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Preprint
Accuracy and limitations of the bond polarizability model in modeling of Raman scattering from molecular dynamics simulations
arXiv.org
11 Jun 2024
Abstract
Calculation of Raman scattering from molecular dynamics (MD) simulations
requires accurate modeling of the evolution of the electronic polarizability of
the system along its MD trajectory. For large systems, this necessitates the
use of atomistic models to represent the dependence of electronic
polarizability on atomic coordinates. The bond polarizability model (BPM) is
the simplest such model and has been used for modeling the Raman spectra of
molecular systems but has not been applied to solid-state systems. Here, we
systematically investigate the accuracy and limitations of the BPM
parameterized from density functional theory (DFT) results for a series of
simple molecules such as CO2, SO2, H2S, H2O, NH3, and CH4, the more complex
CH2O, CH3OH and CH3CH2OH and thiophene molecules and the BaTiO3 and CsPbBr3
perovskite solids. We find that BPM can reliably reproduce the overall features
of the Raman spectra such as shifts of peak positions. However, with the
exception of highly symmetric systems, the assumption of non-interacting bonds
limits the quantitative accuracy of the BPM; this assumption also leads to
qualitatively inaccurate polarizability evolution and Raman spectra for systems
where large deviations from the ground state structure are present.
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Details
- Title
- Accuracy and limitations of the bond polarizability model in modeling of Raman scattering from molecular dynamics simulations
- Creators
- Atanu PaulMaya RubensteinAnthony RuffinoStefan MasiukJonathan SpanierIlya Grinberg
- Publication Details
- arXiv.org
- Resource Type
- Preprint
- Language
- English
- Academic Unit
- Physics; Materials Science and Engineering; Mechanical Engineering and Mechanics
- Other Identifier
- 991021888815304721