Optimized pulses for Raman excitation through the continuum: Verification using the multiconfigurational time-dependent Hartree-Fock method

Greenman, Loren; Whaley, K. Birgitta; Haxton, Daniel J.; McCurdy, C. William

doi:10.1103/PhysRevA.96.013411

Optimized pulses for Raman excitation through the continuum: Verification using the multiconfigurational time-dependent Hartree-Fock method

Journal Article · Thu Jul 13 00:00:00 EDT 2017 · Physical Review A

DOI:https://doi.org/10.1103/PhysRevA.96.013411· OSTI ID:1465413

Greenman, Loren ^[1]; Whaley, K. Birgitta ^[1]; Haxton, Daniel J. ^[2]; McCurdy, C. William ^[3]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Kenneth S. Pitzer Center for Theoretical Chemistry and Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Davis, CA (United States). Dept. of Chemistry

Here, we have verified a mechanism for Raman excitation of atoms through continuum levels previously obtained by quantum optimal control using the multiconfigurational time-dependent Hartree-Fock (MCTDHF) method. For the optimal control, which requires running multiple propagations to determine the optimal pulse sequence, we used the computationally inexpensive time-dependent configuration interaction singles (TDCIS) method. TDCIS captures all of the necessary correlation of the desired processes but assumes that ionization pathways reached via double excitations are not present. MCTDHF includes these pathways and all multiparticle correlations in a set of time-dependent orbitals. The mechanism that was determined to be optimal in the Raman excitation of the Ne 1s²2s²2p⁵3p¹ valence state via the metastable 1s²2s¹2p⁶3p¹ resonance state involves a sequential resonance-valence excitation. First, a long pump pulse excites the core-hole state, and then a shorter Stokes pulse transfers the population to the valence state. This process represents the first step in a multidimensional x-ray spectroscopy scheme that will provide a local probe of valence electronic correlations. Although at the optimal pulse intensities at the TDCIS level of theory the MCTDHF method predicts multiple ionization or excitation ionization of the atom, at slightly lower intensities (reduced by a factor of about 4) the TDCIS mechanism is shown to hold qualitatively. Quantitatively, the MCTDHF populations are reduced from the TDCIS calculations by a factor of 4.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1465413

Alternate ID(s):: OSTI ID: 1369580

Journal Information:: Physical Review A, Journal Name: Physical Review A Journal Issue: 1 Vol. 96; ISSN PLRAAN; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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