Accounting for Electronic Coherences Induced by Broadband Pulses by Using Pulse-Independent Trajectories
Joachim Galiana, Stefano M. Cavaletto, Gilbert Grell, Francisco Fernández-Villoria, Alicia Palacios, Jesús González-Vázquez, Fernando Martín
TL;DR
This paper introduces new methods to model the effects of laser pulses on molecular dynamics without recalculating for each pulse, improving efficiency and accuracy in simulations.
Contribution
The paper presents two trajectory-surface-hopping approaches that account for pump-generated coherences without requiring separate calculations for each pulse.
Findings
The new methods show excellent agreement with simulations that include coherences from the start.
Initial coherences play a significant role in early nonadiabatic dynamics in glycine molecules.
The approaches enable accurate and flexible simulations for pump–probe experiments with broadband laser sources.
Abstract
Recent advances in the generation of ultrashort, few-femtosecond laser pulses in the ultraviolet–visible domain are now enabling the coherent excitation of several electronic states in neutral molecules, with new opportunities for the manipulation of molecular dynamics on ultrafast time scales. Current time-resolved pump–probe experiments can monitor the ensuing coupled electron–nuclear dynamics with ultrashort resolution. Computational modeling of the observables measured in such experiments can be very challenging for medium-sized and large molecules because of (i) the nontrivial treatment of pump-generated coherences with mixed quantum–classical methods and (ii) the high computational cost of probe-step calculations, which cannot be afforded when many different pump pulses have to be considered, as e.g., in control schemes. In this work, we present two trajectory-surface-hopping…
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Taxonomy
TopicsLaser-Matter Interactions and Applications · Spectroscopy and Quantum Chemical Studies · Photoreceptor and optogenetics research