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Role of dipole-forbidden autoionizing resonances in nonresonant one-color two-photon single ionization of N2

Journal Article · · Physical Review A
 [1];  [2];  [2];  [2];  [3];  [2];  [2]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Davis, CA (United States)
+ Show Author Affiliations
We present an experimental and theoretical energy- and angle-resolved study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral N$$_2$$ molecules. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from one-color two-photon ionization in coincidence. Photoionization of N$$_2$$ populates the X $$^2\Sigma^+_g$$, A $$^2\Pi_u$$, and B $$^2\Sigma^+_u$$ ionic states of N$$_2^+$$, where the photoelectron angular distributions associated with the X $$^2\Sigma^+_g$$ and A $$^2\Pi_u$$ states both vary with changes in photoelectron kinetic energy of only a few hundred meV. We attribute the rapid evolution in the photoelectron angular distributions to the excitation and decay of dipole-forbidden autoionizing resonances that belong to series of different symmetries, all of which are members of the Hopfield series, and compete with the direct two-photon single ionization.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES), Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1670144
Journal Information:
Physical Review A, Journal Name: Physical Review A Journal Issue: 6 Vol. 102; ISSN 2469-9926
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (50)

Molpro: a general-purpose quantum chemistry program package: Molpro
  • Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2 https://doi.org/10.1002/wcms.82
journal July 2011
The rotational structure of three-photon resonances of polyatomic molecules journal February 1984
Absolute optical oscillator strengths for discrete and continuum photoabsorption of molecular nitrogen (11–200 eV) journal February 1993
Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics journal June 2000
Multicoincidence studies of photo and Auger electrons from fixed-in-space molecules using the COLTRIMS technique journal December 2004
High-resolution threshold photoelectron and photoion spectroscopy of molecular nitrogen in the 15.0–52.7 eV photon energy range journal August 2014
Electron Correlation in the Ionization Continuum of Molecules: Photoionization of N 2 in the Vicinity of the Hopfield Series of Autoionizing States journal February 2018
Electron localization following attosecond molecular photoionization journal June 2010
Vibrational branching ratios in the photoelectron spectra of N2 and CO: interference and diffraction effects journal January 2012
Recoil anisotropy following multiphoton dissociation via near-resonant intermediate states journal May 2005
Vibrationally resolved photoionization of N 2 near threshold journal March 2012
Vibronic intensities and rotational line strength factors for the three‐photon absorption spectrum of ammonia journal July 1981
The theory of double‐beam three‐photon absorption journal September 1982
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions journal May 1992
Rotational structure in the Hopfield series of N 2 journal March 1993
A graphical unitary group approach to study multiplet specific multichannel electron correlation effects in the photoionization of O 2 journal June 1995
Multiplet‐specific multichannel electron‐correlation effects in the photoionization of NO journal June 1996
Time resolved 3D momentum imaging of ultrafast dynamics by coherent VUV-XUV radiation journal June 2016
Refractive index of alkaline earth halides and its wavelength and temperature derivatives journal January 1980
Distinguishing resonance symmetries with energy-resolved photoion angular distributions from ion-pair formation in O 2 following two-photon absorption of a 9.3 eV femtosecond pulse journal July 2020
Two-photon absorption by rotating diatomic molecules journal April 1976
Ab initio approach to the multichannel quantum defect calculation of the electronic autoionisation in the Hopfield series of N 2 journal December 1983
Recoil-ion and electron momentum spectroscopy: reaction-microscopes journal August 2003
Universal Gaussian basis sets for an optimum representation of Rydberg and continuum wavefunctions journal July 1989
Molecular-frame photoelectron and electron-frame photoion angular distributions and their interrelation journal January 2007
Vibrationally resolved photoelectron angular distributions from randomly oriented and fixed-in-space N 2 and CO molecules journal September 2012
Photoelectron angular distribution studies of the outer valence states of N 2 journal November 2012
Effects of Configuration Interaction on Intensities and Phase Shifts journal December 1961
Absorption and Emission Spectra in the Region λ 600 − 1100 journal May 1930
Angle-resolved nonresonant two-photon single ionization of argon using 9.3-eV photons produced via high-order harmonic generation journal June 2020
Partial photoionization cross sections of N 2 and CO using synchrotron radiation journal June 1977
Studies of differential and total photoionization cross sections of molecular nitrogen journal May 1982
Channel coupling and shape resonance effects in the photoelectron angular distributions of the 3 σ g − 1 and 2 σ u − 1 channels of N 2 journal February 1986
Vibrationally resolved cross sections and asymmetry parameters for the photoionization of N 2 with coupling between the (3 σ g ) − 1 and the (2 σ u ) − 1 channels journal January 1988
Comparison of the random-phase approximation with the multichannel frozen-core Hartree-Fock approximation for the photoionization of N 2 journal July 1991
Electron-correlation effects in the photoionization of N 2 journal May 1995
Attosecond Time-Resolved Autoionization of Argon journal October 2010
Direct Imaging of Transient Fano Resonances in N 2 Using Time-, Energy-, and Angular-Resolved Photoelectron Spectroscopy journal April 2016
Triply-Differential Photoelectron Studies of Molecular Autoionization Profiles: The 710-730 Å Region of the N 2 Spectrum journal January 1981
Pulse Compression of a High-Order Harmonic by Compensating the Atomic Dipole Phase journal September 1999
Measurement of the Intensity-Dependent Atomic Dipole Phase of a High Harmonic by Frequency-Resolved Optical Gating journal April 2002
Multiple hit readout of a microchannel plate detector with a three-layer delay-line anode journal October 2002
Reconstruction of the time-dependent electronic wave packet arising from molecular autoionization journal August 2018
Single Photon-Induced Symmetry Breaking of H2 Dissociation journal February 2007
Observing the ultrafast buildup of a Fano resonance in the time domain journal November 2016
RYDBERG ABSORPTION SERIES OF N 2 journal November 1962
The lowest valence and Rydberg states in the dipole-allowed absorption spectrum of nitrogen. A survey of their interactions journal March 1969
Separation of high order harmonics with fluoride windows journal January 2009
VUV and XUV reflectance of optically coated mirrors for selection of high harmonics journal January 2016

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
Autoionization & Auger processes
Configuration interaction
Femtosecond laser spectroscopy
Molecules
Nonlinear optics
Photoemission
Photoionization
Single- and few-photon ionization & excitation