Hybrid XC functionals in all-electron RT-TDDFT simulation of extended periodic systems

Over the past twenty years real-time time-dependent density functional theory (RT-TDDFT) has emerged as an efficient and accurate method for studying electron dynamics in extended periodic systems[1]. Despite this progress, RT-TDDFT calculations still predominantly employ LDA and GGA exchange-correlation (XC) approximations, while ground-state DFT has increasingly adopted more sophisticated XC functionals, including hybrid XC functionals. Hybrid XC functionals, which incorporate some fraction of exact exchange, are known to improve key ground-state quantities as well as real-time observables such as the optical absorption spectrum. In this work we extend the localized resolution of identity (RI-LVL)[2] implementation of FHI-AIMS[3] code in the context of RT-TDDFT, particularly for extended periodic systems. We first demonstrate that RI-LVL reproduces the results of the established RI-V method using isolated systems. We then discuss the implementation for extended periodic systems, contrasting with our RT-TDDFT implementation based on plane-wave pseudopotential formalism[4].



[1] J. Xu et al., Journal of the American Chemical Society 146, 5011 (2024).

[2] A. C. Ihrig et al., New Journal of Physics 17, 093020 (2015).

[3] J. W. Abbott et al., 2025), p. arXiv:2505.00125.

[4] C. Shepard et al., The Journal of Chemical Physics 161 (2024).