Band Gaps and Stability of CsSiX3 Halides
Abstract
There is a great current interest in lead-free halide perovskites. While Sn based and Ge based compounds of this type have already been demonstrated experimentally, Si based ones have not. In this paper, the authors consider the possibility of CsSiX3 halide perovskites. While previous work for cubic CsSiI3 found the band gap to close or in fact become inverted and to lead to a topological insulator, the authors show here that in the rhombohedrally distorted structure that occurs because of Si off-centering, the band gap becomes larger than 1.5 eV and possibly of interest for photovoltaics. On the other hand, even in the cubic structure at high temperature, fluctuations of the Si position, will lead to a sizable gap. Here, the total energy calculations, show that the materials are unstable toward 3CsSiI3 → Si2I6 + 3CsI + Si and 2CsSiI3 → SiI4 + 2CsI + Si and are thus above the convex hull. Similar results are presented for halogens: I, Br, Cl.
- Publication Date:
- Research Org.:
- Case Western Reserve Univ., Cleveland, OH (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1593133
- Alternate Identifier(s):
- OSTI ID: 1495813
- Grant/Contract Number:
- SC0008933
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physica Status Solidi. A, Applications and Materials Science
- Additional Journal Information:
- Journal Volume: 216; Journal Issue: 15; Journal ID: ISSN 1862-6300
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; halide perovskite silicon; band structure; halides; metastability; Si‐based
Citation Formats
Radha, Santosh K., and Lambrecht, Walter R. L. Band Gaps and Stability of CsSiX3 Halides. United States: N. p., 2019.
Web. doi:10.1002/pssa.201800962.
Radha, Santosh K., & Lambrecht, Walter R. L. Band Gaps and Stability of CsSiX3 Halides. United States. https://doi.org/10.1002/pssa.201800962
Radha, Santosh K., and Lambrecht, Walter R. L. Thu .
"Band Gaps and Stability of CsSiX3 Halides". United States. https://doi.org/10.1002/pssa.201800962. https://www.osti.gov/servlets/purl/1593133.
@article{osti_1593133,
title = {Band Gaps and Stability of CsSiX3 Halides},
author = {Radha, Santosh K. and Lambrecht, Walter R. L.},
abstractNote = {There is a great current interest in lead-free halide perovskites. While Sn based and Ge based compounds of this type have already been demonstrated experimentally, Si based ones have not. In this paper, the authors consider the possibility of CsSiX3 halide perovskites. While previous work for cubic CsSiI3 found the band gap to close or in fact become inverted and to lead to a topological insulator, the authors show here that in the rhombohedrally distorted structure that occurs because of Si off-centering, the band gap becomes larger than 1.5 eV and possibly of interest for photovoltaics. On the other hand, even in the cubic structure at high temperature, fluctuations of the Si position, will lead to a sizable gap. Here, the total energy calculations, show that the materials are unstable toward 3CsSiI3 → Si2I6 + 3CsI + Si and 2CsSiI3 → SiI4 + 2CsI + Si and are thus above the convex hull. Similar results are presented for halogens: I, Br, Cl.},
doi = {10.1002/pssa.201800962},
journal = {Physica Status Solidi. A, Applications and Materials Science},
number = 15,
volume = 216,
place = {United States},
year = {Thu Feb 21 00:00:00 EST 2019},
month = {Thu Feb 21 00:00:00 EST 2019}
}
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Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Kristallstrukturen und Phasentransformationen von Caesiumtrihalogenogermanaten(II) CsGeX3 (X = Cl, Br, I)
journal, February 1987
- Thiele, Gerhard; Rotter, Heinz Wilhelm; Schmidt, Klaus Dieter
- Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 545, Issue 2
Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013
- Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J.
- Nature, Vol. 501, Issue 7467, p. 395-398
Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012
- Lee, M. M.; Teuscher, J.; Miyasaka, T.
- Science, Vol. 338, Issue 6107, p. 643-647
Electronic band structure trends of perovskite halides: Beyond Pb and Sn to Ge and Si
journal, May 2016
- Huang, Ling-yi; Lambrecht, Walter R. L.
- Physical Review B, Vol. 93, Issue 19
Electronic band structure, phonons, and exciton binding energies of halide perovskites CsSnCl , CsSnBr , and CsSnI
journal, October 2013
- Huang, Ling-yi; Lambrecht, Walter R. L.
- Physical Review B, Vol. 88, Issue 16
Low-temperature processed meso-superstructured to thin-film perovskite solar cells
journal, January 2013
- Ball, James M.; Lee, Michael M.; Hey, Andrew
- Energy & Environmental Science, Vol. 6, Issue 6
Critical issues in the design of polycrystalline, thin-film tandem solar cells
journal, January 2003
- Coutts, Timothy J.; Ward, J. Scott; Young, David L.
- Progress in Photovoltaics: Research and Applications, Vol. 11, Issue 6
Perovskite solar cells: an emerging photovoltaic technology
journal, March 2015
- Park, Nam-Gyu
- Materials Today, Vol. 18, Issue 2
Fusion of the LAPW and LMTO methods: The augmented plane wave plus muffin-tin orbital method
journal, March 2010
- Kotani, Takao; van Schilfgaarde, Mark
- Physical Review B, Vol. 81, Issue 12
Organolead Halide Perovskite: New Horizons in Solar Cell Research
journal, February 2014
- Kim, Hui-Seon; Im, Sang Hyuk; Park, Nam-Gyu
- The Journal of Physical Chemistry C, Vol. 118, Issue 11, p. 5615-5625
Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961
- Shockley, William; Queisser, Hans J.
- Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519
Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013
- Burschka, Julian; Pellet, Norman; Moon, Soo-Jin
- Nature, Vol. 499, Issue 7458, p. 316-319
Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009
- Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo
- Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051
Quasiparticle self-consistent method: A basis for the independent-particle approximation
journal, October 2007
- Kotani, Takao; van Schilfgaarde, Mark; Faleev, Sergey V.
- Physical Review B, Vol. 76, Issue 16
Lattice dynamics in perovskite halides with
journal, November 2014
- Huang, Ling-yi; Lambrecht, Walter R. L.
- Physical Review B, Vol. 90, Issue 19
Quasiparticle Self-Consistent Theory
journal, June 2006
- van Schilfgaarde, M.; Kotani, Takao; Faleev, S.
- Physical Review Letters, Vol. 96, Issue 22
Dynamic Stereochemical Activity of the Sn 2+ Lone Pair in Perovskite CsSnBr 3
journal, September 2016
- Fabini, Douglas H.; Laurita, Geneva; Bechtel, Jonathon S.
- Journal of the American Chemical Society, Vol. 138, Issue 36
All-electron quasiparticle self-consistent band structures for including lattice polarization corrections in different phases
journal, January 2018
- Bhandari, Churna; van Schilgaarde, Mark; Kotani, Takao
- Physical Review Materials, Vol. 2, Issue 1
Distortion modes in halide perovskites: To twist or to stretch, a matter of tolerance and lone pairs
journal, June 2018
- Radha, Santosh Kumar; Bhandari, Churna; Lambrecht, Walter R. L.
- Physical Review Materials, Vol. 2, Issue 6
Morphological Control for High Performance, Solution-Processed Planar Heterojunction Perovskite Solar Cells
journal, September 2013
- Eperon, Giles E.; Burlakov, Victor M.; Docampo, Pablo
- Advanced Functional Materials, Vol. 24, Issue 1, p. 151-157
Modeling of two‐junction, series‐connected tandem solar cells using top‐cell thickness as an adjustable parameter
journal, August 1990
- Kurtz, Sarah R.; Faine, P.; Olson, J. M.
- Journal of Applied Physics, Vol. 68, Issue 4
Quasiparticle Self-Consistent GW Theory
text, January 2005
- van Schilfgaarde, M.; Kotani, T.; Faleev, S.
- arXiv
Quasiparticle self-consistent $GW$ method; a basis for the independent-particle approximation
text, January 2006
- Kotani, Takao; van Schilfgaarde, Mark; Faleev, Sergey V.
- arXiv