To describe successive ionization steps of a many-electron atom or molecule driven by an ultrashort, intense laser pulse, we introduce a hierarchy of successive two-subspace Feshbach partitions of the N-electron Hilbert space, and solve the partitioned time-dependent Schrödinger equation by a short-time unitary algorithm. The partitioning scheme allows one to use different level of theory to treat the many-electron dynamics in different subspaces. We illustrate the procedure on a simple two-active-electron model molecular system subjected to a few-cycle extreme Ultra-Violet (XUV) pulse to study channel-resolved photoelectron spectra as a function of the pulse's central frequency and duration. We observe how the momentum and kinetic-energy distributions of photoelectrons accompanying the formation of the molecular cation in a given electronic state (channel) change as the XUV few-cycle pulse's width is varied, from a form characteristic of an impulsive ionization regime, corresponding to the limit of a delta-function pulse, to a form characteristic of multiphoton above-threshold ionization, often associated with continuous-wave infinitely long pulse.
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28 December 2013
Research Article|
December 23 2013
Multicomponent dynamics of coupled quantum subspaces and field-induced molecular ionizations
Thanh-Tung Nguyen-Dang;
Thanh-Tung Nguyen-Dang
Département de Chimie,
Université Laval
, Québec, Québec G1K 7P4, Canada
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Jérémy Viau-Trudel
Jérémy Viau-Trudel
Département de Chimie,
Université Laval
, Québec, Québec G1K 7P4, Canada
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J. Chem. Phys. 139, 244102 (2013)
Article history
Received:
July 30 2013
Accepted:
December 04 2013
Citation
Thanh-Tung Nguyen-Dang, Jérémy Viau-Trudel; Multicomponent dynamics of coupled quantum subspaces and field-induced molecular ionizations. J. Chem. Phys. 28 December 2013; 139 (24): 244102. https://doi.org/10.1063/1.4849755
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