Effect of XC functionals and dispersion corrections on the DFT‐computed structural and vibrational properties of SrCl2–NaCl and ZrF4–LiF

Mofrad, Amir M.; Christian, Matthew S.; Schorne‐Pinto, Juliano; Palma, Jorge P. S.; Besmann, Theodore M.

doi:10.1002/jrs.6670

Effect of XC functionals and dispersion corrections on the DFT‐computed structural and vibrational properties of SrCl₂–NaCl and ZrF₄–LiF

Journal Article · Wed Apr 10 00:00:00 EDT 2024 · Journal of Raman Spectroscopy

DOI:https://doi.org/10.1002/jrs.6670· OSTI ID:2589263

^[1]; Christian, Matthew S. ^[1]; Schorne‐Pinto, Juliano ^[1]; Palma, Jorge P. S. ^[1]; Besmann, Theodore M. ^[1]

Univ. of South Carolina, Columbia, SC (United States)

Density functional theory (DFT) calculations were performed to examine the impact of exchange–correlation (XC) functionals and van der Waals corrections (specifically the D3 method) on the structural and vibrational properties of the SrCl₂–NaCl and ZrF₄–LiF salt systems. Multiple XC functionals, including the local density approximation (LDA), the generalized gradient approximation using the Perdew–Burke–Ernzerhof (PBE) model, and its modified form suitable for solids (PBEsol), the dispersion-corrected PBE-D3 and PBEsol-D3, were considered. Of these functionals, LDA was found to exhibit the highest degree of error, while PBEsol and PBE-D3 displayed the least error. Underestimated lattice parameters compared with experimental values were observed to result in higher force constants, leading to an overprediction of vibrational frequencies. Conversely, an overestimation of lattice parameters was associated with lower vibrational frequencies. The methodology presented in this study yielded results that are in good agreement with experiment, irrespective of the method (finite differences vs. density functional perturbation theory) employed for calculating infrared and Raman spectra. It was further demonstrated that for alkali halides with weak Raman scattering, utilizing a supercell constructed from primitive cells better predicts Raman features than does the use of conventional cells.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Nuclear Energy (NE), Nuclear Energy University Program (NEUP)

Grant/Contract Number:: NA0003525; NE0008772

OSTI ID:: 2589263

Journal Information:: Journal of Raman Spectroscopy, Journal Name: Journal of Raman Spectroscopy Journal Issue: 7 Vol. 55; ISSN 0377-0486; ISSN 1097-4555

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Effect of XC functionals and dispersion corrections on the DFT‐computed structural and vibrational properties of SrCl2–NaCl and ZrF4–LiF

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Effect of XC functionals and dispersion corrections on the DFT‐computed structural and vibrational properties of SrCl₂–NaCl and ZrF₄–LiF