Infrared spectroscopy and tunneling dynamics of the vinyl radical in 4He nanodroplets

Raston, Paul L.; Liang, Tao; Douberly, Gary E.

doi:10.1063/1.4802767

Title: Infrared spectroscopy and tunneling dynamics of the vinyl radical in ⁴He nanodroplets

Abstract

Here, the vinyl radical has been trapped in ⁴He nanodroplets and probed with infrared laser spectroscopy in the CH stretch region between 2850 and 3200 cm^-1. The assigned band origins for the CH₂ symmetric (ν₃), CH₂ antisymmetric (ν₂), and lone α-CH stretch (ν₁) vibrations are in good agreement with previously reported full-dimensional vibrational configuration interaction computations. For all three bands, a-type and b-type transitions are observed from the lowest symmetry allowed roconvibrational state of each nuclear spin isomer, which allows for a determination of the tunneling splittings in both the ground and excited vibrational levels. Comparisons to gas phase millimeter-wave rotation-tunneling and high-resolution jet-cooled infrared spectra reveal that the He solvent effect is to reduce the ground and ν₃ excited state tunneling splittings by ≈20%. This solvent-induced modification of the tunneling dynamics can be reasonably accounted for by assuming either a ≈2.5% increase in the effective barrier height along the tunneling coordinate or a ≈5% increase in the effective reduced mass of the tunneling particles.

Authors:

Raston, Paul L. ^[1]; Liang, Tao ^[1];

^[1]

Univ. of Georgia, Athens, GA (United States)

Publication Date:: Wed May 01 00:00:00 EDT 2013

Research Org.:: Univ. of Georgia, Athens, GA (United States)

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

OSTI Identifier:: 1409045

Grant/Contract Number:: SC0008086

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 138; Journal Issue: 17; 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

Citation Formats


                    Raston, Paul L., Liang, Tao, and Douberly, Gary E. Infrared spectroscopy and tunneling dynamics of the vinyl radical in 4He nanodroplets.  United States: N. p., 2013. 
Web.  doi:10.1063/1.4802767.

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                    Raston, Paul L., Liang, Tao, & Douberly, Gary E. Infrared spectroscopy and tunneling dynamics of the vinyl radical in 4He nanodroplets.  United States.  https://doi.org/10.1063/1.4802767

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                    Raston, Paul L., Liang, Tao, and Douberly, Gary E. Wed .  
"Infrared spectroscopy and tunneling dynamics of the vinyl radical in 4He nanodroplets".  United States.  https://doi.org/10.1063/1.4802767.  https://www.osti.gov/servlets/purl/1409045.

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@article{osti_1409045,

  title        = {Infrared spectroscopy and tunneling dynamics of the vinyl radical in 4He nanodroplets},

  author       = {Raston, Paul L. and Liang, Tao and Douberly, Gary E.},

  abstractNote = {Here, the vinyl radical has been trapped in 4He nanodroplets and probed with infrared laser spectroscopy in the CH stretch region between 2850 and 3200 cm-1. The assigned band origins for the CH2 symmetric (ν3), CH2 antisymmetric (ν2), and lone α-CH stretch (ν1) vibrations are in good agreement with previously reported full-dimensional vibrational configuration interaction computations. For all three bands, a-type and b-type transitions are observed from the lowest symmetry allowed roconvibrational state of each nuclear spin isomer, which allows for a determination of the tunneling splittings in both the ground and excited vibrational levels. Comparisons to gas phase millimeter-wave rotation-tunneling and high-resolution jet-cooled infrared spectra reveal that the He solvent effect is to reduce the ground and ν3 excited state tunneling splittings by ≈20%. This solvent-induced modification of the tunneling dynamics can be reasonably accounted for by assuming either a ≈2.5% increase in the effective barrier height along the tunneling coordinate or a ≈5% increase in the effective reduced mass of the tunneling particles.},

  doi          = {10.1063/1.4802767},

  journal      = {Journal of Chemical Physics},

  number       = 17,

  volume       = 138,

  place        = {United States},

  year         = {Wed May 01 00:00:00 EDT 2013},

  month        = {Wed May 01 00:00:00 EDT 2013}

}

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Works referenced in this record:

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Works referencing / citing this record:

Rovibrational quantum dynamics of the vinyl radical and its deuterated isotopologues
journal, January 2019

Šmydke, Jan; Fábri, Csaba; Sarka, János
Physical Chemistry Chemical Physics, Vol. 21, Issue 7
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A rigorous full-dimensional quantum dynamics study of tunneling splitting of rovibrational states of vinyl radical C ₂ H ₃
journal, June 2017

Yu, Hua-Gen; Song, Hongwei; Yang, Minghui
The Journal of Chemical Physics, Vol. 146, Issue 22
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Title: Infrared spectroscopy and tunneling dynamics of the vinyl radical in 4He nanodroplets

Abstract

Citation Formats

A Fourier transform infrared study of the D and 1 3 C substituted C 2 H 3 vinyl radical in solid argon journal, September 1988

Blueshift and intramolecular tunneling of NH3 umbrella mode in Hen4 clusters journal, November 2007

Vibrational Modes of the Vinyl and Deuterated Vinyl Radicals journal, August 2009

Ab initio large-amplitude quantum-tunneling dynamics in vinyl radical: a vibrationally adiabatic approach journal, January 2008

Rotovibrational spectroscopy of hydrogen peroxide embedded in superfluid helium nanodroplets journal, January 2011

Microcanonical thermodynamic properties of helium nanodroplets journal, August 2003

High-resolution infrared spectroscopy of jet-cooled vinyl radical: Symmetric CH2 stretch excitation and tunneling dynamics journal, January 2008

Large-amplitude dynamics in vinyl radical: The role of quantum tunneling as an isomerization mechanism journal, January 2012

Spectroscopy and dynamics in helium nanodroplets journal, April 2006

Determination of the proton tunneling splitting of the vinyl radical in the ground state by millimeter-wave spectroscopy combined with supersonic jet expansion and ultraviolet photolysis journal, February 2004

Ortho-para mixing interaction in the vinyl radical detected by millimeter-wave spectroscopy journal, September 2009

Infrared absorption spectra of vinyl radicals isolated in solid Ne journal, May 2008

Millimeter-wave spectroscopy of H2CCD: Tunneling splitting and ortho-para mixing interaction journal, October 2010

The infrared spectra of C 2 H 4 + and C 2 H 3 trapped in solid neon journal, February 2011

HF Dimer in Small Helium Clusters: Interchange-Tunneling Dynamics in a Quantum Environment journal, March 2002

Rotationally Resolved Spectroscopy of S F 6 in Liquid Helium Clusters: A Molecular Probe of Cluster Temperature journal, August 1995

Vibrational spectroscopy of a transient species through time-resolved Fourier transform infrared emission spectroscopy: The vinyl radical journal, June 2000

Full-dimensional ab initio potential energy surface and vibrational configuration interaction calculations for vinyl journal, May 2009

Density of states of helium droplets journal, December 2007

Infrared Laser Spectroscopy of the CH 3 OO Radical Formed from the Reaction of CH 3 and O 2 within a Helium Nanodroplet journal, May 2012

Evidence for an energy level substructure of molecular states in helium droplets journal, December 2007

Interchange-tunneling splitting in HCl dimer in helium nanodroplets journal, March 2008

Symmetric Double-Well Potential Model and Its Application to Vibronic Spectra: Studies of Inversion Modes of Ammonia and Nitrogen-Vacancy Defect Centers in Diamond † journal, September 2007

Tunneling Splitting of Energy Levels and Rotational Constants in the Vinyl Radical C 2 H 3 † journal, April 2006

Rotational and vibrational dynamics of ethylene in helium nanodroplets journal, March 2005

The reaction products of the 193 nm photolysis of vinyl bromide and vinyl chloride studied by time-resolved Fourier transform infrared emission spectroscopy journal, January 2006

Superfluid Helium Droplets: A Uniquely Cold Nanomatrix for Molecules and Molecular Complexes journal, May 2004

Free radicals in superfluid liquid helium nanodroplets: A pyrolysis source for the production of propargyl radical journal, July 2002

Observation of Rovibrational Transitions of HCl, (HCl) 2 , and H 2 O−HCl in Liquid Helium Nanodroplets † journal, December 2007

The hydrogen fluoride dimer in liquid helium: A prototype system for studying solvent effects on hydrogen bonding journal, December 2000

(HCl)2 and (HF)2 in small helium clusters: Quantum solvation of hydrogen-bonded dimers journal, December 2005

Infrared spectroscopy of helium nanodroplets: novel methods for physics and chemistry journal, January 2006

Automation of an “Aculight” continuous-wave optical parametric oscillator journal, January 2013

The vinyl radical investigated by infrared diode laser kinetic spectroscopy journal, January 1990

Contaminated torsional tunneling splittings in five normal‐mode vibrations of propene journal, January 1994

Rovibrational quantum dynamics of the vinyl radical and its deuterated isotopologues journal, January 2019

A rigorous full-dimensional quantum dynamics study of tunneling splitting of rovibrational states of vinyl radical C 2 H 3 journal, June 2017

Title: Infrared spectroscopy and tunneling dynamics of the vinyl radical in ⁴He nanodroplets

A Fourier transform infrared study of the D and ¹ ³ C substituted C ₂ H ₃ vinyl radical in solid argon
journal, September 1988

Blueshift and intramolecular tunneling of NH3 umbrella mode in Hen4 clusters
journal, November 2007

Vibrational Modes of the Vinyl and Deuterated Vinyl Radicals
journal, August 2009

Ab initio large-amplitude quantum-tunneling dynamics in vinyl radical: a vibrationally adiabatic approach
journal, January 2008

Rotovibrational spectroscopy of hydrogen peroxide embedded in superfluid helium nanodroplets
journal, January 2011

Microcanonical thermodynamic properties of helium nanodroplets
journal, August 2003

High-resolution infrared spectroscopy of jet-cooled vinyl radical: Symmetric CH2 stretch excitation and tunneling dynamics
journal, January 2008

Large-amplitude dynamics in vinyl radical: The role of quantum tunneling as an isomerization mechanism
journal, January 2012

Spectroscopy and dynamics in helium nanodroplets
journal, April 2006

Determination of the proton tunneling splitting of the vinyl radical in the ground state by millimeter-wave spectroscopy combined with supersonic jet expansion and ultraviolet photolysis
journal, February 2004

Ortho-para mixing interaction in the vinyl radical detected by millimeter-wave spectroscopy
journal, September 2009

Infrared absorption spectra of vinyl radicals isolated in solid Ne
journal, May 2008

Millimeter-wave spectroscopy of H2CCD: Tunneling splitting and ortho-para mixing interaction
journal, October 2010

The infrared spectra of C ₂ H ₄ ⁺ and C ₂ H ₃ trapped in solid neon
journal, February 2011

HF Dimer in Small Helium Clusters: Interchange-Tunneling Dynamics in a Quantum Environment
journal, March 2002

Rotationally Resolved Spectroscopy of S $F_{6}$ in Liquid Helium Clusters: A Molecular Probe of Cluster Temperature
journal, August 1995

Vibrational spectroscopy of a transient species through time-resolved Fourier transform infrared emission spectroscopy: The vinyl radical
journal, June 2000

Full-dimensional ab initio potential energy surface and vibrational configuration interaction calculations for vinyl
journal, May 2009

Density of states of helium droplets
journal, December 2007

Infrared Laser Spectroscopy of the CH ₃ OO Radical Formed from the Reaction of CH ₃ and O ₂ within a Helium Nanodroplet
journal, May 2012

Evidence for an energy level substructure of molecular states in helium droplets
journal, December 2007

Interchange-tunneling splitting in HCl dimer in helium nanodroplets
journal, March 2008

Symmetric Double-Well Potential Model and Its Application to Vibronic Spectra: Studies of Inversion Modes of Ammonia and Nitrogen-Vacancy Defect Centers in Diamond ^†
journal, September 2007

Tunneling Splitting of Energy Levels and Rotational Constants in the Vinyl Radical C ₂ H ₃ ^†
journal, April 2006

Rotational and vibrational dynamics of ethylene in helium nanodroplets
journal, March 2005

The reaction products of the 193 nm photolysis of vinyl bromide and vinyl chloride studied by time-resolved Fourier transform infrared emission spectroscopy
journal, January 2006

Superfluid Helium Droplets: A Uniquely Cold Nanomatrix for Molecules and Molecular Complexes
journal, May 2004

Free radicals in superfluid liquid helium nanodroplets: A pyrolysis source for the production of propargyl radical
journal, July 2002

Observation of Rovibrational Transitions of HCl, (HCl) ₂ , and H ₂ O−HCl in Liquid Helium Nanodroplets ^†
journal, December 2007

The hydrogen fluoride dimer in liquid helium: A prototype system for studying solvent effects on hydrogen bonding
journal, December 2000

(HCl)2 and (HF)2 in small helium clusters: Quantum solvation of hydrogen-bonded dimers
journal, December 2005

Infrared spectroscopy of helium nanodroplets: novel methods for physics and chemistry
journal, January 2006

Automation of an “Aculight” continuous-wave optical parametric oscillator
journal, January 2013

The vinyl radical investigated by infrared diode laser kinetic spectroscopy
journal, January 1990

Contaminated torsional tunneling splittings in five normal‐mode vibrations of propene
journal, January 1994

Rovibrational quantum dynamics of the vinyl radical and its deuterated isotopologues
journal, January 2019

A rigorous full-dimensional quantum dynamics study of tunneling splitting of rovibrational states of vinyl radical C ₂ H ₃
journal, June 2017