Quasiparticle Band Structure and Phonon-Induced Band Gap Renormalization of the Lead-Free Halide Double Perovskite Cs2InAgCl6
| العنوان: | Quasiparticle Band Structure and Phonon-Induced Band Gap Renormalization of the Lead-Free Halide Double Perovskite Cs2InAgCl6 |
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| المؤلفون: | George Volonakis, Viet-Anh Ha, Hyungjun Lee, Feliciano Giustino, Marios Zacharias |
| المساهمون: | University of Texas at Austin [Austin], 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), Cyprus University of Technology, Robert A. Welch FoundationThe Welch Foundation [F-1990-20190330], Computational Materials Sciences Program - U.S. Department of Energy, Office of Science, Basic Energy Sciences United States Department of Energy (DOE) [DESC0020129], LRAC award [2007638], Office of Science of the U.S. Department of Energy United States Department of Energy (DOE) [DE-AC02-05CH11231], 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) |
| المصدر: | Journal of Physical Chemistry C Journal of Physical Chemistry C, 2021, 125 (39), pp.21689-21700. ⟨10.1021/acs.jpcc.1c06542⟩ Journal of Physical Chemistry C, American Chemical Society, 2021, 125 (39), pp.21689-21700. ⟨10.1021/acs.jpcc.1c06542⟩ |
| بيانات النشر: | HAL CCSD, 2021. |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | Materials science, Band gap, Phonon, Halide, 02 engineering and technology, Perovskite, 01 natural sciences, Renormalization, Condensed Matter::Materials Science, Phonon-induced gap, 0103 physical sciences, Doping, [CHIM]Chemical Sciences, Physical and Theoretical Chemistry, 010306 general physics, Electronic band structure, Eigenvalues and eigenfunctions, Condensed matter physics, Materials Engineering, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Light emission properties, General Energy, Quasiparticle, Engineering and Technology, Double perovskite, Condensed Matter::Strongly Correlated Electrons, 0210 nano-technology |
| الوصف: | International audience; The lead-free halide double perovskite Cs2InAgCl6 was recently designed in silico and subsequently synthesized in the lab. This perovskite is a wide-gap semiconductor with a direct band gap and exhibits extraordinary photoluminescence in the visible range upon Na doping. The light emission properties of Cs2InAgCl6 have successfully been exploited to fabricate stable single-emitter-based white-light LEDs with near unity quantum efficiency. An intriguing puzzle in the photophysics of this compound is that the onset of optical absorption is around 3 eV, but the luminescence peak is found around 2 eV. As a first step toward elucidating this mismatch and clarifying the atomic-scale mechanisms underpinning the observed luminescence, here, we report a detailed investigation of the quasiparticle band structure of Cs2InAgCl6 as well as the phonon-induced renormalization of the band structure. We perform calculations of bang gaps and effective masses using the GW method, and we calculate the phonon-induced band structure renormalization using the special displacement method. We find that GW calculations are rather sensitive to the functional used in the density functional theory calculations and that self-consistency on the eigenvalues is necessary to achieve quantitative agreement with experiments. Our most accurate band gap at room temperature is in the range of 3.1-3.2 eV and includes a phonon-induced gap renormalization of 0.2 eV. By computing the phonon-induced mass enhancement, we find that the electron carriers are in the weak polaronic coupling regime, while hole carriers are in the intermediate coupling regime as a result of the localized and directional nature of the Ag e(g) 4d states at the valence band top. |
| وصف الملف: | |
| اللغة: | English |
| تدمد: | 1932-7447 1932-7455 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::7fb24f45143f1c1bf575edbe32c044e9 https://hal.science/hal-03413902/file/manuscript-1.pdf |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.doi.dedup.....7fb24f45143f1c1bf575edbe32c044e9 |
| قاعدة البيانات: | OpenAIRE |
Find this issue from the American Chemical Society | تدمد: | 19327447 19327455 |
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