Details
| Original language | English |
|---|---|
| Pages (from-to) | 2249-2270 |
| Number of pages | 22 |
| Journal | Zeitschrift fur Physikalische Chemie |
| Volume | 238 |
| Issue number | 12 |
| Early online date | 22 Jul 2024 |
| Publication status | Published - 17 Dec 2024 |
Abstract
Hybrid perovskite materials, known for their potential in cost-effective optoelectronic applications, face a knowledge gap in crucial areas, particularly the atomic-level properties of the surface. This study addresses this challenge by refining ab initio methods for characterizing surface structures of cubic methylammonium lead bromide and methylammonium tin bromide (MAMeBr3 with Me = Sn, Pb), avoiding superficial restrictions in atomic movement during geometry optimization. The resulting structures confirmed nearly random MA+ molecule alignment, comparable to real-world experimental conditions. Calculating surface energies for these structures with crystal orientations {100} and {110}, each with different terminations, provides valuable insights into structural properties. Using a carefully chosen thermodynamic reference state, mimicking experimental conditions enables a thermodynamic discussion and facilitates the modulation of the MeBr2 component's chemical potential. This modulation, in turn, allows for the prediction of crystal morphologies, as illustrated by Wulff's construction. This approach establishes a crucial link between theoretical predictions and experimental conditions, shedding light on the complexities of hybrid perovskite materials.
Keywords
- ab initio thermodynamics, density functional theory, hybrid perovskites (HYPE), methylammonium lead bromide, shape-related properties
ASJC Scopus subject areas
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: Zeitschrift fur Physikalische Chemie, Vol. 238, No. 12, 17.12.2024, p. 2249-2270.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Ab initio study of surfaces of lead and tin based metal halide perovskite structures
AU - Kuper, Henning
AU - Jörg August, Becker
N1 - Publisher Copyright: © 2024 Walter de Gruyter GmbH, Berlin/Boston.
PY - 2024/12/17
Y1 - 2024/12/17
N2 - Hybrid perovskite materials, known for their potential in cost-effective optoelectronic applications, face a knowledge gap in crucial areas, particularly the atomic-level properties of the surface. This study addresses this challenge by refining ab initio methods for characterizing surface structures of cubic methylammonium lead bromide and methylammonium tin bromide (MAMeBr3 with Me = Sn, Pb), avoiding superficial restrictions in atomic movement during geometry optimization. The resulting structures confirmed nearly random MA+ molecule alignment, comparable to real-world experimental conditions. Calculating surface energies for these structures with crystal orientations {100} and {110}, each with different terminations, provides valuable insights into structural properties. Using a carefully chosen thermodynamic reference state, mimicking experimental conditions enables a thermodynamic discussion and facilitates the modulation of the MeBr2 component's chemical potential. This modulation, in turn, allows for the prediction of crystal morphologies, as illustrated by Wulff's construction. This approach establishes a crucial link between theoretical predictions and experimental conditions, shedding light on the complexities of hybrid perovskite materials.
AB - Hybrid perovskite materials, known for their potential in cost-effective optoelectronic applications, face a knowledge gap in crucial areas, particularly the atomic-level properties of the surface. This study addresses this challenge by refining ab initio methods for characterizing surface structures of cubic methylammonium lead bromide and methylammonium tin bromide (MAMeBr3 with Me = Sn, Pb), avoiding superficial restrictions in atomic movement during geometry optimization. The resulting structures confirmed nearly random MA+ molecule alignment, comparable to real-world experimental conditions. Calculating surface energies for these structures with crystal orientations {100} and {110}, each with different terminations, provides valuable insights into structural properties. Using a carefully chosen thermodynamic reference state, mimicking experimental conditions enables a thermodynamic discussion and facilitates the modulation of the MeBr2 component's chemical potential. This modulation, in turn, allows for the prediction of crystal morphologies, as illustrated by Wulff's construction. This approach establishes a crucial link between theoretical predictions and experimental conditions, shedding light on the complexities of hybrid perovskite materials.
KW - ab initio thermodynamics
KW - density functional theory
KW - hybrid perovskites (HYPE)
KW - methylammonium lead bromide
KW - shape-related properties
UR - http://www.scopus.com/inward/record.url?scp=85199411955&partnerID=8YFLogxK
U2 - 10.1515/zpch-2024-0616
DO - 10.1515/zpch-2024-0616
M3 - Article
AN - SCOPUS:85199411955
VL - 238
SP - 2249
EP - 2270
JO - Zeitschrift fur Physikalische Chemie
JF - Zeitschrift fur Physikalische Chemie
SN - 0942-9352
IS - 12
ER -