory, Charge carrier, 0210 nano-technology
Abstract

International audience; Solution-processed organometallic perovskites have rapidly developed into a top candidate for the active layer of photovoltaic devices. Despite the remarkable progress associated with perovskite materials, many questions about the fundamental photophysical processes taking place in these devices remain open. High on the list of unexplained phenomena are very modest mobilities despite low charge carrier effective masses. Moreover, experiments elucidate unique degradation of photocurrent affecting stable operation of perovskite solar cells. These puzzles suggest that while ionic hybrid perovskite devices may have efficiencies on par with conventional Si and GaAs devices, they exhibit more complicated charge transport phenomena. Here we report the results from an in-depth computational study of small polaron formation, electronic structure, charge density, and reorganization energies using both periodic boundary conditions and isolated structures. Using the hybrid Density Functional Theory, we found that volumetric strain in a CsPbI3 cluster creates a polaron with binding energy of around 300 meV and 900 meV for holes and electrons, respectively. In the MAPbI3 (MA=CH3NH3) cluster, both volumetric strain and MA reorientation effects lead to larger binding energies at around 600 meV and 1300 meV for holes and electrons, respectively. Such large reorganization energies suggest appearance of small polarons in organometallic perovskite materials. The fact that both volumetric lattice strain and MA molecular rotational degrees of freedom can cooperate to create and stabilize polarons, indicates that in order to mitigate this problem, formamidinium (FA=HC(NH2)2) and cesium (Cs) based crystals and alloys, are potentially better materials for solar cell and other optoelectronic applications.

Published
2016
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8. The effects of electronic impurities and electron-hole recombination dynamics on large-grain organic-inorganic perovskite photovoltaic efficiencies

Author

Jean-Christophe Blancon, Gautam Gupta, Jared Crochet, Aditya D. Mohite, Laurent Cognet, Amanda Neukirch, Wanyie Nie, Sergei Tretiak, Los Alamos National Laboratory (LANL), Laboratoire Photonique, Numérique et Nanosciences (LP2N), Université de Bordeaux (UB)-Institut d'Optique Graduate School (IOGS)-Centre National de la Recherche Scientifique (CNRS), LP2N_A1, and LP2N_G1

Subjects
Materials science, Photoluminescence, business.industry, [PHYS.PHYS.PHYS-BIO-PH]Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Biomaterials, Semiconductor, Impurity, Chemical physics, Electrochemistry, Charge carrier, Thin film, 0210 nano-technology, Spectroscopy, business, Excitation, Perovskite (structure)
Abstract

International audience; Organometallic perovskites have attracted considerable attention after promising developments in energy harvesting and other optoelectronic applications. However, further optimization will require a deeper understanding of the intrinsic photo-physics of materials with relevant structural characteristics. Here we investigate the dynamics of photogenerated charge carriers in large-area grain organometallic perovskite thin films via confocal time-resolved photoluminescence spectroscopy. It is found that the bimolecular recombination of free charges is the dominant decay mechanism at excitation densities relevant for photovoltaic applications. Bimolecular coefficients are found to be on the order of 10-9 cm3/s, comparable to typical direct-gap semiconductors, yet significantly smaller than theoretically expected. We also demonstrate that there is no degradation in carrier transport in these thin films due to electronic impurities. Suppressed electron-hole recombination and transport that is not limited by deep level defects provide a microscopic model for the superior performance of large-area grain hybrid perovskites for photovoltaic applications.

Published
2016
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