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Title: Strictly non-adiabatic quantum control of the acetylene dication using an infrared field

Abstract

We demonstrate the existence of a strictly non-adiabatic control pathway in deprotonation of the acetylene dication. This pathway is identified experimentally by measuring a kinetic energy shift in an ion coincidence experiment. We use a time dependent Schrödinger equation simulation to identify which properties most strongly affect our control. We find that resonant control around conical intersections is limited by the speed of non-adiabatic dynamics.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
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  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford Univ., CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  3. Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1632106
Alternate Identifier(s):
OSTI ID: 1617752
Grant/Contract Number:  
AC02-76SF00515; 1504584
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 152; Journal Issue: 18; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Quantum chemical dynamics; Photoionization; Adiabatic process; Potential energy surfaces; Quantum control theory; Stark effect; Deprotonation

Citation Formats

Liekhus-Schmaltz, Chelsea, Zhu, Xiaolei, McCracken, Gregory A., Cryan, James P., Martinez, Todd J., and Bucksbaum, Philip H. Strictly non-adiabatic quantum control of the acetylene dication using an infrared field. United States: N. p., 2020. Web. doi:10.1063/5.0007058.
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Liekhus-Schmaltz, Chelsea, Zhu, Xiaolei, McCracken, Gregory A., Cryan, James P., Martinez, Todd J., & Bucksbaum, Philip H. Strictly non-adiabatic quantum control of the acetylene dication using an infrared field. United States. https://doi.org/10.1063/5.0007058
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Liekhus-Schmaltz, Chelsea, Zhu, Xiaolei, McCracken, Gregory A., Cryan, James P., Martinez, Todd J., and Bucksbaum, Philip H. Thu . "Strictly non-adiabatic quantum control of the acetylene dication using an infrared field". United States. https://doi.org/10.1063/5.0007058. https://www.osti.gov/servlets/purl/1632106.
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@article{osti_1632106,
title = {Strictly non-adiabatic quantum control of the acetylene dication using an infrared field},
author = {Liekhus-Schmaltz, Chelsea and Zhu, Xiaolei and McCracken, Gregory A. and Cryan, James P. and Martinez, Todd J. and Bucksbaum, Philip H.},
abstractNote = {We demonstrate the existence of a strictly non-adiabatic control pathway in deprotonation of the acetylene dication. This pathway is identified experimentally by measuring a kinetic energy shift in an ion coincidence experiment. We use a time dependent Schrödinger equation simulation to identify which properties most strongly affect our control. We find that resonant control around conical intersections is limited by the speed of non-adiabatic dynamics.},
doi = {10.1063/5.0007058},
journal = {Journal of Chemical Physics},
number = 18,
volume = 152,
place = {United States},
year = {2020},
month = {5}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/5.0007058
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Figures / Tables:

FIG. 1 FIG. 1: The potential energy of the acetylene dication along the C-H stretch calculated using a Fractional-Occupation Molecular Orbital Complete-Active-Space Configuration Interaction (FOMO-CASCI) level of theory relative to the ground state neutral molecule. The upper panel shows the field-free 3Σ$^{-}_{g}$ state as a solid black curve. The field-free 3IIu ismore » the blue curve. The green dotted line is the kinetic energy control pathway. This pathway will result in a KER of 4 eV. Dipole coupling can also occur after the Cl, as shown by the yellow dashed line. This pathway results in a KER of 5 eV. The lower panel shows the dynamic Stark shifted potential curves. The diagonal terms of the dipole coupling matrix represent a Stark shift and can therefore affect the position of the Cl. This can change the population distribution after interacting with a field.« less
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