Multiscale time-dependent density functional theory: Demonstration for plasmons

• Published in: The Journal of chemical physics Vol. 147; no. 5; p. 054102
• Main Authors: Jiang, Jiajian, Abi Mansour, Andrew, Ortoleva, Peter J
• Format: Journal Article
• Language: English
• Published: United States 07.08.2017
• ISSN: 1089-7690
• DOI: 10.1063/1.4994896

Plasmon properties are of significant interest in pure and applied nanoscience. While time-dependent density functional theory (TDDFT) can be used to study plasmons, it becomes impractical for elucidating the effect of size, geometric arrangement, and dimensionality in complex nanosystems. In this study, a new multiscale formalism that addresses this challenge is proposed. This formalism is based on Trotter factorization and the explicit introduction of a coarse-grained (CG) structure function constructed as the Weierstrass transform of the electron wavefunction. This CG structure function is shown to vary on a time scale much longer than that of the latter. A multiscale propagator that coevolves both the CG structure function and the electron wavefunction is shown to bring substantial efficiency over classical propagators used in TDDFT. This efficiency follows from the enhanced numerical stability of the multiscale method and the consequence of larger time steps that can be used in a discrete time evolution. The multiscale algorithm is demonstrated for plasmons in a group of interacting sodium nanoparticles (15-240 atoms), and it achieves improved efficiency over TDDFT without significant loss of accuracy or space-time resolution.