Communication: Mode specific quantum dynamics of the F + CHD3 → HF + CD3 reaction
Abstract
The mode specific reactivity of the F + CHD3 → HF + CD3 reaction is investigated using an eightdimensional quantum dynamical model on a recently developed ab initio based full-dimensional potential energy surface. Here, our results indicate prominent resonance structures at low collision energies and absence of an energy threshold in reaction probabilities. It was also found that excitation of the C–D stretching or CD3 umbrella mode has a relatively small impact on reactivity. On the other hand, the excitation of the C–H vibration (v1) in CHD3 is shown to significantly increase the reactivity, which, like several recent quasi-classical trajectory studies, is at odds with the available experimental data. Possible sources of the disagreement are discussed.
- Authors:
-
[1];
[3];
- Chinese Academy of Sciences (CAS), Wuhan (China). Key Lab. of Magnetic Resonance in Biological Systems, State Key Lab. of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Inst. of Physics and Mathematics
- Chinese Academy of Sciences (CAS), Wuhan (China). Key Lab. of Magnetic Resonance in Biological Systems, State Key Lab. of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Inst. of Physics and Mathematics
- Univ. Nacional de Quilmes, Bernal (Argentina). National Scientific and Technical Research Council (CONICET), Dept. de Ciencia y Tecnologia
- Univ. Bielefeld, Bielefeld (Germany). Theoretische Chemie
- Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology
- Publication Date:
- Research Org.:
- Univ. of New Mexico, Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE; National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1471067
- Alternate Identifier(s):
- OSTI ID: 1250390
- Grant/Contract Number:
- FG02-05ER15694
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 144; 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
Qi, Ji, Song, Hongwei, Yang, Minghui, Palma, Juliana, Manthe, Uwe, and Guo, Hua. Communication: Mode specific quantum dynamics of the F + CHD3 → HF + CD3 reaction. United States: N. p., 2016.
Web. doi:10.1063/1.4948547.
Qi, Ji, Song, Hongwei, Yang, Minghui, Palma, Juliana, Manthe, Uwe, & Guo, Hua. Communication: Mode specific quantum dynamics of the F + CHD3 → HF + CD3 reaction. United States. https://doi.org/10.1063/1.4948547
Qi, Ji, Song, Hongwei, Yang, Minghui, Palma, Juliana, Manthe, Uwe, and Guo, Hua. Sat .
"Communication: Mode specific quantum dynamics of the F + CHD3 → HF + CD3 reaction". United States. https://doi.org/10.1063/1.4948547. https://www.osti.gov/servlets/purl/1471067.
@article{osti_1471067,
title = {Communication: Mode specific quantum dynamics of the F + CHD3 → HF + CD3 reaction},
author = {Qi, Ji and Song, Hongwei and Yang, Minghui and Palma, Juliana and Manthe, Uwe and Guo, Hua},
abstractNote = {The mode specific reactivity of the F + CHD3 → HF + CD3 reaction is investigated using an eightdimensional quantum dynamical model on a recently developed ab initio based full-dimensional potential energy surface. Here, our results indicate prominent resonance structures at low collision energies and absence of an energy threshold in reaction probabilities. It was also found that excitation of the C–D stretching or CD3 umbrella mode has a relatively small impact on reactivity. On the other hand, the excitation of the C–H vibration (v1) in CHD3 is shown to significantly increase the reactivity, which, like several recent quasi-classical trajectory studies, is at odds with the available experimental data. Possible sources of the disagreement are discussed.},
doi = {10.1063/1.4948547},
journal = {Journal of Chemical Physics},
number = 17,
volume = 144,
place = {United States},
year = {Sat May 07 00:00:00 EDT 2016},
month = {Sat May 07 00:00:00 EDT 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 42 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
A five-dimensional quantum dynamics study of the F(P2)+CH4 reaction
journal, December 2009
- Chu, Tianshu; Han, Keli; Espinosa-Garcia, Joaquin
- The Journal of Chemical Physics, Vol. 131, Issue 24
Loss of Memory in H + CH 4 → H 2 + CH 3 State-to-State Reactive Scattering
journal, January 2015
- Welsch, Ralph; Manthe, Uwe
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 3
The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH 4 → H 2 + CH 3 reaction
journal, November 2014
- Welsch, Ralph; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 141, Issue 17
Rotationally selected product pair correlation: F+CD4→DF(ν′)+CD3(ν2=0and2,N)
journal, March 2006
- Zhou, Jingang; Shiu, Weicheng; Lin, Jim J.
- The Journal of Chemical Physics, Vol. 124, Issue 10
Communication: The origin of rotational enhancement effect for the reaction of H 2 O + + H 2 (D 2 )
journal, January 2014
- Li, Anyang; Li, Yongle; Guo, Hua
- The Journal of Chemical Physics, Vol. 140, Issue 1
An eight-dimensional quantum dynamics study of the Cl + CH4→ HCl + CH3 reaction
journal, October 2015
- Liu, Na; Yang, Minghui
- The Journal of Chemical Physics, Vol. 143, Issue 13
State-Specific Correlation of Coincident Product Pairs in the F + CD4 Reaction
journal, May 2003
- Lin, J. J.
- Science, Vol. 300, Issue 5621
Quasiclassical Trajectory Study on the Role of CH-Stretching Vibrational Excitation in the F( 2 P) + CHD 3 ( v 1 =0,1) Reactions
journal, December 2015
- Espinosa-Garcia, J.
- The Journal of Physical Chemistry A, Vol. 120, Issue 1
CH Stretching Excitation in the Early Barrier F + CHD3 Reaction Inhibits CH Bond Cleavage
journal, July 2009
- Zhang, W.; Kawamata, H.; Liu, K.
- Science, Vol. 325, Issue 5938
Mode Specificity, Bond Selectivity, and Product Energy Disposal in X + CH 4 /CHD 3 (X=H, F, O( 3 P), Cl, and OH) Hydrogen Abstraction Reactions: Perspective from Sudden Vector Projection Model
journal, May 2014
- Jiang, Bin; Guo, Hua
- Journal of the Chinese Chemical Society, Vol. 61, Issue 8
Quantum state-resolved reactive scattering of F+CH4→HF(v,J)+CH3: Nascent HF(v,J) product state distributions
journal, September 2000
- Harper, Warren W.; Nizkorodov, Sergey A.; Nesbitt, David J.
- The Journal of Chemical Physics, Vol. 113, Issue 9
Accurate ab initio potential energy surface, dynamics, and thermochemistry of the F+CH4→HF+CH3 reaction
journal, February 2009
- Czakó, Gábor; Shepler, Benjamin C.; Braams, Bastiaan J.
- The Journal of Chemical Physics, Vol. 130, Issue 8
Relative efficacy of vibrational vs. translational excitation in promoting atom-diatom reactivity: Rigorous examination of Polanyi's rules and proposition of sudden vector projection (SVP) model
journal, June 2013
- Jiang, Bin; Guo, Hua
- The Journal of Chemical Physics, Vol. 138, Issue 23
The rate of the F + H2 reaction at very low temperatures
journal, January 2014
- Tizniti, Meryem; Le Picard, Sébastien D.; Lique, François
- Nature Chemistry, Vol. 6, Issue 2
Resonances in the Entrance Channel of the Elementary Chemical Reaction of Fluorine and Methane
journal, December 2013
- Westermann, Till; Kim, Jongjin B.; Weichman, Marissa L.
- Angewandte Chemie International Edition, Vol. 53, Issue 4
Reactive resonances in the F + CHD3 reaction—a quantum dynamics study
journal, January 2011
- von Horsten, H. Frank; Clary, David C.
- Physical Chemistry Chemical Physics, Vol. 13, Issue 10
Vibrational Enhancement Factor of the Cl + CHD 3 ( v 1 = 1) Reaction: Rotational-Probe Effects
journal, January 2013
- Wang, Fengyan; Lin, Jui-San; Cheng, Yuan
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 2
Rotational mode specificity in the Cl + CHD 3 → HCl + CD 3 reaction
journal, August 2014
- Liu, Rui; Wang, Fengyan; Jiang, Bin
- The Journal of Chemical Physics, Vol. 141, Issue 7
The Sudden Vector Projection Model for Reactivity: Mode Specificity and Bond Selectivity Made Simple
journal, October 2014
- Guo, Hua; Jiang, Bin
- Accounts of Chemical Research, Vol. 47, Issue 12
A comparison study of the H + CH4 and H + SiH4 reactions with eight-dimensional quantum dynamics: normal mode versus local mode in the reactant molecule vibration
journal, August 2014
- Wang, Yan; Li, Jun; Guo, Hua
- Theoretical Chemistry Accounts, Vol. 133, Issue 10
Observation of Feshbach Resonances in the F + H2 -> HF + H Reaction
journal, March 2006
- Qiu, M.
- Science, Vol. 311, Issue 5766
CH Stretching Excitation Steers the F Atom to the CD Bond in the F + CHD 3 Reaction
journal, December 2009
- Czakó, Gábor; Bowman, Joel M.
- Journal of the American Chemical Society, Vol. 131, Issue 48
Imaging the Effects of Bend-Excitation in the F + CD 4 ( v b =0,1) → DF( v ) + CD 3 ( v 2 =1,2) Reactions
journal, March 2013
- Wang, Fengyan; Liu, Kopin
- The Journal of Physical Chemistry A, Vol. 117, Issue 36
How Is C–H Vibrational Energy Redistributed in F + CHD 3 (ν 1 = 1) → HF + CD 3 ?
journal, May 2014
- Yang, Jiayue; Zhang, Dong; Jiang, Bo
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 11
Reactive Resonance in a Polyatomic Reaction
journal, March 2004
- Shiu, Weicheng; Lin, Jim J.; Liu, Kopin
- Physical Review Letters, Vol. 92, Issue 10
Reduced dimensionality theory of quantum reactive scattering
journal, June 1991
- Bowman, Joel M.
- The Journal of Physical Chemistry, Vol. 95, Issue 13
A full-dimensional wave packet dynamics study of the photodetachment spectra of FCH 4−
journal, July 2012
- Palma, Juliana; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 137, Issue 4
State-to-State Dynamics Analysis of the F + CHD 3 Reaction: A Quasiclassical Trajectory Study
journal, July 2008
- Espinosa-García, Joaquín; Bravo, José L.
- The Journal of Physical Chemistry A, Vol. 112, Issue 27
Mode-correlated product pairs in the F+CHD3→DF+CHD2 reaction
journal, October 2003
- Zhou, Jingang; Lin, Jim J.; Liu, Kopin
- The Journal of Chemical Physics, Vol. 119, Issue 16
Coupled potential energy surface for the F( 2 P) + CH 4 → HF + CH 3 entrance channel and quantum dynamics of the CH 4 · F − photodetachment
journal, July 2013
- Westermann, Till; Eisfeld, Wolfgang; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 139, Issue 1
Vibrational Dynamics of the CH 4 ·F – Complex
journal, July 2012
- Wodraszka, Robert; Palma, Juliana; Manthe, Uwe
- The Journal of Physical Chemistry A, Vol. 116, Issue 46
Vibrationally resolved transition state spectroscopy of the F + H2 and F + CH4 reactions
journal, January 2012
- Yacovitch, Tara I.; Garand, Etienne; Kim, Jongjin B.
- Faraday Discussions, Vol. 157
An ab initio spin–orbit-corrected potential energy surface and dynamics for the F + CH4 and F + CHD3 reactions
journal, January 2011
- Czakó, Gábor; Bowman, Joel M.
- Physical Chemistry Chemical Physics, Vol. 13, Issue 18
Effects of reactant rotational excitation on reactivity: Perspectives from the sudden limit
journal, January 2014
- Jiang, Bin; Li, Jun; Guo, Hua
- The Journal of Chemical Physics, Vol. 140, Issue 3
Theoretical Study of the Validity of the Polanyi Rules for the Late-Barrier Cl + CHD 3 Reaction
journal, November 2012
- Zhang, Zhaojun; Zhou, Yong; Zhang, Dong H.
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 23
A seven-dimensional quantum study of the H+CH4 reaction
journal, December 2002
- Yang, Minghui; Zhang, Dong H.; Lee, Soo-Y.
- The Journal of Chemical Physics, Vol. 117, Issue 21
Do Vibrational Excitations of CHD3 Preferentially Promote Reactivity Toward the Chlorine Atom?
journal, June 2007
- Yan, S.; Wu, Y. -T.; Zhang, B.
- Science, Vol. 316, Issue 5832
Crossed-beam scattering of F+CD4→DF+CD3(νNK): The integral cross sections
journal, August 2003
- Zhou, Jingang; Lin, Jim J.; Shiu, Weicheng
- The Journal of Chemical Physics, Vol. 119, Issue 5
Reaction Dynamics of Methane with F, O, Cl, and Br on ab Initio Potential Energy Surfaces
journal, March 2014
- Czakó, Gábor; Bowman, Joel M.
- The Journal of Physical Chemistry A, Vol. 118, Issue 16
A Quasiclassical Study of the F( 2 P) + CHD 3 (ν 1 = 0,1) Reactive System on an Accurate Potential Energy Surface
journal, August 2015
- Palma, Juliana; Manthe, Uwe
- The Journal of Physical Chemistry A, Vol. 119, Issue 50
Mode specific dynamics of the H2 + CH3 → H + CH4 reaction studied using quasi-classical trajectory and eight-dimensional quantum dynamics methods
journal, October 2015
- Wang, Yan; Li, Jun; Chen, Liuyang
- The Journal of Chemical Physics, Vol. 143, Issue 15
State-correlation matrix of the product pair from F + CD 4 → DF(ν′) + CD 3 (0 v 2 0 0)
journal, January 2006
- Zhou, Jingang; Lin, Jim J.; Shiu, Weicheng
- Phys. Chem. Chem. Phys., Vol. 8, Issue 25
Mode selectivity in methane dissociative chemisorption on Ni(111)
journal, January 2013
- Jiang, Bin; Liu, Rui; Li, Jun
- Chemical Science, Vol. 4, Issue 8
New Analytical Potential Energy Surface for the F( 2 P) + CH 4 Hydrogen Abstraction Reaction: Kinetics and Dynamics
journal, April 2007
- Espinosa-García, J.; Bravo, J. L.; Rangel, C.
- The Journal of Physical Chemistry A, Vol. 111, Issue 14
Communication: Ro-vibrational control of chemical reactivity in H+CH 4 → H 2 +CH 3 : Full-dimensional quantum dynamics calculations and a sudden model
journal, August 2014
- Welsch, Ralph; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 141, Issue 5
Quasiclassical trajectory calculations analyzing the role of vibrational and translational energy in the F+CH2D2 reaction
journal, February 2009
- Espinosa-García, Joaquín
- The Journal of Chemical Physics, Vol. 130, Issue 5
Observation of a reactive resonance in the integral cross section of a six-atom reaction: F+CHD3
journal, July 2004
- Zhou, Jingang; Lin, Jim J.; Liu, Kopin
- The Journal of Chemical Physics, Vol. 121, Issue 2
Quasiclassical Trajectory Study of the F + CH 4 Reaction Dynamics on a Dual-Level Interpolated Potential Energy Surface
journal, September 2005
- Castillo, J. F.; Aoiz, F. J.; Bañares, L.
- The Journal of Physical Chemistry A, Vol. 109, Issue 38
Communication: Probing the entrance channels of the X + CH4 → HX + CH3 (X = F, Cl, Br, I) reactions via photodetachment of X−–CH4
journal, May 2011
- Cheng, Min; Feng, Yuan; Du, Yikui
- The Journal of Chemical Physics, Vol. 134, Issue 19
Imaging the effects of the antisymmetric stretch excitation of CH4 in the reaction with F atom
journal, January 2012
- Kawamata, Hiroshi; Zhang, Weiqing; Liu, Kopin
- Faraday Discussions, Vol. 157
Effect of CH stretching excitation on the reaction dynamics of F + CHD 3 → DF + CHD 2
journal, July 2015
- Yang, Jiayue; Zhang, Dong; Chen, Zhen
- The Journal of Chemical Physics, Vol. 143, Issue 4
Ab initio potential energy surface, variational transition state theory, and quasiclassical trajectory studies of the F+CH4→HF+CH3 reaction
journal, March 2004
- Troya, Diego; Millán, Judith; Baños, Irene
- The Journal of Chemical Physics, Vol. 120, Issue 11
Modulations of Transition-State Control of State-to-State Dynamics in the F + H 2 O → HF + OH Reaction
journal, February 2015
- Zhao, Bin; Guo, Hua
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 4
Quantum Dynamics Study of the F + CH 4 → HF + CH 3 Reaction on an Ab Initio Potential Energy Surface
journal, May 2013
- Wang, Dunyou; Czakó, Gábor
- The Journal of Physical Chemistry A, Vol. 117, Issue 32
Reduced Dimensionality Quantum Scattering Calculations on the F + CH 4 → FH + CH 3 Reaction
journal, November 2007
- Nyman, G.; Espinosa-Garcia, J.
- The Journal of Physical Chemistry A, Vol. 111, Issue 47
Perspective: Vibrational-induced steric effects in bimolecular reactions
journal, February 2015
- Liu, Kopin
- The Journal of Chemical Physics, Vol. 142, Issue 8
Quasi-Bound States of the F·CH 4 Complex
journal, January 2016
- Schäpers, Daniela; Manthe, Uwe
- The Journal of Physical Chemistry A, Vol. 120, Issue 19
Mode Selectivity for a “Central” Barrier Reaction: Eight-Dimensional Quantum Studies of the O( 3 P) + CH 4 → OH + CH 3 Reaction on an Ab Initio Potential Energy Surface
journal, December 2012
- Liu, Rui; Yang, Minghui; Czakó, Gábor
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 24
Quasi-Classical Trajectory Study of the F + CD 4 Reaction Dynamics
journal, May 2007
- Espinosa-García, Joaquín
- The Journal of Physical Chemistry A, Vol. 111, Issue 18
Experimental Signatures for a Resonance-Mediated Reaction of Bend-Excited CD 4 ( v b = 1) with Fluorine Atoms
journal, May 2011
- Wang, Fengyan; Liu, Kopin
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 12
An eight-dimensional quantum mechanical Hamiltonian for X + YCZ 3 system and its applications to H + CH 4 reaction
journal, November 2012
- Liu, Rui; Xiong, Hongwei; Yang, Minghui
- The Journal of Chemical Physics, Vol. 137, Issue 17
Quasiclassical trajectory calculations of correlated product distributions for the F+CHD3(v1=0,1) reactions using an ab initio potential energy surface
journal, December 2009
- Czakó, Gábor; Bowman, Joel M.
- The Journal of Chemical Physics, Vol. 131, Issue 24
Communication: Experimental and theoretical investigations of the effects of the reactant bending excitations in the F+CHD3 reaction
journal, October 2010
- Czakó, Gábor; Shuai, Quan; Liu, Kopin
- The Journal of Chemical Physics, Vol. 133, Issue 13
A quantum model Hamiltonian to treat reactions of the type X+YCZ3→XY+CZ3: Application to O(3P)+CH4→OH+CH3
journal, January 2000
- Palma, Juliana; Clary, David C.
- The Journal of Chemical Physics, Vol. 112, Issue 4
Works referencing / citing this record:
A neural network potential energy surface for the F + CH 4 reaction including multiple channels based on coupled cluster theory
journal, January 2018
- Chen, Jun; Xu, Xin; Liu, Shu
- Physical Chemistry Chemical Physics, Vol. 20, Issue 14
Understanding mode-specific dynamics in the local mode representation
journal, January 2018
- Song, Hongwei; Yang, Minghui
- Physical Chemistry Chemical Physics, Vol. 20, Issue 29
Imaging pair-correlated reaction cross sections in F + CH 3 D( ν b = 0, 1) → CH 2 D( ν 4 = 1) + HF( ν )
journal, January 2019
- Yang, Chung-Hsin; Hu, Li-Li; Liu, Kopin
- Physical Chemistry Chemical Physics, Vol. 21, Issue 26
Detailed benchmark ab initio mapping of the potential energy surfaces of the X + C 2 H 6 [X = F, Cl, Br, I] reactions
journal, January 2019
- Papp, Dóra; Gruber, Balázs; Czakó, Gábor
- Physical Chemistry Chemical Physics, Vol. 21, Issue 1
Natural reaction channels in H + CHD 3 → H 2 + CD 3
journal, January 2018
- Ellerbrock, Roman; Mantheuwe, Uwe
- Faraday Discussions, Vol. 212
Vibronically and spin-orbit coupled diabatic potentials for X(P) + CH 4 → HX + CH 3 reactions: General theory and application for X(P) = F( 2 P)
journal, February 2019
- Lenzen, Tim; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 150, Issue 6
Counter-propagating wave packets in the quantum transition state approach to reactive scattering
journal, May 2019
- Zhao, Bin; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 150, Issue 18
Vibronically and spin-orbit coupled diabatic potentials for X( 2 P) + CH 4 → HX + CH 3 reactions: Neural network potentials for X = Cl
journal, June 2019
- Lenzen, Tim; Eisfeld, Wolfgang; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 150, Issue 24
Vibronic coupling in the F·CH 4 prereactive complex
journal, September 2019
- Schäpers, Daniela; Manthe, Uwe
- The Journal of Chemical Physics, Vol. 151, Issue 10