Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping
Abstract
In this work, we report two schemes to generate perfect anisotropy in the photoelectron angular distribution of a randomly oriented ensemble of polyatomic molecules. In order to exert full control over the anisotropy of photoelectron emission, we exploit interferences between single-photon pathways and a manifold of resonantly enhanced two-photon pathways. These are shown to outperform nonsequential (ω, 2ω) bichromatic phase control for the example of CHFClBr molecules. We are able to optimize pulses that yield anisotropic photoelectron emission thanks to a very efficient calculation of photoelectron momentum distributions. Finally, this is accomplished by combining elements of quantum chemistry, variational scattering theory, and time-dependent perturbation theory.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1577608
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 7; 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; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Goetz, R. Esteban, Koch, Christiane P., and Greenman, Loren. Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping. United States: N. p., 2019.
Web. doi:10.1063/1.5111362.
Goetz, R. Esteban, Koch, Christiane P., & Greenman, Loren. Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping. United States. https://doi.org/10.1063/1.5111362
Goetz, R. Esteban, Koch, Christiane P., and Greenman, Loren. Thu .
"Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping". United States. https://doi.org/10.1063/1.5111362. https://www.osti.gov/servlets/purl/1577608.
@article{osti_1577608,
title = {Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping},
author = {Goetz, R. Esteban and Koch, Christiane P. and Greenman, Loren},
abstractNote = {In this work, we report two schemes to generate perfect anisotropy in the photoelectron angular distribution of a randomly oriented ensemble of polyatomic molecules. In order to exert full control over the anisotropy of photoelectron emission, we exploit interferences between single-photon pathways and a manifold of resonantly enhanced two-photon pathways. These are shown to outperform nonsequential (ω, 2ω) bichromatic phase control for the example of CHFClBr molecules. We are able to optimize pulses that yield anisotropic photoelectron emission thanks to a very efficient calculation of photoelectron momentum distributions. Finally, this is accomplished by combining elements of quantum chemistry, variational scattering theory, and time-dependent perturbation theory.},
doi = {10.1063/1.5111362},
journal = {Journal of Chemical Physics},
number = 7,
volume = 151,
place = {United States},
year = {Thu Aug 15 00:00:00 EDT 2019},
month = {Thu Aug 15 00:00:00 EDT 2019}
}
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