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Journal article
Accuracy and limitations of the bond polarizability model in modeling of Raman scattering from molecular dynamics simulations
The Journal of chemical physics, v 161(6)
14 Aug 2024
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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 the density functional theory results for a series of simple molecules, such as CO2, SO2, H2S, H2O, NH3, and CH4; the more complex CH2O, CH3OH, 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 Paul - Bar-Ilan UniversityMaya Rubenstein - Bar-Ilan UniversityAnthony Ruffino - Drexel UniversityStefan Masiuk - Drexel UniversityJonathan E. Spanier - Drexel UniversityIlya Grinberg - Bar-Ilan University
- Publication Details
- The Journal of chemical physics, v 161(6)
- Publisher
- AIP Publishing
- Number of pages
- 14
- Grant note
- Army Research Office: W911NF-21-1-0126 Army/ARL via the Collaborative for Hierarchical Agile and Responsive Materials (CHARM): W911NF-19-2-0119 Israel Science Foundation: 1479/21
A.P., A.R., S.M., J.E.S., and I.G. acknowledge the support of the Army Research Office under Grant No. W911NF-21-1-0126 and Army/ARL via the Collaborative for Hierarchical Agile and Responsive Materials (CHARM) under cooperative Agreement No. W911NF-19-2-0119. A.P. and I.G. acknowledge additional support from the Israel Science Foundation under Grant No. 1479/21.DAS:The data that support the findings of this study are available from the corresponding author upon reasonable request.
- Resource Type
- Journal article
- Academic Unit
- Physics; Materials Science and Engineering; Mechanical Engineering and Mechanics
- Web of Science ID
- WOS:001290209700021
- Scopus ID
- 2-s2.0-85201241618
- Other Identifier
- 991021897478204721
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Chemistry, Physical
- Physics, Atomic, Molecular & Chemical