skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on August 15, 2020

Title: 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.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1]
  1. Kansas State Univ., Manhattan, KS (United States)
  2. Universität Kassel (Germany)
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. doi: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. doi:10.1063/1.5111362.
@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 = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on August 15, 2020
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Control of photoelectron momentum distributions by bichromatic polarization-shaped laser fields
journal, October 2017

  • Kerbstadt, Stefanie; Pengel, Dominik; Johannmeyer, Daniela
  • New Journal of Physics, Vol. 19, Issue 10
  • DOI: 10.1088/1367-2630/aa83a4

Cross section and asymmetry parameter calculation for sulfur 1s photoionization of SF6
journal, September 1999

  • Natalense, Alexandra P. P.; Lucchese, Robert R.
  • The Journal of Chemical Physics, Vol. 111, Issue 12
  • DOI: 10.1063/1.479794

Photoelectron Circular Dichroism with Two Overlapping Laser Pulses of Carrier Frequencies ω and 2 ω Linearly Polarized in Two Mutually Orthogonal Directions
journal, December 2018


Laser Aligned Molecules: Applications in Physics and Chemistry
journal, January 2004


Photoelectron Circular Dichroism of Bicyclic Ketones from Multiphoton Ionization with Femtosecond Laser Pulses
journal, December 2014

  • Lux, Christian; Wollenhaupt, Matthias; Sarpe, Cristian
  • ChemPhysChem, Vol. 16, Issue 1
  • DOI: 10.1002/cphc.201402643

General phenomenology of ionization from aligned molecular ensembles
journal, February 2015


Molpro: a general-purpose quantum chemistry program package: Molpro
journal, July 2011

  • Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2
  • DOI: 10.1002/wcms.82

Wavelength dependent photoelectron circular dichroism of limonene studied by femtosecond multiphoton laser ionization and electron-ion coincidence imaging
journal, September 2016

  • Rafiee Fanood, Mohammad M.; Janssen, Maurice H. M.; Powis, Ivan
  • The Journal of Chemical Physics, Vol. 145, Issue 12
  • DOI: 10.1063/1.4963229

Variational treatment of electron–polyatomic-molecule scattering calculations using adaptive overset grids
journal, November 2017


Laser-induced molecular alignment probed by a double-pulse experiment
journal, October 1992

  • Normand, D.; Lompre, L. A.; Cornaggia, C.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 25, Issue 20
  • DOI: 10.1088/0953-4075/25/20/001

Phase, amplitude, and polarization shaping with a pulse shaper in a Mach-Zehnder interferometer
journal, January 2006

  • Plewicki, Mateusz; Weise, Fabian; Weber, Stefan M.
  • Applied Optics, Vol. 45, Issue 32
  • DOI: 10.1364/ao.45.008354

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. I. Propagation of single-active-electron wave packets in chiral pseudo-potentials
journal, June 2015

  • Artemyev, Anton N.; Müller, Anne D.; Hochstuhl, David
  • The Journal of Chemical Physics, Vol. 142, Issue 24
  • DOI: 10.1063/1.4922690

Photoexcitation circular dichroism in chiral molecules
journal, February 2018


Accurate amplitudes for electron-impact ionization
journal, July 2001


Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions
journal, May 1992

  • Kendall, Rick A.; Dunning, Thom H.; Harrison, Robert J.
  • The Journal of Chemical Physics, Vol. 96, Issue 9
  • DOI: 10.1063/1.462569

Generation and characterization of polarization-shaped femtosecond laser pulses
journal, June 2002


Multiphoton photoelectron circular dichroism of limonene with independent polarization state control of the bound-bound and bound-continuum transitions
journal, October 2018

  • Beaulieu, S.; Comby, A.; Descamps, D.
  • The Journal of Chemical Physics, Vol. 149, Issue 13
  • DOI: 10.1063/1.5042533

Asymmetric photoelectron angular distributions from interfering photoionization processes
journal, October 1992


Quantum coherent control of the photoelectron angular distribution in bichromatic-field ionization of atomic neon
journal, January 2018

  • Gryzlova, E. V.; Grum-Grzhimailo, A. N.; Staroselskaya, E. I.
  • Physical Review A, Vol. 97, Issue 1
  • DOI: 10.1103/physreva.97.013420

Universality of photoelectron circular dichroism in the photoionization of chiral molecules
journal, October 2016


Generation of polarization-shaped ultraviolet femtosecond pulses
journal, January 2008

  • Selle, Reimer; Nuernberger, Patrick; Langhojer, Florian
  • Optics Letters, Vol. 33, Issue 8
  • DOI: 10.1364/ol.33.000803

Detecting chirality in molecules by imaging photoelectron circular dichroism
journal, January 2014

  • Janssen, Maurice H. M.; Powis, Ivan
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 3
  • DOI: 10.1039/c3cp53741b

Attosecond coupled electron and nuclear dynamics in dissociative ionization of H2
journal, April 2018


Adaptive control of molecular alignment
journal, March 2006


Coherent interference of molecular electronic states in NO by two-color femtosecond laser pulses
journal, January 2019


Programmable common-path vector field synthesizer for femtosecond pulses
journal, January 2007


Mapping rotational coherences onto time-resolved photoelectron imaging observables
journal, June 2005

  • Suzuki, Yoshi-ichi; Seideman, Tamar
  • The Journal of Chemical Physics, Vol. 122, Issue 23
  • DOI: 10.1063/1.1926282

Circular dichroism in the angle-resolved C 1s photoemission spectra of gas-phase carvone enantiomers
journal, December 2005

  • Harding, Chris J.; Mikajlo, Elisabeth; Powis, Ivan
  • The Journal of Chemical Physics, Vol. 123, Issue 23
  • DOI: 10.1063/1.2136150

Theoretical description of circular dichroism in photoelectron angular distributions of randomly oriented chiral molecules after multi-photon photoionization
journal, January 2017

  • Goetz, R. E.; Isaev, T. A.; Nikoobakht, B.
  • The Journal of Chemical Physics, Vol. 146, Issue 2
  • DOI: 10.1063/1.4973456

Imaging photoelectron photoion coincidence spectroscopy with velocity focusing electron optics
journal, March 2009

  • Bodi, Andras; Johnson, Melanie; Gerber, Thomas
  • Review of Scientific Instruments, Vol. 80, Issue 3
  • DOI: 10.1063/1.3082016

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging–ion mass spectrometry
journal, June 2015

  • Fanood, Mohammad M. Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8511

Applications of polarization-shaped femtosecond laser pulses
journal, July 2016


Training Schrödinger’s cat: quantum optimal control: Strategic report on current status, visions and goals for research in Europe
journal, December 2015

  • Glaser, Steffen J.; Boscain, Ugo; Calarco, Tommaso
  • The European Physical Journal D, Vol. 69, Issue 12
  • DOI: 10.1140/epjd/e2015-60464-1

A new basis set method for quantum scattering calculations
journal, June 1987

  • Miller, William H.; Jansen op de Haar, Bernadette M. D. D.
  • The Journal of Chemical Physics, Vol. 86, Issue 11
  • DOI: 10.1063/1.452459

Photoelectron angular distribution in bichromatic atomic ionization
journal, September 2015

  • Grum-Grzhimailo, A. N.; Gryzlova, E. V.; Staroselskaya, E. I.
  • Journal of Physics: Conference Series, Vol. 635, Issue 1
  • DOI: 10.1088/1742-6596/635/1/012008

Koinzidenzmessung von Photoionen und Photoelektronen bei Methan
journal, January 1967

  • Brehm, Burkhard; von Puttkamer, Ewald
  • Zeitschrift für Naturforschung A, Vol. 22, Issue 1
  • DOI: 10.1515/zna-1967-0103

Enantiomeric Excess Sensitivity to Below One Percent by Using Femtosecond Photoelectron Circular Dichroism
journal, February 2016


Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection
journal, December 2013

  • Lehmann, C. Stefan; Ram, N. Bhargava; Powis, Ivan
  • The Journal of Chemical Physics, Vol. 139, Issue 23
  • DOI: 10.1063/1.4844295

Calculation of low‐energy elastic cross sections for electron‐CF 4 scattering
journal, May 1994

  • Gianturco, F. A.; Lucchese, R. R.; Sanna, N.
  • The Journal of Chemical Physics, Vol. 100, Issue 9
  • DOI: 10.1063/1.467237

Control of selectivity of chemical reaction via control of wave packet evolution
journal, November 1985

  • Tannor, David J.; Rice, Stuart A.
  • The Journal of Chemical Physics, Vol. 83, Issue 10, p. 5013-5018
  • DOI: 10.1063/1.449767

Photoelectron angular distributions in molecular above threshold ionization by two colour circularly polarized ultrashort UV laser pulses
journal, October 2013


Interfering one-photon and two-photon ionization by femtosecond VUV pulses in the region of an intermediate resonance
journal, June 2015

  • Grum-Grzhimailo, Alexei N.; Gryzlova, Elena V.; Staroselskaya, Ekaterina I.
  • Physical Review A, Vol. 91, Issue 6
  • DOI: 10.1103/physreva.91.063418

Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry
journal, October 2016

  • Comby, Antoine; Beaulieu, Samuel; Boggio-Pasqua, Martial
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 22
  • DOI: 10.1021/acs.jpclett.6b02065

Above-threshold ionization in neon produced by combining optical and bichromatic XUV femtosecond laser pulses
journal, January 2017

  • Douguet, Nicolas; Grum-Grzhimailo, Alexei N.; Bartschat, Klaus
  • Physical Review A, Vol. 95, Issue 1
  • DOI: 10.1103/physreva.95.013407

Photoelectron spectroscopic studies of polyatomic molecules. I. Theory
journal, July 1987


Determination of chiral asymmetries in the valence photoionization of camphor enantiomers by photoelectron imaging using tunable circularly polarized light
journal, September 2006

  • Nahon, Laurent; Garcia, Gustavo A.; Harding, Chris J.
  • The Journal of Chemical Physics, Vol. 125, Issue 11
  • DOI: 10.1063/1.2336432

Two-pathway coherent control of photoelectron angular distributions in molecular NO
journal, August 1995


Above-threshold ionisation with a two-colour laser field
journal, August 1990

  • Muller, H. G.; Bucksbaum, P. H.; Schumacher, D. W.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 23, Issue 16
  • DOI: 10.1088/0953-4075/23/16/018

Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet
journal, September 2012


Photoelectron circular dichroism of chiral molecules studied with a continuum-state-corrected strong-field approximation
journal, May 2014


Interference asymmetry of molecular frame photoelectron angular istributions in bichromatic UV ionization processes
journal, February 2016

  • Yuan, Kai-Jun; Bandrauk, André D.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 49, Issue 6
  • DOI: 10.1088/0953-4075/49/6/065601

Enantioselective femtosecond laser photoionization spectrometry of limonene using photoelectron circular dichroism
journal, January 2015

  • Rafiee Fanood, Mohammad M.; Janssen, Maurice H. M.; Powis, Ivan
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 14
  • DOI: 10.1039/c5cp00583c

Coherent control of photoelectron wavepacket angular interferograms
journal, September 2015

  • Hockett, P.; Wollenhaupt, M.; Baumert, T.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 21
  • DOI: 10.1088/0953-4075/48/21/214004

P HOTOELECTRON A NGULAR D ISTRIBUTIONS
journal, October 2003


A new technique for probing chirality via photoelectron circular dichroism
journal, September 2017


Time-resolved photoelectron angular distributions as a probe of intramolecular dynamics: Connecting the molecular frame and the laboratory frame
journal, July 2000

  • Underwood, Jonathan G.; Reid, Katharine L.
  • The Journal of Chemical Physics, Vol. 113, Issue 3
  • DOI: 10.1063/1.481918