Numerical calculations of multiphoton molecular absorption

Author(s)

Brian Kaufman, Philipp Marquetand, Thomas Weinacht, Tamas Rozgonyi

Abstract

Motivated by the possibility of multiphoton-driven pump-probe experiments, such as time-resolved photoelectron spectroscopy, we carry out essential states's calculations of strong-field molecular excitation by solving the time-dependent Schrödinger equation for a molecule in a high-intensity laser field. Usually such calculations rely on adiabatic elimination, but here we make direct use of a large number of energies and transition dipole moments obtained from electronic structure calculations. In this way, we capture a range of multiphoton absorption orders, from 2 to 5, and include dynamic Stark shifts naturally. We consider a range of laser frequencies and intensities to characterize several multiphoton resonances and dynamic Stark shifts. The calculations also include averaging over molecular orientation and geometry, but are carried out for frozen nuclei, which is relevant in the limit of very short laser pulses (

Organisation(s)

Department of Theoretical Chemistry, Research Platform Accelerating Photoreaction Discovery

External organisation(s)

State University of New York, Stony Brook, Hungarian Academy of Sciences

Journal

Physical Review A

Volume

106

No. of pages

10

ISSN

2469-9926

DOI

https://doi.org/10.1103/PhysRevA.106.013111

Publication date

07-2022

Peer reviewed

Yes

Austrian Fields of Science 2012

103036 Theoretical physics, 104022 Theoretical chemistry, 102009 Computer simulation

Keywords

ASJC Scopus subject areas

Atomic and Molecular Physics, and Optics

Portal url

https://ucrisportal.univie.ac.at/en/publications/numerical-calculations-of-multiphoton-molecular-absorption(58182ef7-7638-4dd7-ba55-a856cacc139b).html