Time-Resolved Electronic Spectra with Efficient Quantum Dynamics Methods

Marius Wehrle; Miroslav Šulc; Jiří Vaníček

doi:10.2533/chimia.2011.334

Time-Resolved Electronic Spectra with Efficient Quantum Dynamics Methods

Authors

Marius Wehrle Ecole Polytechnique Fédérale de Lausanne, Institut des Sciences et Ingénierie Chimiques, Laboratory of Theoretical Physical Chemistry, EPFL SB ISIC LCPT, BCH 3110, CH-1015 Lausanne
Miroslav Šulc Ecole Polytechnique Fédérale de Lausanne, Institut des Sciences et Ingénierie Chimiques, Laboratory of Theoretical Physical Chemistry, EPFL SB ISIC LCPT, BCH 3110, CH-1015 Lausanne
Jiří Vaníček Ecole Polytechnique Fédérale de Lausanne, Institut des Sciences et Ingénierie Chimiques, Laboratory of Theoretical Physical Chemistry, EPFL SB ISIC LCPT, BCH 3110, CH-1015 Lausanne;, Email: jiri.vanicek@epfl.ch

DOI:

https://doi.org/10.2533/chimia.2011.334

Keywords:

Pump-probe, Quantum dynamics, Semiclassical approximation, Split-operator method, Stimulated emission

Abstract

We explore three specific approaches for speeding up the calculation of quantum time correlation functions needed for time-resolved electronic spectra. The first relies on finding a minimum set of sufficiently accurate electronic surfaces. The second increases the time step required for convergence of exact quantum simulations by using different split-step algorithms to solve the time-dependent Schrödinger equation. The third approach lowers the number of trajectories needed for convergence of approximate semiclassical dynamics methods.