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Preprint
An atomistic model of electronic polarizability for calculation of Raman scattering from large-scale MD simulations
ArXiv.org
15 Apr 2023
Abstract
The application of molecular dynamics (MD) simulations to the interpretation of Raman scattering spectra is hindered by inability of atomistic simulations to account for the dynamic evolution of electronic polarizability, requiring the use of either ab initio method or parameterization of machine learning models. More broadly, the dynamic evolution of electronic-structure-derived properties cannot be treated by the current atomistic models. Here, we report a simple, physically-based atomistic model with few (maximum 10 parameters for the systems considered here) adjustable parameters that can accurately represent the changes in the electronic polarizability tensor for molecules and solid-state systems. Due to its compactness, the model can be applied for simulations of Raman spectra of large (~ 1,000,000-atom) systems with modest computational cost. To demonstrate its accuracy, the model is applied to the CO2 molecule, water clusters, and BaTiO3 and CsPbBr3 perovskites and shows good agreement with ab-initio-derived and experimental polarizability tensor and Raman data. The atomistic nature of the model enables local analysis of the contributions to Raman spectra, paving the way for the application of MD simulations for the interpretation of Raman spectroscopy results. Furthermore, our successful atomistic representation of the evolution of electronic polarizability suggests that the evolution of electronic structure and its derivative properties can be represented by atomistic models, opening up the possibility of studies of electronic-structure-dependent properties using large-scale atomistic simulations.
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Details
- Title
- An atomistic model of electronic polarizability for calculation of Raman scattering from large-scale MD simulations
- Creators
- Atanu Paul - Bar-Ilan UniversityAnthony Ruffino - Drexel UniversityStefan Masiuk - Drexel UniversityJonathan Spanier - Drexel UniversityIlya Grinberg - Bar-Ilan University
- Publication Details
- ArXiv.org
- Resource Type
- Preprint
- Language
- English
- Academic Unit
- Materials Science and Engineering; Mechanical Engineering and Mechanics
- Other Identifier
- 991020435968104721