Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy

Chang, Kristina F.; Wang, Han; Poullain, Sonia M.; Prendergast, David; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1063/5.0056299

Title: Mapping wave packet bifurcation at a conical intersection in CH₃I by attosecond XUV transient absorption spectroscopy

Abstract

Extreme ultraviolet (XUV) transient absorption spectroscopy has emerged as a sensitive tool for mapping the real-time structural and electronic evolution of molecules. Here, attosecond XUV transient absorption is used to track dynamics in the A-band of methyl iodide (CH₃I). Gaseous CH₃I molecules are excited to the A-band by a UV pump (277 nm, ~20 fs) and probed by attosecond XUV pulses targeting iodine I(4d) core-to-valence transitions. Owing to the excellent temporal resolution of the technique, passage through a conical intersection is mapped through spectral signatures of nonadiabatic wave packet bifurcation observed to occur at 15 ± 4 fs following UV photoexcitation. The observed XUV signatures and time dynamics are in agreement with previous simulations [H. Wang, M. Odelius, and D. Prendergast, J. Chem. Phys. 151, 124106 (2019)]. Furthermore, due to the short duration of the UV pump pulse, coherent vibrational motion in the CH₃I ground state along the C-I stretch mode (538 ± 7 cm^-1) launched by resonant impulsive stimulated Raman scattering and dynamics in multiphoton excited states of CH₃I are also detected.

Authors:

^[1];

^[2];

^[3];

^[2];

^[4];

^[4]

Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. Complutense de Madrid (Spain)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Publication Date:: Tue Jun 15 00:00:00 EDT 2021

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1840946

Alternate Identifier(s):: OSTI ID: 1788285

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 154; Journal Issue: 23; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Quantum chemical dynamics; Photodissocation; Raman scattering; Spin-orbit interaction; XUV transient absorption spectroscopy; Photochemistry

Citation Formats


                    Chang, Kristina F., Wang, Han, Poullain, Sonia M., Prendergast, David, Neumark, Daniel M., and Leone, Stephen R. Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy.  United States: N. p., 2021. 
Web.  doi:10.1063/5.0056299.

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                    Chang, Kristina F., Wang, Han, Poullain, Sonia M., Prendergast, David, Neumark, Daniel M., & Leone, Stephen R. Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy.  United States.  https://doi.org/10.1063/5.0056299

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                    Chang, Kristina F., Wang, Han, Poullain, Sonia M., Prendergast, David, Neumark, Daniel M., and Leone, Stephen R. Tue .  
"Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy".  United States.  https://doi.org/10.1063/5.0056299.  https://www.osti.gov/servlets/purl/1840946.

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@article{osti_1840946,

  title        = {Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy},

  author       = {Chang, Kristina F. and Wang, Han and Poullain, Sonia M. and Prendergast, David and Neumark, Daniel M. and Leone, Stephen R.},

  abstractNote = {Extreme ultraviolet (XUV) transient absorption spectroscopy has emerged as a sensitive tool for mapping the real-time structural and electronic evolution of molecules. Here, attosecond XUV transient absorption is used to track dynamics in the A-band of methyl iodide (CH3I). Gaseous CH3I molecules are excited to the A-band by a UV pump (277 nm, ~20 fs) and probed by attosecond XUV pulses targeting iodine I(4d) core-to-valence transitions. Owing to the excellent temporal resolution of the technique, passage through a conical intersection is mapped through spectral signatures of nonadiabatic wave packet bifurcation observed to occur at 15 ± 4 fs following UV photoexcitation. The observed XUV signatures and time dynamics are in agreement with previous simulations [H. Wang, M. Odelius, and D. Prendergast, J. Chem. Phys. 151, 124106 (2019)]. Furthermore, due to the short duration of the UV pump pulse, coherent vibrational motion in the CH3I ground state along the C-I stretch mode (538 ± 7 cm-1) launched by resonant impulsive stimulated Raman scattering and dynamics in multiphoton excited states of CH3I are also detected.},

  doi          = {10.1063/5.0056299},

  journal      = {Journal of Chemical Physics},

  number       = 23,

  volume       = 154,

  place        = {United States},

  year         = {Tue Jun 15 00:00:00 EDT 2021},

  month        = {Tue Jun 15 00:00:00 EDT 2021}

}

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Title: Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy

Abstract

Citation Formats

An ab initio study of the CH3I photodissociation. I. Potential energy surfaces journal, June 2007

Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy journal, July 2019

Structural dynamics effects on the ultrafast chemical bond cleavage of a photodissociation reaction journal, January 2014

Impulsive excitation of coherent vibrational motion ground surface dynamics induced by intense short pulses journal, November 1994

Coulomb Explosion Imaging for the Visualization of a Conical Intersection journal, December 2018

Vibrational energy distribution of the CH 3 radical photodissociated from CH 3 I journal, October 1980

A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation journal, September 2019

Photofragmentation of CH 3 I: Vibrational distribution of the CH 3 fragment journal, October 1981

The absorption spectrum of CH 3 I in the extreme VUV journal, May 1982

Time-resolved vibrational spectroscopy in the impulsive limit journal, January 1994

Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy journal, July 2019

Two-photon VUV laser-induced fluorescence detection of I★(2P12) and I(2P12) from alkyl iodide photodissociation at 248 nm journal, March 1987

Impulsive stimulated scattering: General importance in femtosecond laser pulse interactions with matter, and spectroscopic applications journal, December 1985

Revealing electronic state-switching at conical intersections in alkyl iodides by ultrafast XUV transient absorption spectroscopy journal, August 2020

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction journal, April 2017

Two‐dimensional imaging of state‐selected photodissociation products detected by multiphoton ionization journal, July 1987

Energy partitioning following photodissociation of methyl iodide in the A band: A velocity mapping study journal, January 1999

Excited fragments from excited molecules: energy partitioning in the photodissociation of alkyl iodides journal, January 1972

Ab initio surface hopping excited‐state molecular dynamics approach on the basis of spin–orbit coupled states: An application to the A‐band photodissociation of CH 3 I journal, November 2018

Ultrafast Intersystem Crossing in Acetylacetone via Femtosecond X-ray Transient Absorption at the Carbon K-Edge journal, November 2017

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Communication: XUV transient absorption spectroscopy of iodomethane and iodobenzene photodissociation journal, July 2016

Quantum nonadiabatic effects in the photodissociation of vibrationally excited CH 3 I journal, May 1991

Quantitative studies of the photoabsorption (4.5–488 eV) and photoionization (9–59.5 eV) of methyl iodide using dipole electron impact techniques journal, June 1998

Magnetic circular dichroism spectra of the methyl halides. Resolution of the n → σ* continuum journal, July 1975

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

Title: Mapping wave packet bifurcation at a conical intersection in CH₃I by attosecond XUV transient absorption spectroscopy

An ab initio study of the CH3I photodissociation. I. Potential energy surfaces
journal, June 2007

Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy
journal, July 2019

Structural dynamics effects on the ultrafast chemical bond cleavage of a photodissociation reaction
journal, January 2014

Impulsive excitation of coherent vibrational motion ground surface dynamics induced by intense short pulses
journal, November 1994

Coulomb Explosion Imaging for the Visualization of a Conical Intersection
journal, December 2018

Vibrational energy distribution of the CH ₃ radical photodissociated from CH ₃ I
journal, October 1980

A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation
journal, September 2019

Photofragmentation of CH ₃ I: Vibrational distribution of the CH ₃ fragment
journal, October 1981

The absorption spectrum of CH ₃ I in the extreme VUV
journal, May 1982

Time-resolved vibrational spectroscopy in the impulsive limit
journal, January 1994

Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy
journal, July 2019

Two-photon VUV laser-induced fluorescence detection of I★(2P12) and I(2P12) from alkyl iodide photodissociation at 248 nm
journal, March 1987

Impulsive stimulated scattering: General importance in femtosecond laser pulse interactions with matter, and spectroscopic applications
journal, December 1985

Revealing electronic state-switching at conical intersections in alkyl iodides by ultrafast XUV transient absorption spectroscopy
journal, August 2020

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction
journal, April 2017

Two‐dimensional imaging of state‐selected photodissociation products detected by multiphoton ionization
journal, July 1987

Energy partitioning following photodissociation of methyl iodide in the A band: A velocity mapping study
journal, January 1999

Excited fragments from excited molecules: energy partitioning in the photodissociation of alkyl iodides
journal, January 1972

Ab initio surface hopping excited‐state molecular dynamics approach on the basis of spin–orbit coupled states: An application to the A‐band photodissociation of CH 3 I
journal, November 2018

Ultrafast Intersystem Crossing in Acetylacetone via Femtosecond X-ray Transient Absorption at the Carbon K-Edge
journal, November 2017

Probing the Dynamics of Rydberg and Valence States of Molecular Nitrogen with Attosecond Transient Absorption Spectroscopy
journal, February 2016

Intensities in Molecular Electronic Spectra X. Calculations on Mixed‐Halogen, Hydrogen Halide, Alkyl Halide, and Hydroxyl Spectra
journal, May 1940

Communication: XUV transient absorption spectroscopy of iodomethane and iodobenzene photodissociation
journal, July 2016

Quantum nonadiabatic effects in the photodissociation of vibrationally excited CH ₃ I
journal, May 1991

Quantitative studies of the photoabsorption (4.5–488 eV) and photoionization (9–59.5 eV) of methyl iodide using dipole electron impact techniques
journal, June 1998

Magnetic circular dichroism spectra of the methyl halides. Resolution of the n → σ* continuum
journal, July 1975

Molecular dynamics with electronic transitions
journal, July 1990

Elucidating the origins of multimode vibrational coherences of polyatomic molecules induced by intense laser fields
journal, September 2017

Transition state region in the A-Band photodissociation of allyl iodide—A femtosecond extreme ultraviolet transient absorption study
journal, March 2016

Photodissociation of gas phase I3− using femtosecond photoelectron spectroscopy
journal, August 1999

Vibrational anharmonicity in CH ₃ I: A joint local and normal mode study
journal, July 1989

Femtosecond Real-Time Probing of Reactions. 23. Studies of Temporal, Velocity, Angular, and State Dynamics from Transition States to Final Products by Femtosecond-Resolved Mass Spectrometry
journal, June 1998

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