Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy

Chatterley, Adam S.; Lackner, Florian; Neumark, Daniel M.; Leone, Stephen R.; Gessner, Oliver

doi:10.1039/c6cp02598f

Title: Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy

Abstract

Using femtosecond time-resolved extreme ultraviolet absorption spectroscopy, the dissociation dynamics of the haloalkane 1,2-dibromoethane (DBE) have been explored following strong field ionization by femtosecond near infrared pulses at intensities between 7.5 × 10¹³ and 2.2 × 10¹⁴ W cm^-2. The major elimination products are bromine atoms in charge states of 0, +1, and +2. The charge state distribution is strongly dependent on the incident NIR intensity. While the yield of neutral fragments is essentially constant for all measurements, charged fragment yields grow rapidly with increasing NIR intensities with the most pronounced effect observed for Br⁺⁺. However, the appearance times of all bromine fragments are independent of the incident field strength; these are found to be 320 fs, 70 fs, and 30 fs for Br˙, Br⁺, and Br⁺⁺, respectively. Transient molecular ion features assigned to DBE⁺ and DBE⁺⁺ are observed, with dynamics linked to the production of Br⁺ products. Neutral Br˙ atoms are produced on a timescale consistent with dissociation of DBE⁺ ions on a shallow potential energy surface. The appearance of Br⁺ ions by dissociative ionization is also seen, as evidenced by the simultaneous decay of a DBE⁺ ionic species. Dicationic Br⁺⁺ products emerge within the instrument response time, presumablymore »« less

Authors:

Chatterley, Adam S. ^[1]; Lackner, Florian ^[1]; Neumark, Daniel M. ^[1]; Leone, Stephen R. ^[2]; Gessner, Oliver ^[3]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Dept. of Physics
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Chemical Sciences Division

Publication Date:: Wed May 11 00:00:00 EDT 2016

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Austrian Science Fund (FWF)

OSTI Identifier:: 1439187

Grant/Contract Number:: AC02-05CH11231; J 3580-N20

Resource Type:: Accepted Manuscript

Journal Name:: Physical Chemistry Chemical Physics. PCCP

Additional Journal Information:: Journal Volume: 18; Journal Issue: 21; Related Information: © 2016 the Owner Societies.; Journal ID: ISSN 1463-9076

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats


                    Chatterley, Adam S., Lackner, Florian, Neumark, Daniel M., Leone, Stephen R., and Gessner, Oliver. Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy.  United States: N. p., 2016. 
Web.  doi:10.1039/c6cp02598f.

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                    Chatterley, Adam S., Lackner, Florian, Neumark, Daniel M., Leone, Stephen R., & Gessner, Oliver. Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy.  United States.  https://doi.org/10.1039/c6cp02598f

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                    Chatterley, Adam S., Lackner, Florian, Neumark, Daniel M., Leone, Stephen R., and Gessner, Oliver. Wed .  
"Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy".  United States.  https://doi.org/10.1039/c6cp02598f.  https://www.osti.gov/servlets/purl/1439187.

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@article{osti_1439187,

  title        = {Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy},

  author       = {Chatterley, Adam S. and Lackner, Florian and Neumark, Daniel M. and Leone, Stephen R. and Gessner, Oliver},

  abstractNote = {Using femtosecond time-resolved extreme ultraviolet absorption spectroscopy, the dissociation dynamics of the haloalkane 1,2-dibromoethane (DBE) have been explored following strong field ionization by femtosecond near infrared pulses at intensities between 7.5 × 1013 and 2.2 × 1014 W cm-2. The major elimination products are bromine atoms in charge states of 0, +1, and +2. The charge state distribution is strongly dependent on the incident NIR intensity. While the yield of neutral fragments is essentially constant for all measurements, charged fragment yields grow rapidly with increasing NIR intensities with the most pronounced effect observed for Br++. However, the appearance times of all bromine fragments are independent of the incident field strength; these are found to be 320 fs, 70 fs, and 30 fs for Br˙, Br+, and Br++, respectively. Transient molecular ion features assigned to DBE+ and DBE++ are observed, with dynamics linked to the production of Br+ products. Neutral Br˙ atoms are produced on a timescale consistent with dissociation of DBE+ ions on a shallow potential energy surface. The appearance of Br+ ions by dissociative ionization is also seen, as evidenced by the simultaneous decay of a DBE+ ionic species. Dicationic Br++ products emerge within the instrument response time, presumably from Coulomb explosion of triply charged DBE.},

  doi          = {10.1039/c6cp02598f},

  journal      = {Physical Chemistry Chemical Physics. PCCP},

  number       = 21,

  volume       = 18,

  place        = {United States},

  year         = {Wed May 11 00:00:00 EDT 2016},

  month        = {Wed May 11 00:00:00 EDT 2016}

}

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Title: Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy

Abstract

Citation Formats

Photoexcitation, Ionization, and Dissociation of Molecules Using Intense Near-Infrared Radiation of Femtosecond Duration journal, August 1999

Concerted elimination of CH2I2 and CH2ICl under intense femtosecond laser excitation journal, January 2004

Excitation and ionization of the monohaloethylenes (C2H3X, X = F, Cl, Br, I). I. Inner-shell excitation by electron energy loss spectroscopy journal, April 1989

Ionization and dissociation dynamics of vinyl bromide probed by femtosecond extreme ultraviolet transient absorption spectroscopy journal, February 2014

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

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Theory of high-harmonic generation by low-frequency laser fields journal, March 1994

Two-step Coulomb explosions of diatoms in intense laser fields journal, December 1995

Ab initio study of methyl-bromide photodissociation in the Ã band journal, June 2009

Carbenium ion stabilities in the gas phase and solution. An ion cyclotron resonance study of bromide transfer reactions involving alkali ions, alkyl carbenium ions, acyl cations, and cyclic halonium ions journal, August 1977

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Ab initio investigation of Br-3 d core-excited states in HBr and HBr + toward XUV probing of photochemical dynamics journal, January 2019

Probing ultrafast C–Br bond fission in the UV photochemistry of bromoform with core-to-valence transient absorption spectroscopy journal, September 2019

Symphony on strong field approximation text, January 2019

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

The ultrafast X-ray spectroscopic revolution in chemical dynamics journal, May 2018

Three-dimensional momentum imaging of dissociation in flight of metastable molecules journal, October 2017

Coherent Vibrational and Dissociation Dynamics of Polyatomic Radical Cations journal, May 2019

Symphony on strong field approximation journal, October 2019

Photoexcitation, Ionization, and Dissociation of Molecules Using Intense Near-Infrared Radiation of Femtosecond Duration
journal, August 1999

Concerted elimination of CH2I2 and CH2ICl under intense femtosecond laser excitation
journal, January 2004

Excitation and ionization of the monohaloethylenes (C2H3X, X = F, Cl, Br, I). I. Inner-shell excitation by electron energy loss spectroscopy
journal, April 1989

Ionization and dissociation dynamics of vinyl bromide probed by femtosecond extreme ultraviolet transient absorption spectroscopy
journal, February 2014

Stabilities of isomeric halonium ions C2H4X+ (X = chlorine, bromine) by photoionization mass spectrometry and ion cyclotron resonance spectroscopy. General considerations of the relative stabilities of cyclic and acyclic isomeric onium ions
journal, February 1979

The dynamics of small molecules in intense laser fields
journal, April 2004

Control and femtosecond time-resolved imaging of torsion in a chiral molecule
journal, May 2012

Capturing Ultrafast Quantum Dynamics with Femtosecond and Attosecond X-ray Core-Level Absorption Spectroscopy
journal, January 2013

Coherent control of the ultrafast dissociative ionization dynamics of bromochloroalkanes
journal, January 2011

Molecular fragmentation driven by ultrafast dynamic ionic resonances
journal, October 2007

Stabilities of isomeric bromonium ions C2H4Br+
journal, June 1983

Nonadiabatic Multielectron Dynamics in Strong Field Molecular Ionization
journal, January 2001

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

Ultrafast strong-field dissociative ionization dynamics of CH2Br2 probed by femtosecond soft x-ray transient absorption spectroscopy
journal, May 2008

Coulomb explosion and dissociative ionization of 1,2-dibromoethane under an intense femtosecond laser field
journal, January 2014

Inner shell excitation of CH 3F, CH 3Cl, CH 3Br and CH 3I by 2.5 keV electron impact
journal, January 1978

Tracing dissociation dynamics of CH3Br in the 3Q0 state with femtosecond extreme ultraviolet ionization
journal, October 2014

Advances in molecular quantum chemistry contained in the Q-Chem 4 program package
journal, September 2014

Nonadiabatic dynamics of polyatomic molecules and ions in strong laser fields
journal, July 2003

The Multielectron Ionization Dynamics Underlying Attosecond Strong-Field Spectroscopies
journal, March 2012

Distinguishing between relaxation pathways by combining dissociative ionization pump probe spectroscopy and ab initio calculations: A case study of cytosine
journal, May 2011

Strong-field induced XUV transmission and multiplet splitting in 4 d ⁻¹ 6 p core-excited Xe studied by femtosecond XUV transient absorption spectroscopy
journal, December 2012

High-order harmonic generation using intense femtosecond pulses
journal, February 1993

Control of Chemical Reactions by Feedback-Optimized Phase-Shaped Femtosecond Laser Pulses
journal, October 1998

Stabilization energy and positional effects in halogen-substituted alkyl ions
journal, December 1988

Generation of Coherent Soft X Rays at 2.7 nm Using High Harmonics
journal, October 1997

Spatiotemporal Imaging of Ultrafast Molecular Motion: Collapse and Revival of the $D_{2}^{+}$ Nuclear Wave Packet
journal, November 2006

Wave packet driven dissociation and concerted elimination in CH2I2
journal, November 2007

Theory of high-harmonic generation by low-frequency laser fields
journal, March 1994

Two-step Coulomb explosions of diatoms in intense laser fields
journal, December 1995

Ab initio study of methyl-bromide photodissociation in the Ã band
journal, June 2009

Carbenium ion stabilities in the gas phase and solution. An ion cyclotron resonance study of bromide transfer reactions involving alkali ions, alkyl carbenium ions, acyl cations, and cyclic halonium ions
journal, August 1977

Roaming-mediated ultrafast isomerization of geminal tri-bromides in the gas and liquid phases
journal, June 2015

Wave Packet Structure and Dynamics Measured by Coulomb Explosion
journal, May 1995

Gaussian basis sets for use in correlated molecular calculations. IX. The atoms gallium through krypton
journal, April 1999

Intense-field laser ionization rates in atoms and molecules
journal, June 2001

Dissociative double ionization of 1-bromo-2-chloroethane irradiated by an intense femtosecond laser field
journal, August 2011

Concerted elimination of Br2+ resulting from the Coulomb explosion of 1,2-dibromoethane in an intense femtosecond laser field
journal, June 2014

Direct Observation of the Transition-State Region in the Photodissociation of CH ₃ I by Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy
journal, December 2015

Ab initio investigation of Br-3 d core-excited states in HBr and HBr ⁺ toward XUV probing of photochemical dynamics
journal, January 2019

Attosecond science
conference, April 2021

Attosecond Science
book, January 2013

Attosecond science
journal, November 2017

Ab initio investigation of Br-3 d core-excited states in HBr and HBr ⁺ toward XUV probing of photochemical dynamics
journal, January 2019

Probing ultrafast C–Br bond fission in the UV photochemistry of bromoform with core-to-valence transient absorption spectroscopy
journal, September 2019

Symphony on strong field approximation
text, January 2019

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

The ultrafast X-ray spectroscopic revolution in chemical dynamics
journal, May 2018

Three-dimensional momentum imaging of dissociation in flight of metastable molecules
journal, October 2017

Coherent Vibrational and Dissociation Dynamics of Polyatomic Radical Cations
journal, May 2019

Symphony on strong field approximation
journal, October 2019