TY  - JOUR
A1  - Klinkusch, Stefan
A1  - Klamroth, Tillmann
T1  - Simulations of pump-probe exitations of electronic wave packets for a  large qusi-rigid molecular system by means of an extension to the time-dependent configuration interaction singles method
JF  - Journal of theoretical and computational chemistry
N2  - In this paper, we report simulations of laser-driven many-electron dynamics by means of the time-dependent configuration interaction singles (TD-CIS) approach. Photoionization is included by a heuristic model within calculations employing standard Gaussian basis sets. Benzo[g]-N-methyl-quinolinium-7-hydroxylate (BMQ7H) serves as a test system to generate predefined wave packets, i.e. a superposition between the ground and fifth excited state, in a large molecule. For this molecule, these two states have a very similar geometry, which enables us to use the fixed nuclei approximation. Furthermore, this geometric stability would also prevent a dephasing of the electron wave packet due to nuclear dynamics in an experimental realization of our simulations. We also simulate the possible detection of such a wave packet by ultra short probe laser pulses, i.e. pump-probe spectra.
KW  - Electron dynamics
KW  - time-dependent configuration interaction
KW  - pump-probe
Y1  - 2013
U6  - https://doi.org/10.1142/S0219633613500053
SN  - 0219-6336
VL  - 12
IS  - 3
PB  - World Scientific
CY  - Singapore
ER  - 
TY  - JOUR
A1  - White, Alec F.
A1  - Heide, Chiara Josephine
A1  - Saalfrank, Peter
A1  - Head-Gordon, Martin
A1  - Luppi, Eleonora
T1  - Computation of high-harmonic generation spectra of the hydrogen molecule using time-dependent configuration-interaction
JF  - Molecular physics
N2  - Here we apply and expand the knowledge developed in the case of the H atom to describe high-harmonic generation (HHG) for the H-2 molecule by using time-dependent configuration interaction with single excitations. The implications of using a finite atomic orbital basis set and the impact of a heuristic lifetime model which addresses ionisation losses are discussed. We also examine the influence of the angular momentum of the basis on the computed HHG spectra. Moreover, we discuss the impact of adding diffuse functions and ghost atoms in different geometrical configurations around the molecule. The effects of these additional centres on the HHG spectra are correlated with the physical interpretation of this nonlinear optical phenomenon as given by the three-step model, relating the maximal radial extent of the electron as predicted by the model to the radial extent of the Gaussian basis sets. [GRAPHICS] .
KW  - High-harmonic generation
KW  - strong field
KW  - time-dependent configuration interaction
Y1  - 2016
U6  - https://doi.org/10.1080/00268976.2015.1119900
SN  - 0026-8976
SN  - 1362-3028
VL  - 114
SP  - 947
EP  - 956
PB  - Springer
CY  - Abingdon
ER  -