Time-dependent coupled cluster theory for ultrafast transient absorption spectroscopy

• URL: http://arxiv.org/abs/2005.12749v1
• Date: Tue, 26 May 2020 14:15:45 GMT
• Title: Time-dependent coupled cluster theory for ultrafast transient absorption spectroscopy
• Authors: Andreas S. Skeidsvoll, Alice Balbi and Henrik Koch
• Abstract summary: We present a spin-adapted time-dependent coupled cluster singles and doubles model for the molecular response to a sequence of ultrashort laser pulses. We assess the accuracy of the integration procedures used in solving the dynamic coupled cluster equations.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• 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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