Dielectrics in a time-dependent electric field: a real-time approach based on density-polarization functional theory

M Grüning (1) , D Sangalli (2) , Claudio Attaccalite (3, 4)

1 QUB - Queen's University [Belfast]
2 Dipartimento di Fisica (Milano)
3 NEEL - TMC - Théorie de la Matière Condensée
4 CINaM - Centre Interdisciplinaire de Nanoscience de Marseille

In the presence of a (time-dependent) macroscopic electric field the electron dynamics of dielectrics cannot be described by the time-dependent density only. We present a real-time formalism that has the density and the macroscopic polarization P as key quantities. We show that a simple local function of P already captures long-range correlation in linear and nonlinear optical response functions. Specifically, after detailing the numerical implementation, we examine the optical absorption, the second-and third-harmonic generation of bulk Si, GaAs, AlAs and CdTe at different level of approximation. We highlight links with ultranonlocal exchange-correlation functional approximations proposed within linear response time-dependent density functional theory framework.

Domains: Materials Science [cond-mat.mtrl-sci]

M Grüning, D Sangalli, Claudio Attaccalite. Dielectrics in a time-dependent electric field: a real-time approach based on density-polarization functional theory. Physical Review B, 2016, 94 (3), pp.035149. ⟨10.1103/PhysRevB.94.035149⟩. ⟨hal-01320532⟩