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Efficient simulation of resonance Raman spectra with tight-binding approximations to density functional theory

Ashtari Jafari, S ; Sharif University of Technology | 2022

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  1. Type of Document: Article
  2. DOI: 10.1063/5.0107220
  3. Publisher: American Institute of Physics Inc , 2022
  4. Abstract:
  5. Resonance Raman spectroscopy has long been established as one of the most sensitive techniques for detection, structure characterization, and probing the excited-state dynamics of biochemical systems. However, the analysis of resonance Raman spectra is much facilitated when measurements are accompanied by Density Functional Theory (DFT) calculations that are expensive for large biomolecules. In this work, resonance Raman spectra are therefore computed with the Density Functional Tight-Binding (DFTB) method in the time-dependent excited-state gradient approximation. To test the accuracy of the tight-binding approximations, this method is first applied to typical resonance Raman benchmark molecules, such as β-carotene, and compared to results obtained with pure and range-separated exchange-correlation functionals. We then demonstrate the efficiency of the approach by considering a computationally challenging heme variation. Overall, we find that the vibrational frequencies and excited-state properties (energies and gradients) that are needed to simulate the spectra are reasonably accurate and suitable for interpretation of experiments. We can therefore recommend DFTB as a fast computational method to interpret resonance Raman spectra. © 2022 Author(s)
  6. Keywords:
  7. Binding energy ; Biochemistry ; Computation theory ; Density functional theory ; Design for testability ; Raman scattering ; Resonance ; Biochemical systems ; Density-functional theory calculations ; Density-functional-theory ; Efficient simulation ; Excited-state dynamics ; Resonance Raman spectra ; Resonance Raman spectroscopy ; Sensitive techniques ; Structure characterization ; Tight-binding approximations ; Excited states ; Computer simulation ; Quantum theory ; Raman spectrometry ; Spectrum Analysis, Raman ; Vibration
  8. Source: Journal of Chemical Physics ; Volume 157, Issue 8 , Volume 157, Issue 8 , 2022 ; 00219606 (ISSN)
  9. URL: https://pubs.aip.org/aip/jcp/article/157/8/084104/2841657/Efficient-simulation-of-resonance-Raman-spectra