Cost-Efficient High-Resolution Linear Absorption Spectra through Extrapolating the Dipole Moment from Real-Time Time-Dependent Electronic-Structure Theory.

ABSTRACT: We present a novel function fitting method for approximating the propagation of the time-dependent electric dipole moment from real-time electronic structure calculations. Real-time calculations of the electronic absorption spectrum require discrete Fourier transforms of the electric dipole moment. The spectral resolution is determined by the total propagation time, i.e., the trajectory length of the dipole moment, causing a high computational cost. Our developed method uses function fitting on shorter trajectories of the dipole moment, achieving arbitrary spectral resolution through extrapolation. Numerical testing shows that the fitting method can reproduce high-resolution spectra by using short dipole trajectories. The method converges with as little as 100 a.u. dipole trajectories for

SUBMITTER: Hauge E 

PROVIDER: S-EPMC10653104 | biostudies-literature | 2023 Nov

REPOSITORIES: biostudies-literature