Optical response of extended systems from time-dependent Hartree-Fock and time-dependent density-functional theory

Bernasconi, L; Webster, R; Tomic, S; Harrison, NM

Abstract

We describe a unified formulation of time-dependent Hartree-Fock (TD-HF) and time-dependent density-functional theory (TD-DFT) for the accurate and efficient calculation of the optical response of infinite (periodic) systems. The method is formulated within the linear-response approximation, but it can easily be extended to include higher-order response contributions, and, in TD-DFT, it can treat with comparable computational efficiency purely local, semi-local or fully non-local approximations for the ground-state exchange-correlation (XC) functional and for the response TD-DFT XC kernel in the adiabatic approximation. At variance with existing methods for computing excitation energies based on the diagonalisation of suitable coupling matrices, or on the inversion of a dielectric matrix, our approach exploits an iterative procedure similar to a standard self-consistent field calculation. This results in a particularly efficient treatment of the coupling of excitations at different k points in the Brillouin zone. As a consequence, our method has the potential to describe completely from first principles the optically induced formation of bound particle-hole pairs in wide classes of materials. This point is illustrated by computing the optical gaps of a series of representative bulk semiconductors, (non-spin polarised) oxides and ionic insulators.

Citation

Bernasconi, L., Webster, R., Tomic, S., & Harrison, N. (2012). Optical response of extended systems from time-dependent Hartree-Fock and time-dependent density-functional theory. Journal of Physics: Conference Series, 367, 012001. https://doi.org/10.1088/1742-6596/367/1/012001

• Journal Article Type: Article
• Acceptance Date: May 11, 2012
• Publication Date: May 21, 2012
• Deposit Date: Apr 6, 2016
• Journal: Journal of Physics: Conference Series
• Print ISSN: 1742-6588
• Electronic ISSN: 1742-6596
• Publisher: IOP Publishing
• Volume: 367
• Pages: 012001
• DOI: https://doi.org/10.1088/1742-6596/367/1/012001
• Publisher URL: http://dx.doi.org/10.1088/1742-6596/367/1/012001
• Related Public URLs: http://iopscience.iop.org/journal/1742-6596