Development of ab initio Hubbard parameter calculation schemes in the k-point sampling real-time TDDFT program in CP2K

TL;DR

This paper introduces new ab initio schemes for calculating Hubbard parameters within the RT-TDDFT framework in CP2K, enabling energy-dependent and exchange-correlation reflective calculations.

Contribution

The authors extend the linear-response method to compute energy-dependent Hubbard parameters, comparing its properties with the ACBN0 scheme.

Findings

The new scheme reflects exchange-correlation effects in Hubbard parameters.

Comparison shows no clear accuracy superiority between the schemes.

Each scheme has unique advantages for different dynamical applications.

Abstract

We implemented ab initio Hubbard parameter calculation schemes in the k-point sampling real-time TDDFT (RT-TDDFT) program in CP2K. We propose a new linear-response-based calculation scheme for energy-dependent Hubbard parameters. Our scheme extends the minimum-tracking linear-response method proposed in [Moynihan et al., arXiv preprint arXiv:1704.08076(2017); E. B. Linscott et al., Phys. Rev. B 98, 235157 (2018)] to realize the calculation of energy-dependent Hubbard parameters that reflect the exchange-correlation (xc) effects included in the xc-functional. We discuss the properties of the minimum-tracking linear-response method in comparison to another promising scheme, ACBN0 [Agapito et al., Phys. Rev. X, 5, 011006 (2015)]. We show that, while neither clearly outperforms the other in the accuracy of static property calculations, each has a distinct dynamical application depending on its theoretical formulation.