A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation
Abstract
UV pump-XUV/X-ray probe measurements have been successfully applied in the study of photo-induced chemical reactions. Although rich element-specific electronic structure information is accessible within XUV/X-ray (inner-shell) absorption spectra, it can be difficult to interpret the chemistry directly from the spectrum without supporting theoretical simulations. A multireference method to completely simulate UV pump-XUV/X-ray probe measurement has been developed and applied to study the methyl iodide photodissociation process. Multireference, fewest-switches surface hopping (FSSH) trajectories were used to explore the coupled electronic and ionic dynamics upon photoexcitation of methyl iodide. Interpretation of previous measurements is provided by associated multireference, restricted active space, inner-shell spectral simulations. This combination of multireference FSSH trajectories and XUV spectra provides an interpretation of transient features appearing in previous measurements within the first 100 fs after photoexcitation and validates the significant branching ratio in the final excited-state population. This methodology should prove useful for interpretation of the increasing number of inner-shell probe studies of molecular excited states or for directing new experiments toward interesting regions of the potential energy landscape.
- Authors:
-
[1];
[2];
[3]
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Stockholm Univ. (Sweden). AlbaNova University Center
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences & Biosciences Division (SC-22.1)
- OSTI Identifier:
- 1577613
- Alternate Identifier(s):
- OSTI ID: 1656530
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 12; 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; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Wang, Han, Odelius, Michael, and Prendergast, David. A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation. United States: N. p., 2019.
Web. doi:10.1063/1.5116816.
Wang, Han, Odelius, Michael, & Prendergast, David. A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation. United States. https://doi.org/10.1063/1.5116816
Wang, Han, Odelius, Michael, and Prendergast, David. Wed .
"A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation". United States. https://doi.org/10.1063/1.5116816. https://www.osti.gov/servlets/purl/1577613.
@article{osti_1577613,
title = {A combined multi-reference pump-probe simulation method with application to XUV signatures of ultrafast methyl iodide photodissociation},
author = {Wang, Han and Odelius, Michael and Prendergast, David},
abstractNote = {UV pump-XUV/X-ray probe measurements have been successfully applied in the study of photo-induced chemical reactions. Although rich element-specific electronic structure information is accessible within XUV/X-ray (inner-shell) absorption spectra, it can be difficult to interpret the chemistry directly from the spectrum without supporting theoretical simulations. A multireference method to completely simulate UV pump-XUV/X-ray probe measurement has been developed and applied to study the methyl iodide photodissociation process. Multireference, fewest-switches surface hopping (FSSH) trajectories were used to explore the coupled electronic and ionic dynamics upon photoexcitation of methyl iodide. Interpretation of previous measurements is provided by associated multireference, restricted active space, inner-shell spectral simulations. This combination of multireference FSSH trajectories and XUV spectra provides an interpretation of transient features appearing in previous measurements within the first 100 fs after photoexcitation and validates the significant branching ratio in the final excited-state population. This methodology should prove useful for interpretation of the increasing number of inner-shell probe studies of molecular excited states or for directing new experiments toward interesting regions of the potential energy landscape.},
doi = {10.1063/1.5116816},
journal = {Journal of Chemical Physics},
number = 12,
volume = 151,
place = {United States},
year = {Wed Sep 25 00:00:00 EDT 2019},
month = {Wed Sep 25 00:00:00 EDT 2019}
}
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Works referenced in this record:
Self-Consistent Field Calculations of Excited States Using the Maximum Overlap Method (MOM) †
journal, December 2008
- Gilbert, Andrew T. B.; Besley, Nicholas A.; Gill, Peter M. W.
- The Journal of Physical Chemistry A, Vol. 112, Issue 50
Acetylacetone photodynamics at a seeded free-electron laser
journal, January 2018
- Squibb, R. J.; Sapunar, M.; Ponzi, A.
- Nature Communications, Vol. 9, Issue 1
Relativistic electronic-structure calculations employing a two-component no-pair formalism with external-field projection operators
journal, June 1986
- Hess, Bernd A.
- Physical Review A, Vol. 33, Issue 6
Ultrafast X-ray Transient Absorption Spectroscopy of Gas-Phase Photochemical Reactions: A New Universal Probe of Photoinduced Molecular Dynamics
journal, November 2018
- Bhattacherjee, Aditi; Leone, Stephen R.
- Accounts of Chemical Research, Vol. 51, Issue 12
Linear-Response and Real-Time Time-Dependent Density Functional Theory Studies of Core-Level Near-Edge X-Ray Absorption
journal, August 2012
- Lopata, K.; Van Kuiken, B. E.; Khalil, M.
- Journal of Chemical Theory and Computation, Vol. 8, Issue 9
Maximum Overlap Atomic and Molecular Orbitals
journal, July 1961
- Lykos, Peter G.; Schmeising, Howard N.
- The Journal of Chemical Physics, Vol. 35, Issue 1
Application of an InGaAsP diode laser to probe photodissociation dynamics: I* quantum yields from n ‐ and i ‐C 3 F 7 I and CH 3 I by laser gain vs absorption spectroscopy
journal, February 1986
- Hess, Wayne P.; Kohler, Susan J.; Haugen, Harold K.
- The Journal of Chemical Physics, Vol. 84, Issue 4
Methyl iodide A-band decomposition study by photofragment velocity imaging
journal, September 1998
- Eppink, André T. J. B.; Parker, David H.
- The Journal of Chemical Physics, Vol. 109, Issue 12
How to select active space for multiconfigurational quantum chemistry?
journal, April 2011
- Veryazov, Valera; Malmqvist, Per Åke; Roos, Björn O.
- International Journal of Quantum Chemistry, Vol. 111, Issue 13
Quantum electrodynamical corrections to the fine structure of helium
journal, January 1974
- Douglas, Marvin; Kroll, Norman M.
- Annals of Physics, Vol. 82, Issue 1
Nonadiabatic dynamics: The SHARC approach
journal, May 2018
- Mai, Sebastian; Marquetand, Philipp; González, Leticia
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 8, Issue 6
Main Group Atoms and Dimers Studied with a New Relativistic ANO Basis Set
December 2003
- Roos, Björn O.; Lindh, Roland; Malmqvist, Per-Åke
Energy partitioning following photodissociation of methyl iodide in the A band: A velocity mapping study
journal, January 1999
- Eppink, A. T. J. B.; Parker, D. H.
- The Journal of Chemical Physics, Vol. 110, Issue 2
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
- Kamiya, Muneaki; Taketsugu, Tetsuya
- Journal of Computational Chemistry, Vol. 40, Issue 2
Ab initio molecular dynamics of thiophene: the interplay of internal conversion and intersystem crossing
journal, January 2017
- Schnappinger, Thomas; Kölle, Patrick; Marazzi, Marco
- Physical Chemistry Chemical Physics, Vol. 19, Issue 37
Corresponding Orbitals and the Nonorthogonality Problem in Molecular Quantum Mechanics
journal, September 1967
- King, Harry F.; Stanton, Richard E.; Kim, Hojing
- The Journal of Chemical Physics, Vol. 47, Issue 6
Ultrafast Intersystem Crossing in Acetylacetone via Femtosecond X-ray Transient Absorption at the Carbon K-Edge
journal, November 2017
- Bhattacherjee, Aditi; Pemmaraju, Chaitanya Das; Schnorr, Kirsten
- Journal of the American Chemical Society, Vol. 139, Issue 46
A detailed experimental and theoretical study of the femtosecond A-band photodissociation of CH3I
journal, June 2008
- de Nalda, Rebeca; Durá, Judith; García-Vela, Alberto
- The Journal of Chemical Physics, Vol. 128, Issue 24
A mean-field spin-orbit method applicable to correlated wavefunctions
journal, March 1996
- Heß, Bernd A.; Marian, Christel M.; Wahlgren, Ulf
- Chemical Physics Letters, Vol. 251, Issue 5-6
Photoinduced Heterocyclic Ring Opening of Furfural: Distinct Open-Chain Product Identification by Ultrafast X-ray Transient Absorption Spectroscopy
journal, September 2018
- Bhattacherjee, Aditi; Schnorr, Kirsten; Oesterling, Sven
- Journal of the American Chemical Society, Vol. 140, Issue 39
R2PI detection of the quantum yields of I( P1/2) and I( P3/2) in the photodissociation of C2F5I, n-C3F7I, i-C3F7I and CH3I
journal, July 2000
- Baklanov, Alexey V.; Aldener, Mattias; Lindgren, Bosse
- Chemical Physics Letters, Vol. 325, Issue 4
Potential energy surfaces for rotational excitation of CH3 product in photodissociation of CH3I
journal, December 1988
- Yabushita, Satoshi; Morokuma, Keiji
- Chemical Physics Letters, Vol. 153, Issue 6
Tracing the 267 nm-Induced Radical Formation in Dimethyl Disulfide Using Time-Resolved X-ray Absorption Spectroscopy
journal, February 2019
- Schnorr, Kirsten; Bhattacherjee, Aditi; Oosterbaan, Katherine J.
- The Journal of Physical Chemistry Letters, Vol. 10, Issue 6
Electronic Curves Crossing in Methyl Iodide by Spin–Orbit Ab Initio Calculation
journal, May 2008
- Rui, Li; Bin, Yan; Shu-Tao, Zhao
- Chinese Physics Letters, Vol. 25, Issue 5
New Relativistic ANO Basis Sets for Transition Metal Atoms
journal, July 2005
- Roos, Björn O.; Lindh, Roland; Malmqvist, Per-Åke
- The Journal of Physical Chemistry A, Vol. 109, Issue 29
Structural dynamics effects on the ultrafast chemical bond cleavage of a photodissociation reaction
journal, January 2014
- Corrales, María E.; Loriot, Vincent; Balerdi, Garikoitz
- Physical Chemistry Chemical Physics, Vol. 16, Issue 19
The restricted active space (RAS) state interaction approach with spin–orbit coupling
journal, May 2002
- Malmqvist, Per Åke; Roos, Björn O.; Schimmelpfennig, Bernd
- Chemical Physics Letters, Vol. 357, Issue 3-4
Ab Initio Multiple Spawning: Photochemistry from First Principles Quantum Molecular Dynamics
journal, June 2000
- Ben-Nun, M.; Quenneville, Jason; Martínez, Todd J.
- The Journal of Physical Chemistry A, Vol. 104, Issue 22
Femtosecond multichannel photodissociation dynamics of CH3I from the A band by velocity map imaging
journal, January 2007
- de Nalda, R.; Izquierdo, J. G.; Durá, J.
- The Journal of Chemical Physics, Vol. 126, Issue 2
The multi-state CASPT2 method
journal, May 1998
- Finley, James; Malmqvist, Per-Åke; Roos, Björn O.
- Chemical Physics Letters, Vol. 288, Issue 2-4
Effects of vibrational motion on core-level spectra of prototype organic molecules
journal, December 2008
- Uejio, Janel S.; Schwartz, Craig P.; Saykally, Richard J.
- Chemical Physics Letters, Vol. 467, Issue 1-3
The spin–flip approach within time-dependent density functional theory: Theory and applications to diradicals
journal, March 2003
- Shao, Yihan; Head-Gordon, Martin; Krylov, Anna I.
- The Journal of Chemical Physics, Vol. 118, Issue 11
Ab Initio Calculations of X-ray Spectra: Atomic Multiplet and Molecular Orbital Effects in a Multiconfigurational SCF Approach to the L-Edge Spectra of Transition Metal Complexes
journal, November 2012
- Josefsson, Ida; Kunnus, Kristjan; Schreck, Simon
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 23
Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction
journal, April 2017
- Attar, Andrew R.; Bhattacherjee, Aditi; Pemmaraju, C. D.
- Science, Vol. 356, Issue 6333
Excited fragments from excited molecules: energy partitioning in the photodissociation of alkyl iodides
journal, January 1972
- Riley, Stephen J.; Wilson, Kent R.
- Faraday Discussions of the Chemical Society, Vol. 53
Mechanism of Ultrafast Intersystem Crossing in 2-Nitronaphthalene
journal, March 2018
- Zobel, J. Patrick; Nogueira, Juan J.; González, Leticia
- Chemistry - A European Journal, Vol. 24, Issue 20
Methyl rotation, vibration, and alignment from a multiphoton ionization study of the 266 nm photodissociation of methyl iodide
journal, April 1989
- Ogorzalek Loo, R.; Haerri, H. ‐P.; Hall, G. E.
- The Journal of Chemical Physics, Vol. 90, Issue 8
Intensities in Molecular Electronic Spectra X. Calculations on Mixed‐Halogen, Hydrogen Halide, Alkyl Halide, and Hydroxyl Spectra
journal, May 1940
- Mulliken, Robert S.
- The Journal of Chemical Physics, Vol. 8, Issue 5
Including quantum decoherence in surface hopping
journal, October 2010
- Granucci, Giovanni; Persico, Maurizio; Zoccante, Alberto
- The Journal of Chemical Physics, Vol. 133, Issue 13
Halogen-atom effect on the ultrafast photodissociation dynamics of the dihalomethanes CH 2 ICl and CH 2 BrI
journal, January 2018
- Murillo-Sánchez, Marta L.; Marggi Poullain, Sonia; Bajo, Juan J.
- Physical Chemistry Chemical Physics, Vol. 20, Issue 32
SHARC: ab Initio Molecular Dynamics with Surface Hopping in the Adiabatic Representation Including Arbitrary Couplings
journal, March 2011
- Richter, Martin; Marquetand, Philipp; González-Vázquez, Jesús
- Journal of Chemical Theory and Computation, Vol. 7, Issue 5
Simulations of iron K pre-edge X-ray absorption spectra using the restricted active space method
journal, January 2016
- Guo, Meiyuan; Sørensen, Lasse Kragh; Delcey, Mickaël G.
- Physical Chemistry Chemical Physics, Vol. 18, Issue 4
The DNA nucleobase thymine in motion – Intersystem crossing simulated with surface hopping
journal, January 2017
- Mai, Sebastian; Richter, Martin; Marquetand, Philipp
- Chemical Physics, Vol. 482
Molecular dynamics with electronic transitions
journal, July 1990
- Tully, John C.
- The Journal of Chemical Physics, Vol. 93, Issue 2
A 4D wave packet study of the CH 3 I photodissociation in the A -band. Comparison with femtosecond velocity map imaging experiments
journal, October 2011
- García-Vela, A.; de Nalda, R.; Durá, J.
- The Journal of Chemical Physics, Vol. 135, Issue 15
Multiconfigurational Second-Order Perturbation Theory Restricted Active Space (RASPT2) Method for Electronic Excited States: A Benchmark Study
journal, December 2010
- Sauri, Vicenta; Serrano-Andrés, Luis; Shahi, Abdul Rehaman Moughal
- Journal of Chemical Theory and Computation, Vol. 7, Issue 1
Direct Observation of the Transition-State Region in the Photodissociation of CH 3 I by Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy
journal, December 2015
- Attar, Andrew R.; Bhattacherjee, Aditi; Leone, Stephen R.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 24
Works referencing / citing this record:
Revealing electronic state-switching at conical intersections in alkyl iodides by ultrafast XUV transient absorption spectroscopy
journal, August 2020
- Chang, Kristina F.; Reduzzi, Maurizio; Wang, Han
- Nature Communications, Vol. 11, Issue 1