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Title: Electronic and optical properties of orthorhombic (CH 3 NH 3 )BX 3 (B = Sn, Pb; X = F, Cl, Br, I) perovskites: a first-principles investigation

Journal Article · · RSC Advances
DOI:https://doi.org/10.1039/D1RA01586A· OSTI ID:1798236
 [1];  [2];  [3]; ORCiD logo [2]
  1. National Energy Technology Laboratory, United States Department of Energy, Pittsburgh, USA, Chemical Engineering Department
  2. National Energy Technology Laboratory, United States Department of Energy, Pittsburgh, USA
  3. Chemical Engineering Department, Louisiana Tech, University, Ruston, USA
+ Show Author Affiliations

Lead halide perovskites have generated considerable interest in solar cell, sensor, and electronics applications. While great focus has been placed on (CH3NH3)PbI3, an organic–inorganic hybrid perovskite, comparatively little work has been done to understand some of its existing crystal phases and analogous materials after substituting with Sn and/or other halogens in the framework. Here, first-principles density functional theory calculations are performed to comprehensively evaluate the electronic and optical properties of (CH3NH3)BX3 (B = Sn, Pb; X = F, Cl, Br, I) in a low-temperature orthorhombic phase. Bulk modulus, electronic structures, and several optical properties of these perovskite systems are further calculated. The obtained results are first confirmed by comparing with existing perovskite systems in literature. The shifting trends on those physical properties when extending to other barely studied systems of (CH3NH3)BX3 is further revealed. The band gap of these perovskites is found to decrease when varying halogen anion in “X” sites from F to I, and/or substituting Pb cations with Sn in “B” sites. Notably, the less toxic Sn-containing perovskites, (CH3NH3)SnI3 in particular, display higher absorption coefficients in the visible light range than their Pb-containing counterparts. An orthorhombic (CH3NH3)PbF3 is predicted to exist at low temperature, and adsorb strongly UV energy. Our systematical examination efforts on the two groups of perovskites provide valuable physical insights in these materials, and the accompanied new findings warrant further investigation on such subjects.

Research Organization:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
Sponsoring Organization:
USDOE Office of Fossil Energy (FE)
Grant/Contract Number:
FWP-1022427
OSTI ID:
1798236
Alternate ID(s):
OSTI ID: 1822164; OSTI ID: 1822165
Journal Information:
RSC Advances, Journal Name: RSC Advances Vol. 11 Journal Issue: 36; ISSN 2046-2069
Publisher:
Royal Society of Chemistry (RSC)Copyright Statement
Country of Publication:
United Kingdom
Language:
English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY