Fast real-time time-dependent density functional theory calculations with the parallel transport gauge

Research paper by Weile Jia, Dong An, Lin-Wang Wang, Lin Lin

Indexed on: 26 May '18Published on: 26 May '18Published in: arXiv - Physics - Computational Physics


Real-time time-dependent density functional theory (RT-TDDFT) is known to be hindered by the very small time step (attosecond or smaller) needed in the numerical simulation due to the fast oscillation of electron wavefunctions, which significantly limits its range of applicability for the study of ultrafast dynamics. In this paper, we demonstrate that such oscillation can be considerably reduced by optimizing the gauge choice using the parallel transport formalism. RT-TDDFT calculations can thus be significantly accelerated using a combination of the parallel transport gauge and implicit integrators, and the resulting scheme can be used to accelerate any electronic structure software that uses a Schr\"odinger representation. Using absorption spectrum, ultrashort laser pulse, and Ehrenfest dynamics calculations for example, we show that the new method can utilize a time step that is on the order of $10\sim 100$ attoseconds in a planewave basis set, and is no less than $5\sim 10$ times faster when compared to the standard explicit 4th order Runge-Kutta time integrator.