Time-dependent coupled-cluster theory for ultrafast transient-absorption spectroscopy

Andreas S. Skeidsvoll, Alice Balbi, and Henrik Koch
Phys. Rev. A 102, 023115 – Published 20 August 2020

Abstract

We present a spin-adapted time-dependent coupled-cluster singles and doubles model for the molecular response to a sequence of ultrashort laser pulses. The implementation is used to calculate the electronic response to a valence-exciting pump pulse, and a subsequent core-exciting probe pulse. We assess the accuracy of the integration procedures used in solving the dynamic coupled-cluster equations, in order to find a compromise between computational cost and accuracy. The transient absorption spectrum of lithium fluoride is calculated for various delays of the probe pulse with respect to the pump pulse. We observe that the transient probe absorption oscillates with the pump-probe delay, an effect that is attributed to the interference of states in the pump-induced superposition.

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  • Received 22 May 2020
  • Accepted 24 July 2020

DOI:https://doi.org/10.1103/PhysRevA.102.023115

©2020 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Andreas S. Skeidsvoll1,*, Alice Balbi2,*, and Henrik Koch1,2,†

  • 1Department of Chemistry, Norwegian University of Science and Technology, NO-7491 Trondheim, Norway
  • 2Scuola Normale Superiore, Piazza dei Cavalieri, 7, IT-56126 Pisa, Italy

  • *These authors contributed equally to this work.
  • henrik.koch@sns.it

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Vol. 102, Iss. 2 — August 2020

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