Spectral dependence of photoemission in multiphoton ionization of NO2 by femtosecond pulses in the 375–430 nm range

Poullain, S. Marggi; Cireasa, R.; Cornaggia, C.; Simon, M.; Marin, T.; Guillemin, R.; Houver, J. C.; Lucchese, R. R.; Dowek, D.

doi:10.1039/c7cp02057k

Title: Spectral dependence of photoemission in multiphoton ionization of NO₂ by femtosecond pulses in the 375–430 nm range

Abstract

In this paper, we investigate the multiphoton ionization of NO₂ using tunable (430–375 nm) femtosecond pulses and photoelectron–photoion coincidence momentum spectroscopy. In order to understand the complex electronic and nuclear photodynamics at play following absorption of three to five photons, we also report extended photoionization calculations using correlated targets and coupled channels. Exploring the multiphoton dissociative ionization (MPDI) and multiphoton ionization (MPI) processes over such a broad energy range enables us to lend further support to our work carried out around 400 nm of a femtosecond laser [S. Marggi Poullain et al., J. Phys. B: At., Mol. Opt. Phys., 2014, 47, 124024]. Two excitation energy regions are identified and discussed in terms of the proposed reaction pathways, highlighting the significant role of Rydberg states, such as the [R*(6a₁)^-1, 3pσ] Rydberg state, in the NO₂ multiphoton excitation and photoionization. These new results support our previous assumption that different bent and linear geometries of the NO₂⁺(X¹Σ_g) ionic state contribute to the MPDI and MPI, consistent with the reported calculations which reveal an important vibronic coupling characterizing the photoemission. Finally, remarkably, the strong anisotropy of the recoil frame photoelectron angular distribution (RFPAD) previously observed at 400 nm appears as a fingerprint across themore » whole explored photon energy range.« less

Authors:

^[1]; Cireasa, R. ^[2]; Cornaggia, C. ^[3]; Simon, M. ^[4]; Marin, T. ^[4]; Guillemin, R. ^[4]; Houver, J. C. ^[2]; Lucchese, R. R. ^[5]; Dowek, D. ^[2]

Univ. of Paris-Sud, Orsay (France). Inst. of Molecular Sciences of Orsay (ISMO); Complutense Univ. of Madrid (Spain). Dept. of Physical Chemistry. Faculty of Chemical Sciences
Univ. of Paris-Sud, Orsay (France). Inst. of Molecular Sciences of Orsay (ISMO)
Alternative Energies and Atomic Energy Commission (CEA), Saclay (France). Interactions, Dynamics and Lasers Lab. (LIDYL)
National Centre for Scientific Research (CNRS) and Pierre and Marie Curie Univ, Paris (France). Lab. of Physical Chemistry - Matter and Radiation (LCPMR)
Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry

Publication Date:: Thu Jul 27 00:00:00 EDT 2017

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Robert A. Welch Foundation (United States); National Research Agency (ANR) (France)

OSTI Identifier:: 1461114

Grant/Contract Number:: SC0012198; A-1020; ANR-10-LABX-0039-PALM

Resource Type:: Accepted Manuscript

Journal Name:: Physical Chemistry Chemical Physics. PCCP

Additional Journal Information:: Journal Volume: 19; Journal Issue: 33; Journal ID: ISSN 1463-9076

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Poullain, S. Marggi, Cireasa, R., Cornaggia, C., Simon, M., Marin, T., Guillemin, R., Houver, J. C., Lucchese, R. R., and Dowek, D. Spectral dependence of photoemission in multiphoton ionization of NO2 by femtosecond pulses in the 375–430 nm range.  United States: N. p., 2017. 
Web.  doi:10.1039/c7cp02057k.

Copy to clipboard


                    Poullain, S. Marggi, Cireasa, R., Cornaggia, C., Simon, M., Marin, T., Guillemin, R., Houver, J. C., Lucchese, R. R., & Dowek, D. Spectral dependence of photoemission in multiphoton ionization of NO2 by femtosecond pulses in the 375–430 nm range.  United States.  https://doi.org/10.1039/c7cp02057k

Copy to clipboard


                    Poullain, S. Marggi, Cireasa, R., Cornaggia, C., Simon, M., Marin, T., Guillemin, R., Houver, J. C., Lucchese, R. R., and Dowek, D. Thu .  
"Spectral dependence of photoemission in multiphoton ionization of NO2 by femtosecond pulses in the 375–430 nm range".  United States.  https://doi.org/10.1039/c7cp02057k.  https://www.osti.gov/servlets/purl/1461114.

Copy to clipboard


                    
@article{osti_1461114,

  title        = {Spectral dependence of photoemission in multiphoton ionization of NO2 by femtosecond pulses in the 375–430 nm range},

  author       = {Poullain, S. Marggi and Cireasa, R. and Cornaggia, C. and Simon, M. and Marin, T. and Guillemin, R. and Houver, J. C. and Lucchese, R. R. and Dowek, D.},

  abstractNote = {In this paper, we investigate the multiphoton ionization of NO2 using tunable (430–375 nm) femtosecond pulses and photoelectron–photoion coincidence momentum spectroscopy. In order to understand the complex electronic and nuclear photodynamics at play following absorption of three to five photons, we also report extended photoionization calculations using correlated targets and coupled channels. Exploring the multiphoton dissociative ionization (MPDI) and multiphoton ionization (MPI) processes over such a broad energy range enables us to lend further support to our work carried out around 400 nm of a femtosecond laser [S. Marggi Poullain et al., J. Phys. B: At., Mol. Opt. Phys., 2014, 47, 124024]. Two excitation energy regions are identified and discussed in terms of the proposed reaction pathways, highlighting the significant role of Rydberg states, such as the [R*(6a1)-1, 3pσ] Rydberg state, in the NO2 multiphoton excitation and photoionization. These new results support our previous assumption that different bent and linear geometries of the NO2+(X1Σg) ionic state contribute to the MPDI and MPI, consistent with the reported calculations which reveal an important vibronic coupling characterizing the photoemission. Finally, remarkably, the strong anisotropy of the recoil frame photoelectron angular distribution (RFPAD) previously observed at 400 nm appears as a fingerprint across the whole explored photon energy range.},

  doi          = {10.1039/c7cp02057k},

  journal      = {Physical Chemistry Chemical Physics. PCCP},

  number       = 33,

  volume       = 19,

  place        = {United States},

  year         = {Thu Jul 27 00:00:00 EDT 2017},

  month        = {Thu Jul 27 00:00:00 EDT 2017}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1039/c7cp02057k

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 4 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Self-referenced spectral interferometry
journal, February 2010

Oksenhendler, T.; Coudreau, S.; Forget, N.
Applied Physics B, Vol. 99, Issue 1-2
DOI: 10.1007/s00340-010-3916-y

Femtosecond fluorescence depletion spectroscopy of NO2 multiphoton dissociation dynamics
journal, October 1999

López-Martens, R. B.; Schmidt, T. W.; Roberts, G.
The Journal of Chemical Physics, Vol. 111, Issue 16
DOI: 10.1063/1.480046

A Theoretical Study on the Electronic States and O-Loss Photodissociation of the NO ₂ ⁺ Ion
journal, February 2009

Chang, Hai-Bo; Huang, Ming-Bao
ChemPhysChem, Vol. 10, Issue 3
DOI: 10.1002/cphc.200800626

Some remarks on the photodynamics of NO2
journal, January 2010

Wilkinson, Iain; J. Whitaker, Benjamin
Annual Reports Section "C" (Physical Chemistry), Vol. 106
DOI: 10.1039/b924653n

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

Excitation of the symmetry forbidden bending mode in molecular photoionization
journal, January 2001

Miller, J. Scott; Poliakoff, E. D.; Miller, Thomas F.
The Journal of Chemical Physics, Vol. 114, Issue 10
DOI: 10.1063/1.1349090

Femtosecond time-resolved photoelectron–photoion coincidence imaging studies of dissociation dynamics
journal, July 1999

Davies, J. A.; LeClaire, J. E.; Continetti, R. E.
The Journal of Chemical Physics, Vol. 111, Issue 1
DOI: 10.1063/1.479248

The role of multichannel effects in the photoionization of the NO ₂ molecule: an ab initio R -matrix study
journal, November 2015

Brambila, Danilo S.; Harvey, Alex G.; Mašín, Zdeněk
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 24
DOI: 10.1088/0953-4075/48/24/245101

Vector Correlations in Dissociative Photoionization of Diatomic Molecules in the VUV Range: Strong Anisotropies in Electron Emission from Spatially Oriented NO Molecules
journal, June 2000

Lafosse, A.; Lebech, M.; Brenot, J. C.
Physical Review Letters, Vol. 84, Issue 26
DOI: 10.1103/PhysRevLett.84.5987

Rydberg Fingerprint Spectroscopy: A New Spectroscopic Tool with Local and Global Structural Sensitivity
journal, June 2005

Gosselin, Jaimie L.; Weber, Peter M.
The Journal of Physical Chemistry A, Vol. 109, Issue 22
DOI: 10.1021/jp0503866

Ion Pair Formation in Multiphoton Excitation of NO ₂ Using Linearly and Circularly Polarized Femtosecond Light Pulses: Kinetic Energy Distribution and Fragment Recoil Anisotropy ^†
journal, September 2010

Elkharrat, C.; Picard, Y. J.; Billaud, P.
The Journal of Physical Chemistry A, Vol. 114, Issue 36
DOI: 10.1021/jp103672h

Recoil frame photoemission in multiphoton ionization of small polyatomic molecules: photodynamics of NO ₂ probed by 400 nm fs pulses
journal, June 2014

Marggi Poullain, S.; Elkharrat, C.; Li, W. B.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 47, Issue 12
DOI: 10.1088/0953-4075/47/12/124024

Ion–electron velocity vector correlations in dissociative photoionization of simple molecules using electrostatic lenses
journal, April 2002

Lebech, M.; Houver, J. C.; Dowek, D.
Review of Scientific Instruments, Vol. 73, Issue 4
DOI: 10.1063/1.1458063

Femtosecond Time-Resolved Photoelectron Angular Distributions Probed during Photodissociation of ${NO}_{2}$
journal, June 2000

Davies, J. A.; Continetti, R. E.; Chandler, D. W.
Physical Review Letters, Vol. 84, Issue 26
DOI: 10.1103/PhysRevLett.84.5983

Femtosecond time-resolved photoelectron-photoion coincidence imaging of multiphoton multichannel photodynamics in NO2
journal, May 2008

Vredenborg, Arno; Roeterdink, Willem G.; Janssen, Maurice H. M.
The Journal of Chemical Physics, Vol. 128, Issue 20
DOI: 10.1063/1.2924134

Double momentum spectrometer for ion-electron vector correlations in dissociative photoionization
journal, October 2013

Bomme, C.; Guillemin, R.; Marin, T.
Review of Scientific Instruments, Vol. 84, Issue 10
DOI: 10.1063/1.4824194

Imaging fast relaxation dynamics of NO ₂
journal, October 2009

Cireasa, Raluca; Hamard, Jean-Benoît; Maury, Cécile
Physica Scripta, Vol. 80, Issue 4
DOI: 10.1088/0031-8949/80/04/048106

The role of Rydberg states in photoionization of NO ₂ and (NO ⁺ , O ⁻ ) ion pair formation induced by one VUV photon
journal, July 2013

Marggi Poullain, S.; Veyrinas, K.; Billaud, P.
The Journal of Chemical Physics, Vol. 139, Issue 4
DOI: 10.1063/1.4811713

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

Molecular frame and recoil frame photoelectron angular distributions from dissociative photoionization of NO2
journal, February 2007

Toffoli, Daniele; Lucchese, Robert R.; Lebech, M.
The Journal of Chemical Physics, Vol. 126, Issue 5
DOI: 10.1063/1.2432124

What does the term "Vibronic Coupling" Mean?
journal, March 1977

Azumi, Tohru; Matsuzaki, Kazuo
Photochemistry and Photobiology, Vol. 25, Issue 3
DOI: 10.1111/j.1751-1097.1977.tb06918.x

Vibration–rotation interaction constants and the cubic potential function of the NO ₂ molecule in the small-amplitude approximation
journal, December 1984

Morino, Yonezo; Tanimoto, Mitsutoshi
Canadian Journal of Physics, Vol. 62, Issue 12
DOI: 10.1139/p84-178

Works referencing / citing this record:

High resolution vibronic state-specific dissociation of NO ₂ ⁺ in the 10.0–15.5 eV energy range by synchrotron double imaging photoelectron photoion coincidence
journal, January 2020

Tang, Xiaofeng; Garcia, Gustavo A.; Nahon, Laurent
Physical Chemistry Chemical Physics, Vol. 22, Issue 4
DOI: 10.1039/c9cp05847h

Similar Records in DOE PAGES and OSTI.GOV collections:

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection

Journal Article Lehmann, C. Stefan ; Ram, N. Bhargava ; Janssen, Maurice H. M., ; ... - Journal of Chemical Physics

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flightmore »« less
https://doi.org/10.1063/1.4844295
Ultrafast Curve Crossing Dynamics through Conical Intersections in Methylated Cyclopentadienes

Journal Article Rudakov, Fedor M - Journal of Physical Chemistry A

We explored the curve crossing dynamics of 1,2,3,4-tetramethyl-cyclopentadiene (TMCPD) and 1,2,3,4,5-pentamethyl-cyclopentadiene (PMCPD) upon {pi} {yields} {pi}* excitation to the 1B{sub 2} state using time-resolved, resonance-enhanced multiphoton ionization mass and photoelectron spectroscopy. Upon excitation with a femtosecond laser pulse at 267 nm, the energy relaxation pathway is observed by a time-delayed probe pulse at 400 nm, which ionizes the molecule through Rydberg states that reveal the momentary state of the molecule in the photoelectron spectra. We observe that the initially populated 1B{sub 2} state decays to the 2A{sub 1} surface in 135 fs in TMCPD and 183 fs in PMCPD, followedmore »« less
https://doi.org/10.1021/jp910786s
Effects of molecular rotation after ionization and prior to fragmentation on observed recoil-frame photoelectron angular distributions in the dissociative photoionization of nonlinear molecules

Journal Article Lopez-Dominguez, Jesus A. ; Lucchese, Robert R. - Physical Review A

Experimental angle-resolved photoelectron-photoion coincidence experiments measure photoelectron angular distributions (PADs) in dissociative photoionization (DPI) in the reference frame provided by the momenta of the emitted heavy fragments. By extension of the nomenclature used with DPI of diatomic molecules, we refer to such a PAD as a recoil-frame PAD (RFPAD). When the dissociation is fast compared to molecular rotational and bending motions, the emission directions of the heavy fragments can be used to determine the orientation of the bonds that are broken in the DPI at the time of the ionization, which is known as the axial-recoil approximation (ARA). When the ARA is valid, the RFPADs correspond to molecular-frame photoelectron angular distributions (MFPADs) when the momenta of a sufficient number of the heavy fragments are determined. When only two fragments are formed, the experiment cannot measure the orientation of the fragments about the recoil axes so that the resulting measured PAD is an azimuthally averaged RFPAD (AA-RFPAD). In this paper we consider how the breakdown of the ARA due to rotation will modify the observed RFPADs for DPI processes in nonlinear molecules for ionization by light of arbitrary polarization. This model is applied to the core Cmore »« less
https://doi.org/10.1103/PhysRevA.93.033421

Full Text Available
Photoionization and photoelectron spectroscopy of molecular Rydberg states

Miscellaneous Miller, P J

Spectroscopic investigations of molecular Rydberg states have been carried out using both one- and multi-photon laser techniques. Third-harmonic generation of tunable vacuum ultraviolet (VUV) radiation has been employed to obtain high resolution one-photon ionization spectra of NO and NH{sub 3}. The NO results have yielded autoionization linewidths that can be compared to multichannel quantum defect theory calculations. In NH{sub 3}, autoionizing Rydberg states have been seen converging to the v{sub 2}{sup +} = 3 and 5 levels of the ion. Photoelectron spectroscopy of these levels confirms a propensity for {Delta}v = {minus}1 vibrational autoionization. In another application of coherent VUVmore »« less
Dynamics of the H/sub 2//sup +//H/sub 2/ ion-molecule reaction and multiphoton ionization photoelectron spectroscopy of the H/sub 2/S molecule

Thesis/Dissertation Cole, S K

Charge exchange and collision induced dissociation reactions of the H/sub 2//sup +//H/sub 2/ system were measured at the reactant ion vibrational levels 0 to 10 and collision energies 4, 8, and 16 eV in the center of mass. The photoelectron photoion coincidence technique was used for the preparation of the state selected reactant ions. Cross sections for the charge exchange reaction were found to vary slowly with internal excitation of the reactant ion and also with collision energy. In contrast, cross sections for the collision induced dissociation reaction were found to depend strongly upon the reactant ion internal energy andmore »« less

Similar Records

Title: Spectral dependence of photoemission in multiphoton ionization of NO2 by femtosecond pulses in the 375–430 nm range

Abstract

Citation Formats

Self-referenced spectral interferometry journal, February 2010

Femtosecond fluorescence depletion spectroscopy of NO2 multiphoton dissociation dynamics journal, October 1999

A Theoretical Study on the Electronic States and O-Loss Photodissociation of the NO 2 + Ion journal, February 2009

Some remarks on the photodynamics of NO2 journal, January 2010

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

Excitation of the symmetry forbidden bending mode in molecular photoionization journal, January 2001

Femtosecond time-resolved photoelectron–photoion coincidence imaging studies of dissociation dynamics journal, July 1999

The role of multichannel effects in the photoionization of the NO 2 molecule: an ab initio R -matrix study journal, November 2015

Vector Correlations in Dissociative Photoionization of Diatomic Molecules in the VUV Range: Strong Anisotropies in Electron Emission from Spatially Oriented NO Molecules journal, June 2000

Rydberg Fingerprint Spectroscopy: A New Spectroscopic Tool with Local and Global Structural Sensitivity journal, June 2005

Ion Pair Formation in Multiphoton Excitation of NO 2 Using Linearly and Circularly Polarized Femtosecond Light Pulses: Kinetic Energy Distribution and Fragment Recoil Anisotropy † journal, September 2010

Recoil frame photoemission in multiphoton ionization of small polyatomic molecules: photodynamics of NO 2 probed by 400 nm fs pulses journal, June 2014

Ion–electron velocity vector correlations in dissociative photoionization of simple molecules using electrostatic lenses journal, April 2002

Femtosecond Time-Resolved Photoelectron Angular Distributions Probed during Photodissociation of NO 2 journal, June 2000

Femtosecond time-resolved photoelectron-photoion coincidence imaging of multiphoton multichannel photodynamics in NO2 journal, May 2008

Double momentum spectrometer for ion-electron vector correlations in dissociative photoionization journal, October 2013

Imaging fast relaxation dynamics of NO 2 journal, October 2009

The role of Rydberg states in photoionization of NO 2 and (NO + , O − ) ion pair formation induced by one VUV photon journal, July 2013

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

Molecular frame and recoil frame photoelectron angular distributions from dissociative photoionization of NO2 journal, February 2007

What does the term "Vibronic Coupling" Mean? journal, March 1977

Vibration–rotation interaction constants and the cubic potential function of the NO 2 molecule in the small-amplitude approximation journal, December 1984

High resolution vibronic state-specific dissociation of NO 2 + in the 10.0–15.5 eV energy range by synchrotron double imaging photoelectron photoion coincidence journal, January 2020

Title: Spectral dependence of photoemission in multiphoton ionization of NO₂ by femtosecond pulses in the 375–430 nm range

Self-referenced spectral interferometry
journal, February 2010

Femtosecond fluorescence depletion spectroscopy of NO2 multiphoton dissociation dynamics
journal, October 1999

A Theoretical Study on the Electronic States and O-Loss Photodissociation of the NO ₂ ⁺ Ion
journal, February 2009

Some remarks on the photodynamics of NO2
journal, January 2010

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

Excitation of the symmetry forbidden bending mode in molecular photoionization
journal, January 2001

Femtosecond time-resolved photoelectron–photoion coincidence imaging studies of dissociation dynamics
journal, July 1999

The role of multichannel effects in the photoionization of the NO ₂ molecule: an ab initio R -matrix study
journal, November 2015

Vector Correlations in Dissociative Photoionization of Diatomic Molecules in the VUV Range: Strong Anisotropies in Electron Emission from Spatially Oriented NO Molecules
journal, June 2000

Rydberg Fingerprint Spectroscopy: A New Spectroscopic Tool with Local and Global Structural Sensitivity
journal, June 2005

Ion Pair Formation in Multiphoton Excitation of NO ₂ Using Linearly and Circularly Polarized Femtosecond Light Pulses: Kinetic Energy Distribution and Fragment Recoil Anisotropy ^†
journal, September 2010

Recoil frame photoemission in multiphoton ionization of small polyatomic molecules: photodynamics of NO ₂ probed by 400 nm fs pulses
journal, June 2014

Ion–electron velocity vector correlations in dissociative photoionization of simple molecules using electrostatic lenses
journal, April 2002

Femtosecond Time-Resolved Photoelectron Angular Distributions Probed during Photodissociation of ${NO}_{2}$
journal, June 2000

Femtosecond time-resolved photoelectron-photoion coincidence imaging of multiphoton multichannel photodynamics in NO2
journal, May 2008

Double momentum spectrometer for ion-electron vector correlations in dissociative photoionization
journal, October 2013

Imaging fast relaxation dynamics of NO ₂
journal, October 2009

The role of Rydberg states in photoionization of NO ₂ and (NO ⁺ , O ⁻ ) ion pair formation induced by one VUV photon
journal, July 2013

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

Molecular frame and recoil frame photoelectron angular distributions from dissociative photoionization of NO2
journal, February 2007

What does the term "Vibronic Coupling" Mean?
journal, March 1977

Vibration–rotation interaction constants and the cubic potential function of the NO ₂ molecule in the small-amplitude approximation
journal, December 1984

High resolution vibronic state-specific dissociation of NO ₂ ⁺ in the 10.0–15.5 eV energy range by synchrotron double imaging photoelectron photoion coincidence
journal, January 2020