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1. Rapid spin depolarization in the layered 2D Ruddlesden Popper perovskite (BA)(MA)PbI

Author

Kempf, Michael, Moser, Philipp, Tomoscheit, Maximilian, Schröer, Julian, Blancon, Jean-Christophe, Schwartz, Rico, Deb, Swarup, Mohite, Aditya, Stier, Andreas V., Finley, Jonathan J., and Korn, Tobias

Subjects
Condensed Matter - Mesoscale and Nanoscale Physics, Condensed Matter - Materials Science
Abstract

We report temperature-dependent spectroscopy on the layered (n=4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneaously recorded time-resolved differential reflectivity (TR$\Delta$R) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin dephasing time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, the spin dephasing is nearly T-independent. Our results highlight that spin dephasing in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aimingto utilize this degree of freedom.

Published
2023
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2. Deterministic synthesis of phase pure 2D perovskites via progressive transformation of layer thickness

Author

Hou, Jin, Li, Wenbin, Zhang, Hao, Sidhik, Siraj, Blancon, Jean-Christophe, Even, Jacky, Kanatzidis, Mercouri G., and Mohite, Aditya D.

Subjects
Condensed Matter - Materials Science
Abstract

Two-dimensional (2D) halide perovskites have emerged as semiconductor platforms for realizing efficient and durable optoelectronic devices. However, the reproducible synthesis of 2D perovskite crystals with desired layer thickness (or n value) greater than 2, has been an enduring challenge due to the lack of kinetic control (temperature, time, stoichiometry) for each layer thickness. Here, we demonstrate a novel method term as the kinetically controlled space confinement (KCSC) for the deterministic growth of phase pure Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) 2D perovskites. The phase-pure growth was achieved by progressively increasing the temperature (fixed time) or the crystallization time (fixed temperature), which allowed for an acute control of the crystallization kinetics. We also observe a systematic transformation from a lower n-value to n=3, 4, 5, 6 in 2D perovskites. In-situ photoluminescence spectroscopy and imaging suggest that the progressive transformation from lower to higher n-value occurs via intercalation of excess precursor ions. These experiments enabled the development of a machine learning assisted multi-parameter phase diagram, which predicts the growth of 2D phase with a specific n-value., Comment: 32 pages, 15 figures

Published
2022

4. Integrated halide perovskite photoelectrochemical cells with solar-driven water-splitting efficiency of 20.8%

Author

Fehr, Austin MK, Agrawal, Ayush, Mandani, Faiz, Conrad, Christian L, Jiang, Qi, Park, So Yeon, Alley, Olivia, Li, Bor, Sidhik, Siraj, Metcalf, Isaac, Botello, Christopher, Young, James L, Even, Jacky, Blancon, Jean Christophe, Deutsch, Todd G, Zhu, Kai, Albrecht, Steve, Toma, Francesca M, Wong, Michael, and Mohite, Aditya D

Subjects
Affordable and Clean Energy
Abstract

Achieving high solar-to-hydrogen (STH) efficiency concomitant with long-term durability using low-cost, scalable photo-absorbers is a long-standing challenge. Here we report the design and fabrication of a conductive adhesive-barrier (CAB) that translates >99% of photoelectric power to chemical reactions. The CAB enables halide perovskite-based photoelectrochemical cells with two different architectures that exhibit record STH efficiencies. The first, a co-planar photocathode-photoanode architecture, achieved an STH efficiency of 13.4% and 16.3 h to t60, solely limited by the hygroscopic hole transport layer in the n-i-p device. The second was formed using a monolithic stacked silicon-perovskite tandem, with a peak STH efficiency of 20.8% and 102 h of continuous operation before t60 under AM 1.5G illumination. These advances will lead to efficient, durable, and low-cost solar-driven water-splitting technology with multifunctional barriers.

Published
2023

5. Direct visualization of ultrafast lattice ordering triggered by an electron-hole plasma in 2D perovskites

Author

Zhang, Hao, Li, Wenbin, Essman, Joseph, Quarti, Claudio, Metcalf, Isaac, Chiang, Wei-Yi, Sidhik, Siraj, Hou, Jin, Fehr, Austin, Attar, Andrew, Lin, Ming-Fu, Britz, Alexander, Shen, Xiaozhe, Link, Stephan, Wang, Xijie, Bergmann, Uwe, Kanatzidis, Mercouri G., Katan, Claudine, Even, Jacky, Blancon, Jean-Christophe, and Mohite, Aditya D.

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

Direct visualization of ultrafast coupling between charge carriers and lattice degrees of freedom in photo-excited semiconductors has remained a long-standing challenge and is critical for understanding the light-induced physical behavior of materials under extreme non-equilibrium conditions. Here, by monitoring the evolution of the wave-vector resolved ultrafast electron diffraction intensity following above-bandgap photo-excitation, we obtain a direct visual of the structural dynamics in monocrystalline 2D perovskites. Analysis reveals a surprising, light-induced ultrafast lattice ordering resulting from a strong interaction between hot-carriers and the perovskite lattice, which induces an in-plane octahedra rotation, towards a more symmetric phase. Correlated ultrafast spectroscopy performed at the same carrier density as ultrafast electron diffraction reveals that the creation of a hot and dense electron-hole plasma triggers lattice ordering at short timescales by modulating the crystal cohesive energy. Finally, we show that the interaction between the carrier gas and the lattice can be altered by tailoring the rigidity of the 2D perovskite by choosing the appropriate organic spacer layer., Comment: 25 pages, 4 figures

Published
2022

6. Self-Hybridized Polaritonic Emission from Layered Perovskites

Author

Anantharaman, Surendra B., Stevens, Christopher E., Lynch, Jason, Song, Baokun, Hou, Jin, Zhang, Huiqin, Jo, Kiyoung, Kumar, Pawan, Blancon, Jean-Christophe, Mohite, Aditya D., Hendrickson, Joshua R., and Jariwala, Deep

Subjects
Physics - Optics, Condensed Matter - Mesoscale and Nanoscale Physics, Condensed Matter - Materials Science, Condensed Matter - Other Condensed Matter, Physics - Applied Physics
Abstract

Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (> 100 nm) crystals and near-unity absorption in thin (< 20 nm) crystals. We observe resonances with quality factors > 250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D-HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry.

Published
2021
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7. Ultrafast relaxation of lattice distortion in two-dimensional perovskites

Author

Zhang, Hao, Li, Wenbin, Essman, Joseph, Quarti, Claudio, Metcalf, Isaac, Chiang, Wei-Yi, Sidhik, Siraj, Hou, Jin, Fehr, Austin, Attar, Andrew, Lin, Ming-Fu, Britz, Alexander, Shen, Xiaozhe, Link, Stephan, Wang, Xijie, Bergmann, Uwe, Kanatzidis, Mercouri G., Katan, Claudine, Even, Jacky, Blancon, Jean-Christophe, and Mohite, Aditya D.

Published
2023
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8. Determination of Dielectric Functions and Exciton Oscillator Strength of Two-Dimensional Hybrid Perovskites

Author

Song, Baokun, Hou, Jin, Wang, Haonan, Sidhik, Siraj, Miao, Jinshui, Gu, Honggang, Zhang, Huiqin, Liu, Shiyuan, Fakhraai, Zahra, Even, Jacky, Blancon, Jean-Christophe, Mohite, Aditya D., and Jariwala, Deep

Subjects
Physics - Applied Physics, Physics - Optics
Abstract

Two-dimensional (2D) hybrid organic inorganic perovskite (HOIP) semiconductors have attracted widespread attention as a platform of next generation optoelectronic devices benefiting from their naturally occurring and tunable multiple quantum-well like (QW) structures, which enable a wide range of physical properties. Determining the intrinsic optical/electronic properties of 2D HOIPs is extremely important for further utility in photonic and optoelectronics devices. Here, we obtain the optical dielectric functions, complex refractive indices, and complex optical conductivities of both Ruddlesden-Popper (RP) and Dion-Jacobsen (DJ) phases of 2D HOIPs as a function of the perovskite QW thickness via spectroscopic ellipsometry over a broad energy range of 0.73 - 3.34 eV. We identify a series of feature peaks in the dielectric functions, and explain the evolution of ground state exciton peak with unit cell thickness and changing excitonic confinement. We observe extraordinary values of optical extinction and electric loss tangents at the primary excitonic resonances and provide their detailed comparison with other known excitonic materials. Our study is expected to lay foundation for understanding optical properties of pure phase 2D HOIPs, which will be helpful for the accurate modelling of their photonics and optoelectronic devices.

Published
2020

9. Structural and thermodynamic limits of layer thickness in 2D halide perovskites

Author

Soe, Chan Myae Myae, Nagabhushana, GP, Shivaramaiah, Radha, Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Melkonyan, Ferdinand, Cao, Duyen H, Traoré, Boubacar, Pedesseau, Laurent, Kepenekian, Mikaël, Katan, Claudine, Even, Jacky, Marks, Tobin J, Navrotsky, Alexandra, Mohite, Aditya D, Stoumpos, Constantinos C, and Kanatzidis, Mercouri G

Subjects
Macromolecular and Materials Chemistry, Chemical Sciences, Physical Chemistry, Affordable and Clean Energy, layered compounds, homologous series, Ruddlesden-Popper halide perovskites, formation enthalpy, photovoltaics, Ruddlesden–Popper halide perovskites
Abstract

In the fast-evolving field of halide perovskite semiconductors, the 2D perovskites (A')2(A) n-1M n X3n+1 [where A = Cs+, CH3NH3+, HC(NH2)2+; A' = ammonium cation acting as spacer; M = Ge2+, Sn2+, Pb2+; and X = Cl-, Br-, I-] have recently made a critical entry. The n value defines the thickness of the 2D layers, which controls the optical and electronic properties. The 2D perovskites have demonstrated preliminary optoelectronic device lifetime superior to their 3D counterparts. They have also attracted fundamental interest as solution-processed quantum wells with structural and physical properties tunable via chemical composition, notably by the n value defining the perovskite layer thickness. The higher members (n > 5) have not been documented, and there are important scientific questions underlying fundamental limits for n To develop and utilize these materials in technology, it is imperative to understand their thermodynamic stability, fundamental synthetic limitations, and the derived structure-function relationships. We report the effective synthesis of the highest iodide n-members yet, namely (CH3(CH2)2NH3)2(CH3NH3)5Pb6I19 (n = 6) and (CH3(CH2)2NH3)2(CH3NH3)6Pb7I22 (n = 7), and confirm the crystal structure with single-crystal X-ray diffraction, and provide indirect evidence for "(CH3(CH2)2NH3)2(CH3NH3)8Pb9I28" ("n = 9"). Direct HCl solution calorimetric measurements show the compounds with n > 7 have unfavorable enthalpies of formation (ΔHf), suggesting the formation of higher homologs to be challenging. Finally, we report preliminary n-dependent solar cell efficiency in the range of 9-12.6% in these higher n-members, highlighting the strong promise of these materials for high-performance devices.

Published
2019

12. Spatially Resolved Photo-Excited Charge Carrier Dynamics in Phase-Engineered Monolayer MoS2

Author

Yamaguchi, Hisato, Blancon, Jean-Christophe, Kappera, Rajesh, Lei, Sidong, Najmaei, Sina, Mangum, Benjamin D., Gupta, Gautam, Ajayan, Pulickel M., Lou, Jun, Chhowalla, Manish, Crochet, Jared J., and Mohite, Aditya D.

Subjects
Condensed Matter - Materials Science
Abstract

A fundamental understanding of the intrinsic optoelectronic properties of atomically thin transition metal dichalcogenides (TMDs) is crucial for its integration into high performance semiconductor devices. Here, we investigate the transport properties of chemical vapor deposition (CVD) grown monolayer molybdenum disulfide (MoS2) under photo-excitation using correlated scanning photocurrent microscopy and photoluminescence imaging. We examined the effect of local phase transformation underneath the metal electrodes on the generation of photocurrent across the channel length with diffraction-limited spatial resolution. While maximum photocurrent generation occurs at the Schottky contacts of semiconducting (2H-phase) MoS2, after the metallic phase transformation (1T-phase), the photocurrent peak is observed towards the center of the device channel, suggesting a strong reduction of native Schottky barriers. Analysis using the bias and position dependence of the photocurrent indicates that the Schottky barrier heights are few meV for 1T- and ~200 meV for 2H-contacted devices. We also demonstrate that a reduction of native Schottky barriers in a 1T device enhances the photo responsivity by more than one order of magnitude, a crucial parameter in achieving high performance optoelectronic devices. The obtained results pave a pathway for the fundamental understanding of intrinsic optoelectronic properties of atomically thin TMDs where Ohmic contacts are necessary for achieving high efficiency devices with low power consumption., Comment: 20 pages, 6 figures, 8 pages of supporting information, accepted to ACS Nano

Published
2014

17. Integrated halide perovskite photoelectrochemical cells with solar-driven water-splitting efficiency of 20.8%

Author

Fehr, Austin, Agrawal, Ayush, Mandani, Faiz, Conrad, Christian, Jiang, Qi, Park, So Yeon, Alley, Olivia, Li, Bor, Sidhik, Siraj, Metcalf, Isaac, Botello, Christopher, Young, James, Even, Jacky, Blancon, Jean Christophe, Deutsch, Todd, Zhu, Kai, Albrecht, Steve, Toma, Francesca, Mohite, Aditya, Rice University [Houston], National Renewable Energy Laboratory (NREL), Lawrence Berkeley National Laboratory [Berkeley] (LBNL), Helmholtz-Zentrum Berlin, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), 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
Abstract

Achieving high solar-to-hydrogen (STH) efficiency concomitant with long-term durability using low-cost, scalable photo-absorbers is a long-standing challenge. Here we report the design and fabrication of a conductive adhesive-barrier (CAB) that translates >99% of photoelectric power to chemical reactions. The CAB enables halide perovskite-based photoelectrochemical cells with two different architectures that exhibit record STH efficiencies. The first, a co-planar photocathode-photoanode architecture, achieved an STH efficiency of 13.4% and 16.3 h to t 60 , solely limited by the hygroscopic hole transport layer in the n-i-p device. The second was formed using a monolithic stacked silicon-perovskite tandem, with a peak STH efficiency of 20.8% and 102 h of continuous operation before t 60 under AM 1.5G illumination. These advances will lead to efficient, durable, and low-cost solar-driven water-splitting technology with multifunctional barriers.

Published
2023
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21. Optically active cross-band transition in double-walled carbon nanotube and its impact on Raman resonances

Author

Agence Nationale de la Recherche (France), Universidad de Zaragoza, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Diputación General de Aragón, European Commission, Gobierno de Aragón, Bulgarian National Science Fund, Paillet, Matthieu, Popov, Valentin N., Tran, Huy Nam, Blancon, Jean Christophe, Levshov, Dmitry I., Arenal, Raúl, Parret, Romain, Ayari, Anthony, San Miguel, Alfonso, Vallèe, Fabrice G., Fatti, Natalia del, Zahab, Ahmed Azmi, Sauvajol, Jean Louis, Agence Nationale de la Recherche (France), Universidad de Zaragoza, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Diputación General de Aragón, European Commission, Gobierno de Aragón, Bulgarian National Science Fund, Paillet, Matthieu, Popov, Valentin N., Tran, Huy Nam, Blancon, Jean Christophe, Levshov, Dmitry I., Arenal, Raúl, Parret, Romain, Ayari, Anthony, San Miguel, Alfonso, Vallèe, Fabrice G., Fatti, Natalia del, Zahab, Ahmed Azmi, and Sauvajol, Jean Louis

Abstract

Double-walled carbon nanotubes (DWNTs), often regarded as the simplest one-dimensional (1D) van der Waals moiré superlattices, are the ideal structures to explore the interlayer coupling, including mechanical and electronical coupling, at the nanoscale in 1D systems. By combining spatial modulation spectroscopy (SMS) and resonant Raman scattering (RRS) experiments on well-identified individual free-standing DWNTs with the calculations of their optical absorption by using the recursion method with non-orthogonal tight-binding (NTB) basis functions, we are able to unambiguously assign the nature, namely mirror transition or cross transition, of each optical transitions in DWNTs. Our study identifies and allows to determine the conditions of the mixing of the electronic states leading to the appearance of cross transitions in the optical absorption of DWNTs, beyond of the so-called Koshino's criteria previously derived. On the other hand, the striking behavior of the resonant excitation profile (REP) of the Raman active modes around the cross transition reveals the strong sensitivity of the modes intensity on the electronic interlayer coupling in DWNTs, emphasizing the relevance of Raman spectroscopy for studying the electronic and mechanical coupling at the nanoscale.

Published
2022

22. Influence of Chemical Engineering, Photodoping and Lattice Distortions on the Optoelectronic Properties of Multilayered Perovskites

Author

even, jacky, primary, katan, claudine, additional, li, wenbin, additional, zhang, hao, additional, traoré, boubacar, additional, quarti, claudio, additional, sidhik, siraj, additional, mercier, nicolas, additional, li, wei, additional, kanatzidis, mercouri, additional, blancon, jean-christophe, additional, mohite, aditya, additional, and Skorokhod, alia, additional

Published
2022
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24. Physics of 2D perovskites

Author

Even, Jacky, Blancon, Jean Christophe, Sidhik, Siraj, li, weibin, Zhang, Hao, Li, Wei, Traore, Boubacar, Pedesseau, Laurent, Volonakis, George, Kepenekian, Mikael, Stoumpos, Constantinos, Kanatzidis, Mercouri, Mohite, Aditya, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Nankai University (NKU), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), University of Crete [Heraklion] (UOC), Northwestern University [Evanston], European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics]
Abstract

International audience; In the past years, solution-processed organometallic perovskite based solar cells have emerged as a promising low-cost thin-film photovoltaic technology. 3D halide perovskite semiconductors and their 2D or OD nanostructures present specific symmetry and electronic properties, including giant spin-orbit coupling (SOC) effects. The ultrahigh softness of the halide perovskite lattice is also characteristic, and the role of the electron-phonon coupling, especially at temperatures relevant for device operation, is not fully understood. The presentation will focus on 2D perovskites, composed of perovskites layers sandwiched between two layers of large organic cations, described in the 90’s as self-assembled quantum and dielectric well systems.

Published
2021

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

Author

Even, Jacky, Sidhik, Siraj, li, weibin, Zhang, Hao, Traoré, Boubacar, Bourges, Philippe, Kanatzidis, Mercouri, Blancon, Jean Christophe, Mohite, Aditya, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Northwestern University [Evanston], Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), J. Even acknowledges the financial support from the Institut Universitaire de France., European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, even, jacky, Polariton logic - PoLLoC - 899141 - INCOMING, High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING, and DRop-on demand flexible Optoelectronics & Photovoltaics by means of Lead-Free halide perovskITes - DROPIT - 862656 - INCOMING

Subjects
[PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract

National audience; The presentation will describe a few recent results on the structural and optoelectronic properties in 2D and 3D halide perovskites, focusing on some possibilities offered by nowadays neutron, X-rays and electron large scale scattering facilities.

Published
2021

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

Author

Traoré, Boubacar, Li, Wenbin, Sidhik, Siraj, Asadpour, Reza, Hou, Jin, Zhang, Hao, Fehr, Austin, Essman, Joseph, Wang, Yafei, Hoffman, Justin, Spanopoulos, Ioannis, Crochet, Jared, Tsai, Esther, Strzalka, Joseph, Alam, Muhammad, Kanatzidis, Mercouri, Katan, Claudine, Blancon, Jean Christophe, Mohite, Aditya, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Rice University [Houston], Purdue University [West Lafayette], Northwestern University [Evanston], Los Alamos National Laboratory (LANL), Brookhaven National Laboratory [Upton, NY] (BNL), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE), Argonne National Laboratory [Lemont] (ANL), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J. Even acknowledges the financial support from the Institut Universitaire de France. DFT calculations were performed at Institut FOTON as well as Institut des Sciences Chimiques de Rennes, and the work was granted access to the HPC resources of Très Grand Centre de Calcul du CEA (TGCC), the Centre Informatique National de I’Enseignement Supérieur (CINES) and Institut du développement et des ressources en informatique scientifique (IDRIS) under allocations 2019-A0060906724 and 2019-A0070907682 made by Grand Équipement National de Calcul Intensif (GENCI)., CNRS Israeli French scientific cooperation (Joint Research Projects 2019-2021 ALLPOA)., European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), even, jacky, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING

Subjects
[PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract

National audience; Despite their improved stability and versatility, 2D layered perovskites’ solar cell efficiencies lag behind those of their 3D counterparts, which currently exceed 25%. Through a proper selection of the organic spacer, 2D perovskites can be synthetized in different configurations adopting various phases such as the Ruddlesden-Popper (RP), the Alternating Cation Interlayer (ACI) or the Dion-Jacobson ones. Tailoring the organic spacer type has been shown to enhance the electronic coupling along the layered perovskite stacking axis and thereby enhance carrier transport resulting in improved efficiencies.

Published
2021

27. Interstitial Nature of Mn2+ Doping in 2D Perovskites

Author

Torma, Andrew J., primary, Li, Wenbin, additional, Zhang, Hao, additional, Tu, Qing, additional, Klepov, Vladislav V., additional, Brennan, Michael C., additional, McCleese, Christopher L., additional, Krzyaniak, Matthew D., additional, Wasielewski, Michael R., additional, Katan, Claudine, additional, Even, Jacky, additional, Holt, Martin V., additional, Grusenmeyer, Tod A., additional, Jiang, Jie, additional, Pachter, Ruth, additional, Kanatzidis, Mercouri G., additional, Blancon, Jean-Christophe, additional, and Mohite, Aditya D., additional

Published
2021
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28. Light-activated interlayer contraction in two-dimensional perovskites for high-efficiency solar cells

Author

Li, Wenbin, primary, Sidhik, Siraj, additional, Traore, Boubacar, additional, Asadpour, Reza, additional, Hou, Jin, additional, Zhang, Hao, additional, Fehr, Austin, additional, Essman, Joseph, additional, Wang, Yafei, additional, Hoffman, Justin M., additional, Spanopoulos, Ioannis, additional, Crochet, Jared J., additional, Tsai, Esther, additional, Strzalka, Joseph, additional, Katan, Claudine, additional, Alam, Muhammad A., additional, Kanatzidis, Mercouri G., additional, Even, Jacky, additional, Blancon, Jean-Christophe, additional, and Mohite, Aditya D., additional

Published
2021
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30. Anisotropic Lattice Deformations Control Photocarrier Relaxation Dynamics in 2D Halide Perovskites

Author

Zhang, Hao, Li, Wenbin, Essman, Joseph, Quarti, Claudio, Sidhik, Siraj, Hou, Jin, Metcalf, Isaac, Crochet, Jared, Kanatzidis, Mercouri, Katan, Claudine, Even, Jacky, Blancon, Jean Christophe, Mohite, Aditya, 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), Los Alamos National Laboratory (LANL), 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)-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)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2021

31. Light-Activated Contraction in Organic-Inorganic 2D Perovskites Enables High-Efficiency Photovoltaics

Author

Li, Wenbin, Sidhik, Siraj, Traoré, Boubacar, Asadpour, Reza, Zhang, Hao, Hou, Jin, Strzalka, Joseph, Tsai, Esther, Hoffman, Justin, Spanopoulos, Ioannis, Alam, Muhammad, Katan, Claudine, Kanatzidis, Mercouri, Even, Jacky, Blancon, Jean Christophe, Mohite, Aditya, 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), Argonne National Laboratory [Lemont] (ANL), 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), Northwestern University [Evanston], Purdue University [West Lafayette], 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), 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), 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), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2021

32. Band engineering of nickel oxide interfaces and connection between absolute valence energy alignment and surface dipoles in halide perovskite heterostructures

Author

Traore, Boubacar, primary, Even, Jacky, additional, Pedesseau, Laurent, additional, Ramadan, Alexandra, additional, Blancon, Jean-Christophe, additional, Basera, Pooja, additional, Mohite, Aditya, additional, Snaith, Henry, additional, Kepenekian, Mikael, additional, Katan, Claudine, additional, and Tretiak, Sergei, additional

Published
2021
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34. Self-Hybridized Polaritonic Emission from Layered Perovskites

Author

Anantharaman, Surendra B., primary, Stevens, Christopher E., additional, Lynch, Jason, additional, Song, Baokun, additional, Hou, Jin, additional, Zhang, Huiqin, additional, Jo, Kiyoung, additional, Kumar, Pawan, additional, Blancon, Jean-Christophe, additional, Mohite, Aditya D., additional, Hendrickson, Joshua R., additional, and Jariwala, Deep, additional

Published
2021
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35. Cesium-Coated Halide Perovskites as a Photocathode Material: Modeling Insights

Author

Lewis, Sina G., primary, Ghosh, Dibyajyoti, additional, Jensen, Kevin L., additional, Finkenstadt, Daniel, additional, Shabaev, Andrew, additional, Lambrakos, Samuel G., additional, Liu, Fangze, additional, Nie, Wanyi, additional, Blancon, Jean-Christophe, additional, Zhou, Liujiang, additional, Crochet, Jared J., additional, Moody, Nathan, additional, Mohite, Aditya D., additional, Tretiak, Sergei, additional, and Neukirch, Amanda J., additional

Published
2021
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36. Memory Seeds Enable High Structural Phase Purity in 2D Perovskite Films for High‐Efficiency Devices

Author

Sidhik, Siraj, primary, Li, Wenbin, additional, Samani, Mohammad H. K., additional, Zhang, Hao, additional, Wang, Yafei, additional, Hoffman, Justin, additional, Fehr, Austin K., additional, Wong, Michael S., additional, Katan, Claudine, additional, Even, Jacky, additional, Marciel, Amanda B., additional, Kanatzidis, Mercouri G., additional, Blancon, Jean‐Christophe, additional, and Mohite, Aditya D., additional

Published
2021
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37. Effect of light-induced lattice expansion in high-efficiency halide perovskites solar cells

Author

Durand, Olivier, Tsai, Hsinhan, Asadpour, Reza, Blancon, Jean-Christophe, Stoumpos, Constantinos, Strzalka, Joseph, Verduzco, Rafael, Chen, Bo, Ajayan, Pulickel, Tretiak, Sergei, Even, Jacky, Alam, Muhammad, Kanatzidis, Mercouri, Nie, Wanyie, Mohite, Aditya, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Los Alamos National Laboratory (LANL), Department of Materials Science and NanoEngineering, Rice university, Purdue University [West Lafayette], Northwestern University [Evanston], X-ray Science Division (XSD), Rice University [Houston], 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
[SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2020

38. Determination of Dielectric Functions and Exciton Oscillator Strength of Two-Dimensional Hybrid Perovskites

Author

Song, Baokun, primary, Hou, Jin, additional, Wang, Haonan, additional, Sidhik, Siraj, additional, Miao, Jinshui, additional, Gu, Honggang, additional, Zhang, Huiqin, additional, Liu, Shiyuan, additional, Fakhraai, Zahra, additional, Even, Jacky, additional, Blancon, Jean-Christophe, additional, Mohite, Aditya D., additional, and Jariwala, Deep, additional

Published
2020
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42. High-efficiency two-dimensional RuddlesdenPopper perovskite solar cells

Author

Tsai, Hsinhan, Nie, Wanyi, Blancon, Jean-Christophe, Stoumpos, Constantinos C., Asadpour, Reza, Harutyunyan, Boris, Neukirch, Amanda J., Verduzco, Rafael, Crochet, Jared J., Tretiak, Sergei, Pedesseau, Laurent, Even, Jacky, Alam, Muhammad A., Gupta, Gautam, Lou, Jun, Ajayan, Pulickel M., Bedzyk, Michael J., Kanatzidis, Mercouri G., and Mohite, Aditya D.

Subjects
Crystal structure -- Analysis, Solar cells -- Research -- Properties -- Analysis, Perovskite -- Usage -- Properties, Environmental issues, Science and technology, Zoology and wildlife conservation
Abstract

Author(s): Hsinhan Tsai [1, 2]; Wanyi Nie [1]; Jean-Christophe Blancon [1]; Constantinos C. Stoumpos [3, 4, 5]; Reza Asadpour [6]; Boris Harutyunyan [4, 5]; Amanda J. Neukirch [1]; Rafael Verduzco [...]

Published
2016
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43. Tailoring Structural Disorder and Crystal Orientation in 2D Perovskite Thin Films for High-Efficiency Optoelectronics

Author

Sidhik, Siraj, Li, Wenbin, Fehr, Austin, Wang, Yafei, Kanatzidis, Mercouri, Even, Jacky, Blancon, Jean-Christophe, Mohite, Aditya, 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)-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), 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

44. Theoretical insight on quantum and dielectric confinement in metal-halide perovskites

Author

Katan, Claudine, Traore, Boubacar, Kepenekian, Mikael, Pedesseau, Laurent, Even, Jacky, Leveillee, Joshua, Schleife, André, Neukirch, Amanda, Tretiak, Sergei, Blancon, Jean-Christophe, Mohite, Aditya, Stoumpos, Constantinos, Kanatzidis, Mercouri, Smith, Matthew, Karunadasa, Hemamala, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Illinois at Urbana-Champaign [Urbana], University of Illinois System, Los Alamos National Laboratory (LANL), Rice University [Houston], University of Crete [Heraklion] (UOC), Northwestern University [Evanston], Department of Chemistry [Stanford], Stanford University, C-Nano PACA, ANR-15-CE05-0018,TRANSHYPERO,Vers une compréhension des propriétés de transport électronique des cellules solaires basées sur les pérovskites hybrides(2015), 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
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat]
Abstract

International audience; Both all inorganic and hybrid halide perovskites recently demonstrated undeniably remarkable characteristics for a wide range of optoelectronic applications. The perovskite fever began with 3D halide perovskites of chemical formula AMX3 with A a small organic or an inorganic cation, M a metal (Pb2+, Sn2+, Ge2+), and X a halogen (I-, Br-, Cl-), which opened a route toward low-cost manufacture of solar cells, offering currently certified conversion efficiencies over 25%.[1] Since the initial breakthrough mid-2012,[2] halide perovskites attracted worldwide efforts from the scientific community[3] leading to an extensive exploration of their structural versatility and an ever-growing diversity of structures.[3] Prior to the perovskite fever, especially in the 90's, most experimental efforts on halide perovskites focused on chemistry and optical characterizations of monolayered halide perovskites of chemical formula A'MX4, with A' a larger organic cation.[4]Currently, many different perovskite as well as non-perovskite metal-halide networks are synthesized and their optoelectronic properties deserve to be unraveled (Figure). Among others, new compositions such as A'2An-1MnX3n+1 afford layered structures with a controlled number (n) of octahedra in the perovskite layer and thus offer an ideal platform for fundamental understanding.3,5 Here, through a couple of recent examples,[5,6] we will discuss their optoelectronic properties based on theoretical modeling. Impact of composition and structural pattern on properties will be inspected, with particular emphasis on the effect of quantum and dielectric confinements on charge carriers and excitons. [1] https://www.nrel.gov/pv/cell-efficiency.html. [2] M. M. Lee & al. JACS 134, 17396 (2012); H.-S Kim & al. Sci. Rep. 2, 591(2012). [2] Special issue, Chem. Rev. 119, 3033 (2019). [3] C. Katan & al. Chem. Rev. 119, 3140 (2019). [4] G. C. Papavassiliou Prog. Solid State Chem. 25, 125 (1997); D. B. Mitzi Prog. Inorg. Chem. John Wiley & Sons (1999). [5] L. Mao & al. Chem, in press (2019). [6] M. Smith & al. Chem. Sci. 8, 1960 (2017); J.-C. Blancon & al. Science 355, 1288 (2017); B. Traore & al. ACS Nano 12, 3321 (2018); J.-C. Blancon & al. Nat. Com. 9, 2254 (2018); M. Kepenekian & al. Nano Lett. 18, 5603 (2018); J. Leveillee & al. PRMater. 2, 105406 (2018) and submitted. X. Li & al. Chem. Mater. 31, 3582 and JACS 141, 12880 (2019).

Published
2019

45. Giant Enhancement of Photoluminescence Emission in WS_2-2D Perovskite Heterostructures

Author

Yang, Arky, Blancon, Jean-Christophe, Jiang, Wei, Zhang, Hao, Wong, Joeson, Yan, Ellen, Lin, Yi-Rung, Crochet, Jared, Kanatzidis, Mercouri G., Jariwala, Deep, Low, Tony, Mohite, Aditya D., and Atwater, Harry A.

Abstract

Transition metal dichalcogenides (TMDCs) and two-dimensional organic and inorganic hybrid lead halide perovskites (2DPVSKs) have emerged as highly promising materials for ultralight and ultrathin optoelectronics application. They both exhibit tunability of electronic properties such as band structure, and they can form heterostructures with various types of two-dimensional materials for novel physical properties not observed in single components. However, TMDCs exhibit poor emission efficiency due to defect states and direct-to-indirect interband transition, and 2DPVSKs suffer from poor stability in ambient atmosphere. Here we report that fabrication of TMDC-on-2DPVSK heterostructures using a solvent-free process leads to novel optical transitions unique to the heterostructure which arise from the hybrid interface and exhibit a strong photoluminescence. Moreover, a two orders of magnitude enhancement of the photoluminescence as compared to WS_2 emission is observed. The TMDC on top of 2DPVSK also significantly improves the stability as compared to bare 2DPVSK. Enhanced emission can be explained by electronic structure modification of TMDC by novel interfacial interactions between TMDC and 2DPVSK materials, which shows promise of the heterostructure for high efficiency and stable optoelectronic devices.

Published
2019

46. Metal Halide Perovskites: A New Class of Semiconductors

Author

Katan, Claudine, TRAORE, Boubacar, Kepenekian, Mikael, Pedesseau, Laurent, Leveillee, Joshua, Schleife, André, Neukirch, Amanda, Tretiak, Sergei, Blancon, Jean-Christophe, Mohite, Aditya, Stoumpos, Constantinos, Kanatzidis, Mercouri, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Illinois at Urbana-Champaign [Urbana], University of Illinois System, Los Alamos National Laboratory (LANL), Rice University [Houston], University of Crete [Heraklion] (UOC), Northwestern University [Evanston], ANR-15-CE05-0018,TRANSHYPERO,Vers une compréhension des propriétés de transport électronique des cellules solaires basées sur les pérovskites hybrides(2015), 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
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat]
Abstract

International audience; Metal halide perovskites have recently demonstrated undeniably remarkable characteristics for a wide range of optoelectronic applications. The perovskite fever began with 3D hybrid perovskites of chemical formula AMX 3 , made of corner-sharing MX 6 with M a metal, X a halogen, and A a small organic cation. These perovskites have opened a route toward low-cost manufacture of solar cells while offering currently certified conversion efficiencies over 24%, at the level of the best known thin film technologies and not far from monocrystalline silicon. Since the initial breakthrough mid-2012, halide perovskites have attracted worldwide efforts from the scientific community leading to an extensive exploration of their structural versatility and an ever-growing diversity of composition with a revival of all inorganic metal halide perovskites. Currently, many different metal-halide networks are synthetized and their optoelectronic properties deserve to be unraveled. Among others, new compositions such as A' 2 A n-1 M n X 3n+1 afford layered structures with a controlled number of octahedra in the perovskite layer interspaced with larger organic cations A' for most. Here, through a couple of recent examples including newly discovered halide perovskite phases as well as experimental data from the early 90's, we will discuss their optoelectronic properties based on first-principles calculations, semi-empirical and empirical modelling. Differences between this class of perovskite materials and conventional semiconductors will be highlighted. Impact of composition and structural pattern on properties will be inspected, with particular emphasis on the effect of quantum and dielectric confinements on charge carriers and excitons. Opportunities to further engineer halide perovskite properties will also be tackled in the prospect to provide guidance for the design of new synthetic targets.

Published
2019

47. Quantum and dielectric confinements in halide perovskites: from a theoretical perspective

Author

Katan, Claudine, Traore, Boubacar, Leveillee, Joshua, Kepenekian, Mikael, Blancon, Jean-Christophe, Mohite, Aditya, Tretiak, Sergei, Stoumpos, Constantinos, Kanatzidis, Mercouri, 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), University of Illinois at Urbana-Champaign [Urbana], University of Illinois System, Los Alamos National Laboratory (LANL), Rice University [Houston], Northwestern University [Evanston], University of Crete [Heraklion] (UOC), 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)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)

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

International audience

Published
2019

48. Versatility of metal halide perovskites: insight from atomic scale modelling

Author

Katan, Claudine, Traore, Boubacar, Kepenekian, Mikael, Blancon, Jean-Christophe, Mohite, Aditya, Tretiak, Sergei, Stoumpos, Constantinos, Kanatzidis, Mercouri, Even, Jacky, 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), Rice University [Houston], Los Alamos National Laboratory (LANL), Northwestern University [Evanston], University of Crete [Heraklion] (UOC), ANR-15-CE05-0018,TRANSHYPERO,Vers une compréhension des propriétés de transport électronique des cellules solaires basées sur les pérovskites hybrides(2015), European Project: 687008,H2020,H2020-FETOPEN-2014-2015-RIA,GOTSolar(2016), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat]
Abstract

International audience; Both all inorganic and hybrid halide perovskites have recently demonstrated undeniably remarkable characteristics for a wide range of optoelectronic applications. The perovskite fever began with 3D halide perovskites of chemical formula AMX3 with A a small organic (e.g. methylammonium, formamidinium) or an inorganic cation (e.g. Cs+), M a metal (Pb2+, Sn2+, Ge2+), and X a halogen (I-, Br-, Cl-), which have opened a route toward low-cost manufacture of solar cells while offering currently certified conversion efficiencies over 24%, at the level of the best known thin film technologies and not far from monocrystalline silicon (25%). Since the initial breakthrough mid-2012, halide perovskites have attracted worldwide efforts from the scientific community leading to an extensive exploration of their structural versatility and an ever-growing diversity of structures. Prior to the perovskite fever, especially in the 80's and 90's, most experimental efforts on halide perovskites were focused on chemistry and optical characterizations of monolayered halide perovskites of chemical formula A'MX4, with A' a larger organic cation (e.g. alkylammonium). Currently, many different perovskite -with corner-sharing octahedra- as well as non-perovskite metal-halide networks are synthetized and their optoelectronic properties deserve to be unraveled. Among others, new compositions such as A'2An-1MnX3n+1 afford layered structures with a controlled number (n) of octahedra in the perovskite layer and thus offer an ideal platform for fundamental understanding.[6] Here, through a couple of recent examples including newly discovered halide perovskite phases as well as experimental data from the early 90's, we will discuss their optoelectronic properties based on first-principles calculations, semi-empirical and empirical modelling.

Published
2019

49. Interplay between structure and physical properties in organic-inorganic 2D perovskites

Author

Blancon, Jean-Christophe, Even, Jacky, Stier, Andreas, Katan, Claudine, Crochet, Jared, Mohite, Aditya, 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), Technische Universität Munchen - Université Technique de Munich [Munich, Allemagne] (TUM), 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), Los Alamos National Laboratory (LANL), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2019

50. Making and breaking the exciton in layered halide hybrid perovskites

Author

Kepenekian, Mikael, Traoré, Boubacar, Blancon, Jean-Christophe, Pedesseau, Laurent, Nie, Wanyie, Stoumpos, Constantinos, Kanatzidis, Mercouri, Even, Jacky, Mohite, Aditya, Tretiak, Sergei, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), 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], Los Alamos National Laboratory (LANL), University of Crete [Heraklion] (UOC), Northwestern University [Evanston], Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2019

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