DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy

Abstract

In this paper, we report on spectral intensity and group delay measurements of the highest-occupied molecular-orbital (HOMO) recombination dipole moment of $${\mathrm{N}}_{2}$$ in the molecular-frame using high harmonic spectroscopy. We take advantage of the long-wavelength $$1.3\text{ }\text{ }{\mu}\mathrm{m}$$ driving laser to isolate the HOMO in the near threshold region, 19–67 eV. Finally, the precision of our group delay measurements reveals previously unseen angle-resolved spectral features associated with autoionizing resonances, and allows quantitative comparison with cutting-edge correlated 8-channel photoionization dipole moment calculations.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1]
  1. The Ohio State Univ., Columbus, OH (United States). Dept. of Physics
  2. Alternative Energies and Atomic Energy Commission (CEA), Saclay (France). Interactions, Dynamics and Lasers Lab. (LIDYL)
  3. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Center for Scientific Research (CNRS) International Project of Scientific Cooperation (PICS) (France)
OSTI Identifier:
1461115
Alternate Identifier(s):
OSTI ID: 1341314
Grant/Contract Number:  
FG02-04ER15614; FG02-06ER15833; 5460
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 118; Journal Issue: 3; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; electronic structure of atoms & molecules; high-order harmonic generation

Citation Formats

Schoun, S. B., Camper, A., Salieres, P., Lucchese, R. R., Agostini, P., and DiMauro, L. F. Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy. United States: N. p., 2017. Web. doi:10.1103/PhysRevLett.118.033201.
Schoun, S. B., Camper, A., Salieres, P., Lucchese, R. R., Agostini, P., & DiMauro, L. F. Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy. United States. https://doi.org/10.1103/PhysRevLett.118.033201
Schoun, S. B., Camper, A., Salieres, P., Lucchese, R. R., Agostini, P., and DiMauro, L. F. Thu . "Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy". United States. https://doi.org/10.1103/PhysRevLett.118.033201. https://www.osti.gov/servlets/purl/1461115.
@article{osti_1461115,
title = {Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy},
author = {Schoun, S. B. and Camper, A. and Salieres, P. and Lucchese, R. R. and Agostini, P. and DiMauro, L. F.},
abstractNote = {In this paper, we report on spectral intensity and group delay measurements of the highest-occupied molecular-orbital (HOMO) recombination dipole moment of ${\mathrm{N}}_{2}$ in the molecular-frame using high harmonic spectroscopy. We take advantage of the long-wavelength $1.3\text{ }\text{ }{\mu}\mathrm{m}$ driving laser to isolate the HOMO in the near threshold region, 19–67 eV. Finally, the precision of our group delay measurements reveals previously unseen angle-resolved spectral features associated with autoionizing resonances, and allows quantitative comparison with cutting-edge correlated 8-channel photoionization dipole moment calculations.},
doi = {10.1103/PhysRevLett.118.033201},
journal = {Physical Review Letters},
number = 3,
volume = 118,
place = {United States},
year = {Thu Jan 19 00:00:00 EST 2017},
month = {Thu Jan 19 00:00:00 EST 2017}
}

Journal Article:

Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Shape‐resonant and many‐electron effects in the S 2 p photoionization of SF 6
journal, October 1988

  • Ferrett, T. A.; Lindle, D. W.; Heimann, P. A.
  • The Journal of Chemical Physics, Vol. 89, Issue 8
  • DOI: 10.1063/1.455666

Theoretical Fine Spectroscopy with SAC-CI Method: Outer- and Inner-Valence Ionization Spectra of CO and N2
journal, January 2005

  • Ehara, Masahiro; Ishida, Mayumi; Nakatsuji, Hiroshi
  • Collection of Czechoslovak Chemical Communications, Vol. 70, Issue 7
  • DOI: 10.1135/cccc20050881

High Harmonic Generation from Multiple Orbitals in N2
journal, November 2008


Spectrally resolved multi-channel contributions to the harmonic emission in N 2
journal, February 2012


Correlation states of ethylene
journal, April 1995

  • Desjardins, S. J.; Bawagan, A. D. O.; Liu, Z. F.
  • The Journal of Chemical Physics, Vol. 102, Issue 16
  • DOI: 10.1063/1.469354

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

Direct Measurement of the Angular Dependence of Ionization for N 2 , O 2 , and CO 2 in Intense Laser Fields
journal, June 2007


Interference in the Photo-Ionization of Molecules
journal, October 1966


Generation of Femtosecond Pulses of Synchrotron Radiation
journal, March 2000


Multiplet‐specific multichannel electron‐correlation effects in the photoionization of NO
journal, June 1996

  • Stratmann, R. E.; Zurales, Robert W.; Lucchese, Robert R.
  • The Journal of Chemical Physics, Vol. 104, Issue 22
  • DOI: 10.1063/1.471632

Above threshold ionization beyond the high harmonic cutoff
journal, March 1993


Colloquium : Aligning molecules with strong laser pulses
journal, April 2003


Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen
journal, January 1989

  • Dunning, Thom H.
  • The Journal of Chemical Physics, Vol. 90, Issue 2
  • DOI: 10.1063/1.456153

Alignment dependence of high harmonics contributed from HOMO and HOMO-1 orbitals of N 2 molecules
journal, October 2010

  • Lee, Gae Hwang; Kim, I. Jong; Park, Seung Beom
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 43, Issue 20
  • DOI: 10.1088/0953-4075/43/20/205602

Theoretical study of photoelectron angular distributions in single-photon ionization of aligned N 2 and CO 2
journal, March 2010


The inner valence photoionization of acetylene
journal, April 1999

  • Wells, M.; Lucchese, Robert R.
  • The Journal of Chemical Physics, Vol. 110, Issue 13
  • DOI: 10.1063/1.478540

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

Theory of high-order harmonic generation from molecules by intense laser pulses
journal, April 2008

  • Le, Anh-Thu; Picca, R. Della; Fainstein, P. D.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 41, Issue 8
  • DOI: 10.1088/0953-4075/41/8/081002

Fixed‐molecule photoelectron angular distributions
journal, August 1976

  • Dill, Dan
  • The Journal of Chemical Physics, Vol. 65, Issue 3
  • DOI: 10.1063/1.433187

Phase-resolved attosecond near-threshold photoionization of molecular nitrogen
journal, July 2009


Reconstruction of attosecond harmonic beating by interference of two-photon transitions
journal, June 2002


Inner valence satellite structure in high resolution X-ray excited photoelectron spectra of N 2 and CO
journal, August 1991


Spectral phase measurement of a Fano resonance using tunable attosecond pulses
journal, February 2016

  • Kotur, M.; Guénot, D.; Jiménez-Galán, Á
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10566

Polarization and ellipticity of high-order harmonics from aligned molecules generated by linearly polarized intense laser pulses
journal, August 2010


Tomographic imaging of molecular orbitals
journal, December 2004


Electron-correlation effects in the photoionization of N 2
journal, May 1995

  • Stratmann, R. E.; Bandarage, Gunadya; Lucchese, Robert R.
  • Physical Review A, Vol. 51, Issue 5
  • DOI: 10.1103/PhysRevA.51.3756

Introduction to attosecond delays in photoionization
journal, August 2012

  • Dahlström, J. M.; L’Huillier, A.; Maquet, A.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 18
  • DOI: 10.1088/0953-4075/45/18/183001

Phase distortions of attosecond pulses produced by resonance-enhanced high harmonic generation
journal, January 2013


Size-Dependent High-order Harmonic Generation in Rare-Gas Clusters
journal, December 2014


Analytic confirmation that the factorized formula for harmonic generation involves the exact photorecombination cross section
journal, April 2011


Shape-resonance effects mediated by channel interaction: Angular distributions of N 2 2 σ u photoelectrons
journal, March 1985


Extracting the polarizability anisotropy from the transient alignment of HBr
journal, August 2008

  • Pinkham, D.; Vogt, T.; Jones, R. R.
  • The Journal of Chemical Physics, Vol. 129, Issue 6
  • DOI: 10.1063/1.2968557

Direct Measurement of the Angular Dependence of the Single-Photon Ionization of Aligned N 2 and CO 2
journal, October 2008

  • Thomann, Isabell; Lock, Robynne; Sharma, Vandana
  • The Journal of Physical Chemistry A, Vol. 112, Issue 39
  • DOI: 10.1021/jp8023414

Transverse Electromagnetic Mode Conversion for High-Harmonic Self-Probing Spectroscopy
journal, February 2015


A graphical unitary group approach to study multiplet specific multichannel electron correlation effects in the photoionization of O 2
journal, June 1995

  • Stratmann, R. E.; Lucchese, Robert R.
  • The Journal of Chemical Physics, Vol. 102, Issue 21
  • DOI: 10.1063/1.468841

Magnetic field paralleliser for 2π electron-spectrometer and electron-image magnifier
journal, April 1983


Attosecond imaging of molecular electronic wavepackets
journal, January 2010

  • Haessler, S.; Caillat, J.; Boutu, W.
  • Nature Physics, Vol. 6, Issue 3
  • DOI: 10.1038/nphys1511

Photoelectron kinetic and angular distributions for the ionization of aligned molecules using a HHG source
journal, March 2012

  • Rouzée, Arnaud; Kelkensberg, Freek; Siu, Wing Kiu
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 7
  • DOI: 10.1088/0953-4075/45/7/074016

Spectral variation of fixed‐molecule photoelectron angular distributions
journal, October 1976

  • Dill, Dan; Siegel, Jon; Dehmer, J. L.
  • The Journal of Chemical Physics, Vol. 65, Issue 8
  • DOI: 10.1063/1.433486

Observation of a Train of Attosecond Pulses from High Harmonic Generation
journal, June 2001


Plasma perspective on strong field multiphoton ionization
journal, September 1993


Towards imaging of ultrafast molecular dynamics using FELs
journal, August 2013

  • Rouzée, A.; Johnsson, P.; Rading, L.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
  • DOI: 10.1088/0953-4075/46/16/164029

Molecular Spectra and Molecular Structure
book, January 1979


Photoelectron angular distribution studies of the outer valence states of N 2
journal, November 2012

  • Ilchen, Markus; Deinert, Sascha; Glaser, Leif
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 22
  • DOI: 10.1088/0953-4075/45/22/225102

Spectral phase measurement of a Fano resonance using tunable attosecond pulses
text, January 2016

  • Kotur, M.; Guénot, D.; Jiménez-Galán, Á
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/pubdb-2016-04867

Molecular Spectra and Molecular Structure
journal, November 1929

  • Garner, W. E.; Lennard-Jones, J. E.
  • Nature, Vol. 124, Issue 3133
  • DOI: 10.1038/124762b0

Molecular Spectra and Molecular Structure
journal, October 1929

  • Garner, W. E.; Lennard-Jones, J. E.
  • Nature, Vol. 124, Issue 3128
  • DOI: 10.1038/124584a0

Theory of high-order harmonic generation from molecules by intense laser pulses
text, January 2008


Quantitative Rescattering Theory for high-order harmonic generation from molecules
text, January 2009


Attosecond pulse shaping around a Cooper minimum
text, January 2013


Works referencing / citing this record:

Attosecond imaging of molecules using high harmonic spectroscopy
journal, January 2019


Probing the interplay between geometric and electronic-structure features via high-harmonic spectroscopy
journal, May 2019

  • Gorman, T. T.; Scarborough, T. D.; Abanador, P. M.
  • The Journal of Chemical Physics, Vol. 150, Issue 18
  • DOI: 10.1063/1.5086036

Resonantly-initiated quantum trajectories and their role in the generation of near-threshold harmonics
journal, February 2018

  • Camp, Seth; Beaulieu, Samuel; Schafer, Kenneth J.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 6
  • DOI: 10.1088/1361-6455/aaac12