Time-dependent coupled cluster theory for ultrafast transient absorption spectroscopy

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.

12 pages, 9 figures

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Cited by in corpus (16)

• Accurate Relativistic Real-Time Time-Dependent Density Functional Theory for Valence and Core Attosecond Transient Absorption Spectroscopy
• Electron Dynamics with the Time-Dependent Density Matrix Renormalization Group
• Interpretation of Coupled-Cluster Many-Electron Dynamics in Terms of Stationary States
• Ab-initio variational wave functions for the time-dependent many-electron Schrödinger equation
• Simulating weak-field attosecond processes with a Lanczos reduced basis approach to time-dependent equation of motion coupled cluster theory
• Coupled nuclear and electron dynamics in the vicinity of a conical intersection
• Linear and nonlinear optical properties from TDOMP2 theory
• Cost-Efficient High-Resolution Linear Absorption Spectra Through Extrapolating the Dipole Moment from Real-Time Time-Dependent Electronic-Structure Theory
• Comparing real-time coupled cluster methods through simulation of collective Rabi oscillations
• Transient spectroscopy from time-dependent electronic-structure theory without multipole expansions
• Adiabatic extraction of nonlinear optical properties from real-time time-dependent electronic-structure theory
• Revealing fingerprints of valence excitons in x-ray absorption spectra with the Bethe-Salpeter equation
• Coupled cluster simulation of impulsive stimulated X-ray Raman scattering
• First-principles approach to ultrafast pump-probe spectroscopy in solids
• Energy-filtered excited states and real-time dynamics served in a contour integral
• Chemical Interpretation of Time-Dependent Coupled-Cluster Theory