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Kopin Liu - One of the best experts on this subject based on the ideXlab platform.
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Differential steric effects in Cl reactions with aligned CHD3(v1 = 1) by the R(0) and Q(1) transitions. II. Abstracting the unexcited D-atoms.
The Journal of Chemical Physics, 2016Co-Authors: Fengyan Wang, Kopin LiuAbstract:A complete set of four polarization-dependent differential cross sections in the reactions of Cl + aligned-CHD3(v1=1,jK)→DCl(v=0)+CHD2(v1=1) is reported here for two different, rotationally polarized states with j = 1: specifically the jK=10 state prepared via the R(0) excitation and the 1±1 state via Q(1). In stark contrast to the complicated situation of the HCl(v) + CD3(v = 0) channel reported in Paper-I, the stereo-requirement of this isotopic channel for both polarized reactants appears quite straightforward and consistent with a direct rebound mechanism. The extent of steric effects is moderate and relatively smaller than the alternative H-atom abstraction channel. All major findings reported here can qualitatively be understood by first noting that the present reaction invokes abstracting a D-atom, which is the spectator in the IR-excitation process. Next, it is recognized that the directional properties of two polarized states of CHD3(v1=1, jK) should manifest primarily in the IR-excited C–H bond, leaving secondary imprints in the unexcited CD3-moiety. The stereo-specificity of the DCl + CHD2 product channel is further reduced by the fact that the abstraction can occur with any one of the three spatially distinct D-atoms.
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differential steric effects in cl reactions with aligned chd3 v1 1 by the r 0 and q 1 transitions ii abstracting the unexcited d atoms
Journal of Chemical Physics, 2016Co-Authors: Fengyan Wang, Kopin LiuAbstract:A complete set of four polarization-dependent differential cross sections in the reactions of Cl + aligned-CHD3(v1=1,jK)→DCl(v=0)+CHD2(v1=1) is reported here for two different, rotationally polarized states with j = 1: specifically the jK=10 state prepared via the R(0) excitation and the 1±1 state via Q(1). In stark contrast to the complicated situation of the HCl(v) + CD3(v = 0) channel reported in Paper-I, the stereo-requirement of this isotopic channel for both polarized reactants appears quite straightforward and consistent with a direct rebound mechanism. The extent of steric effects is moderate and relatively smaller than the alternative H-atom abstraction channel. All major findings reported here can qualitatively be understood by first noting that the present reaction invokes abstracting a D-atom, which is the spectator in the IR-excitation process. Next, it is recognized that the directional properties of two polarized states of CHD3(v1=1, jK) should manifest primarily in the IR-excited C–H bond, leaving secondary imprints in the unexcited CD3-moiety. The stereo-specificity of the DCl + CHD2 product channel is further reduced by the fact that the abstraction can occur with any one of the three spatially distinct D-atoms.
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correlated dynamics of the o 3p chd3 v 0 reaction a joint crossed beam and quasiclassical trajectory study
Journal of Physical Chemistry A, 2015Co-Authors: Bailin Zhang, Kopin Liu, Gábor CzakóAbstract:Crossed beam experiments and quasiclassical trajectory computations on an ab initio potential energy surface are performed for the O(3P) + CHD3(v=0) → OH(v′=0) + CD3(v2=0,2) and OD(v′=0,1) + CHD2(v=0) reactions. Both experiment and theory show that the excitation functions display a concave-up behavior and the angular distributions are backward scattered, indicating a direct rebound mechanism and a tight-bend transition state. The reaction produces mainly ground-state products showing the dominance of a vibrationally adiabatic reaction pathway. The standard histogram binning cannot reproduce the observed vibrational adiabaticity, whereas Gaussian binning gives good agreement with experiment.
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Correlated Dynamics of the O(3P) + CHD3(v=0) Reaction: A Joint Crossed-Beam and Quasiclassical Trajectory Study
The Journal of Physical Chemistry A, 2014Co-Authors: Bailin Zhang, Kopin Liu, Gábor CzakóAbstract:Crossed beam experiments and quasiclassical trajectory computations on an ab initio potential energy surface are performed for the O(3P) + CHD3(v=0) → OH(v′=0) + CD3(v2=0,2) and OD(v′=0,1) + CHD2(v=0) reactions. Both experiment and theory show that the excitation functions display a concave-up behavior and the angular distributions are backward scattered, indicating a direct rebound mechanism and a tight-bend transition state. The reaction produces mainly ground-state products showing the dominance of a vibrationally adiabatic reaction pathway. The standard histogram binning cannot reproduce the observed vibrational adiabaticity, whereas Gaussian binning gives good agreement with experiment.
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Communication: Experimental and theoretical investigations of the effects of the reactant bending excitations in the F+CHD3 reaction
The Journal of Chemical Physics, 2010Co-Authors: Gábor Czakó, Kopin Liu, Quan Shuai, Joel M. BowmanAbstract:The effects of the reactant bending excitations in the F+CHD3 reaction are investigated by crossed molecular beam experiments and quasiclassical trajectory (QCT) calculations using a high-quality ab initio potential energy surface. The collision energy (Ec) dependence of the cross sections of the F+CHD3(vb=0,1) reactions for the correlated product pairs HF(v′)+CD3(v2=0,1) and DF(v′)+CHD2(v4=0,1) is obtained. Both experiment and theory show that the bending excitation activates the reaction at low Ec and begins to inactivate at higher Ec. The experimental F+CHD3(vb=1) excitation functions display surprising peak features, especially for the HF(v′=3)+CD3(v2=0,1) channels, indicating reactive resonances (quantum effects), which cannot be captured by quasiclassical calculations. The reactant state-specific QCT calculations predict that the v5(e) bending mode excitation is the most efficient to drive the reaction and the v6(e) and v5(e) modes enhance the DF and HF channels, respectively.
Joaquin Espinosa-garcia - One of the best experts on this subject based on the ideXlab platform.
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Theoretical Study of the Pair-Correlated F + CHD3(v = 0,ν1 = 1) Reaction: Effect of CH Stretching Vibrational Excitation
The Journal of Physical Chemistry A, 2017Co-Authors: Joaquin Espinosa-garcia, L Bonnet, Jose C CorchadoAbstract:The F + CHD3(v) reaction is a benchmark system in polyatomic reactions. Theoretical/experimental comparisons have been reported in recent years that present some controversies, specifically the role of the reactant CH stretching vibrational excitation, CHD3(ν1 = 1), on the reactivity of both isotope channels, DF(v) + CHD2(v′) and HF(v) + CD3(v′). However, in many cases, these comparisons are not made on an equal footing. Previous theoretical studies were concerned with overall reactivity of each isotope channel, while fine velocity map imaging experiments provided results in a product pair-correlated manner. In order to shed some light on these controversies, we perform here a pair-correlated theory/experiment comparison for the title reaction, using quasi-classical trajectory calculations on a full dimensional potential energy surface. When these calculations are analyzed in a quantum spirit, i.e., by discarding those trajectories whose results do not meet quantum-mechanical requirements and aiming to re...
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Quasiclassical Trajectory Study on the Role of CH-Stretching Vibrational Excitation in the F(2P) + CHD3(v1=0,1) Reactions
The Journal of Physical Chemistry A, 2015Co-Authors: Joaquin Espinosa-garciaAbstract:To analyze the role of CH-stretching vibrational excitation on the reactivity and dynamics of the F(2P) + CHD3(v1=0,1) reactions, quasiclassical trajectory calculations using a full-dimensional analytical potential energy surface at different collision energies were performed. The extra energy of the CH excitation had almost no effect on the reactivity for the DF + CHD2 channel, although it increased the reactivity for the HF + CD3 channel, with the net effect being that CH excitation barely modified overall reactivity. In addition, the DF/HF branching ratio was not far from the statistical value for the ground-state reaction, whereas CH excitation decreased this ratio. These results, intimately related to the topology of the entrance channel, agree with recent theoretical results obtained using different surfaces (although some differences even persist among them) but strongly contradict recent experiments. This controversy will doubtless guarantee more accurate experiments and theoretical calculations i...
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The abstraction reaction of H and C–H stretch excited CHD3: A QCT study on an ab initio based potential energy surface
Computational and Theoretical Chemistry, 2013Co-Authors: Joaquin Espinosa-garcia, Jose C CorchadoAbstract:Abstract Using a recent ab initio based potential energy surface, PES-2009, quasi-classical trajectory calculations were performed to analyse the effects of the C–H stretch excitation on the reactivity and dynamics of the H + CHD3 abstraction reaction at a collision energy of 1.53 eV. Firstly, we found that the C–H stretch mode excitation has little influence on the product rotational distributions and on the scattering distribution for both channels. However, it has significant influence on the product energy distribution for the CHD2 + HD channel, indicating that the reaction shows mode selectivity, reproducing the experimental evidence. Finally, excitation of the C–H stretch by one quantum increases the reactivity of the vibrational ground-state for both channels reproducing the experimental evidence, although for the H-abstraction channel we report an enhancement of reactivity somewhat lower than other theoretical results.
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State-to-state dynamics analysis of the F + CHD3 reaction: a quasiclassical trajectory study.
The Journal of Physical Chemistry A, 2008Co-Authors: Joaquin Espinosa-garcia, José Luis BravoAbstract:An exhaustive state-to-state dynamics study was performed to analyze the F + CHD3 → FD(ν′,j′) + CHD2(ν) gas-phase abstraction reaction. Quasiclassical trajectory (QCT) calculations, including corrections to avoid zero-point energy leakage along the trajectories, were performed at different collision energies on an analytical potential energy surface (PES-2006) recently developed by our group. Whereas the CHD2 coproduct appears vibrationally and rotationally cold, most of the available energy appears as FD(ν′) product vibrational energy, peaking at ν′ = 2 and ν′ = 3, with the population in the latter level growing as the energy increases. The excitation function rises from the threshold of the reaction and then levels off at higher energies, with the maximum contribution from the FD(ν′ = 3) level. The state-specific FD(ν′) scattering distributions correlated with the coproduct CHD2 in the ν4 = 2 and ν3 = 1 states, at different collision energies, show a steady change from backward to forward scattering as ...
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Role of the C-H stretch mode excitation in the dynamics of the Cl + CHD3 reaction: a quasi-classical trajectory calculation.
The Journal of Physical Chemistry A, 2007Co-Authors: Joaquin Espinosa-garciaAbstract:To analyze the effect of the C−H stretch mode excitation on the dynamics of the Cl + CHD3 gas-phase abstraction reaction, an exhaustive state-to-state dynamics study was performed. This reaction can evolve along two channels: H-abstraction, CD3 + ClH, and D-abstraction, CHD2 + ClD. On an analytical potential energy surface constructed previously by our group, named PES-2005, quasi-classical trajectory calculations were performed at a collision energy of 0.18 eV, including corrections to avoid zero-point energy leakage along the trajectories. First, strong coupling between different vibrational modes in the entry valley was observed; i.e., the reaction is vibrationally nonadiabatic. Second, for the ground-state CHD3(ν=0) reaction, the diatomic fragments appeared in their ground states, and the H- and D-abstraction reactions showed similar reactivities. However, when the reactivity per atom is considered, the H is three times more reactive than the D atom. Third, when the C−H stretch mode is excited by one...
J Espinosagarcia - One of the best experts on this subject based on the ideXlab platform.
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theoretical study of the pair correlated f chd3 v 0 ν1 1 reaction effect of ch stretching vibrational excitation
Journal of Physical Chemistry A, 2017Co-Authors: J Espinosagarcia, L Bonnet, Jose C CorchadoAbstract:The F + CHD3(v) reaction is a benchmark system in polyatomic reactions. Theoretical/experimental comparisons have been reported in recent years that present some controversies, specifically the role of the reactant CH stretching vibrational excitation, CHD3(ν1 = 1), on the reactivity of both isotope channels, DF(v) + CHD2(v′) and HF(v) + CD3(v′). However, in many cases, these comparisons are not made on an equal footing. Previous theoretical studies were concerned with overall reactivity of each isotope channel, while fine velocity map imaging experiments provided results in a product pair-correlated manner. In order to shed some light on these controversies, we perform here a pair-correlated theory/experiment comparison for the title reaction, using quasi-classical trajectory calculations on a full dimensional potential energy surface. When these calculations are analyzed in a quantum spirit, i.e., by discarding those trajectories whose results do not meet quantum-mechanical requirements and aiming to re...
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quasiclassical trajectory study on the role of ch stretching vibrational excitation in the f 2p chd3 v1 0 1 reactions
Journal of Physical Chemistry A, 2016Co-Authors: J EspinosagarciaAbstract:To analyze the role of CH-stretching vibrational excitation on the reactivity and dynamics of the F(2P) + CHD3(v1=0,1) reactions, quasiclassical trajectory calculations using a full-dimensional analytical potential energy surface at different collision energies were performed. The extra energy of the CH excitation had almost no effect on the reactivity for the DF + CHD2 channel, although it increased the reactivity for the HF + CD3 channel, with the net effect being that CH excitation barely modified overall reactivity. In addition, the DF/HF branching ratio was not far from the statistical value for the ground-state reaction, whereas CH excitation decreased this ratio. These results, intimately related to the topology of the entrance channel, agree with recent theoretical results obtained using different surfaces (although some differences even persist among them) but strongly contradict recent experiments. This controversy will doubtless guarantee more accurate experiments and theoretical calculations i...
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the abstraction reaction of h and c h stretch excited chd3 a qct study on an ab initio based potential energy surface
Computational and Theoretical Chemistry, 2013Co-Authors: J Espinosagarcia, Jose C CorchadoAbstract:Abstract Using a recent ab initio based potential energy surface, PES-2009, quasi-classical trajectory calculations were performed to analyse the effects of the C–H stretch excitation on the reactivity and dynamics of the H + CHD3 abstraction reaction at a collision energy of 1.53 eV. Firstly, we found that the C–H stretch mode excitation has little influence on the product rotational distributions and on the scattering distribution for both channels. However, it has significant influence on the product energy distribution for the CHD2 + HD channel, indicating that the reaction shows mode selectivity, reproducing the experimental evidence. Finally, excitation of the C–H stretch by one quantum increases the reactivity of the vibrational ground-state for both channels reproducing the experimental evidence, although for the H-abstraction channel we report an enhancement of reactivity somewhat lower than other theoretical results.
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state to state dynamics analysis of the f chd3 reaction a quasiclassical trajectory study
Journal of Physical Chemistry A, 2008Co-Authors: J Espinosagarcia, José Luis BravoAbstract:An exhaustive state-to-state dynamics study was performed to analyze the F + CHD3 → FD(ν′,j′) + CHD2(ν) gas-phase abstraction reaction. Quasiclassical trajectory (QCT) calculations, including corrections to avoid zero-point energy leakage along the trajectories, were performed at different collision energies on an analytical potential energy surface (PES-2006) recently developed by our group. Whereas the CHD2 coproduct appears vibrationally and rotationally cold, most of the available energy appears as FD(ν′) product vibrational energy, peaking at ν′ = 2 and ν′ = 3, with the population in the latter level growing as the energy increases. The excitation function rises from the threshold of the reaction and then levels off at higher energies, with the maximum contribution from the FD(ν′ = 3) level. The state-specific FD(ν′) scattering distributions correlated with the coproduct CHD2 in the ν4 = 2 and ν3 = 1 states, at different collision energies, show a steady change from backward to forward scattering as ...
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role of the c h stretch mode excitation in the dynamics of the cl chd3 reaction a quasi classical trajectory calculation
Journal of Physical Chemistry A, 2007Co-Authors: J EspinosagarciaAbstract:To analyze the effect of the C−H stretch mode excitation on the dynamics of the Cl + CHD3 gas-phase abstraction reaction, an exhaustive state-to-state dynamics study was performed. This reaction can evolve along two channels: H-abstraction, CD3 + ClH, and D-abstraction, CHD2 + ClD. On an analytical potential energy surface constructed previously by our group, named PES-2005, quasi-classical trajectory calculations were performed at a collision energy of 0.18 eV, including corrections to avoid zero-point energy leakage along the trajectories. First, strong coupling between different vibrational modes in the entry valley was observed; i.e., the reaction is vibrationally nonadiabatic. Second, for the ground-state CHD3(ν=0) reaction, the diatomic fragments appeared in their ground states, and the H- and D-abstraction reactions showed similar reactivities. However, when the reactivity per atom is considered, the H is three times more reactive than the D atom. Third, when the C−H stretch mode is excited by one...
Fengyan Wang - One of the best experts on this subject based on the ideXlab platform.
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Differential steric effects in Cl reactions with aligned CHD3(v1 = 1) by the R(0) and Q(1) transitions. II. Abstracting the unexcited D-atoms.
The Journal of Chemical Physics, 2016Co-Authors: Fengyan Wang, Kopin LiuAbstract:A complete set of four polarization-dependent differential cross sections in the reactions of Cl + aligned-CHD3(v1=1,jK)→DCl(v=0)+CHD2(v1=1) is reported here for two different, rotationally polarized states with j = 1: specifically the jK=10 state prepared via the R(0) excitation and the 1±1 state via Q(1). In stark contrast to the complicated situation of the HCl(v) + CD3(v = 0) channel reported in Paper-I, the stereo-requirement of this isotopic channel for both polarized reactants appears quite straightforward and consistent with a direct rebound mechanism. The extent of steric effects is moderate and relatively smaller than the alternative H-atom abstraction channel. All major findings reported here can qualitatively be understood by first noting that the present reaction invokes abstracting a D-atom, which is the spectator in the IR-excitation process. Next, it is recognized that the directional properties of two polarized states of CHD3(v1=1, jK) should manifest primarily in the IR-excited C–H bond, leaving secondary imprints in the unexcited CD3-moiety. The stereo-specificity of the DCl + CHD2 product channel is further reduced by the fact that the abstraction can occur with any one of the three spatially distinct D-atoms.
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differential steric effects in cl reactions with aligned chd3 v1 1 by the r 0 and q 1 transitions ii abstracting the unexcited d atoms
Journal of Chemical Physics, 2016Co-Authors: Fengyan Wang, Kopin LiuAbstract:A complete set of four polarization-dependent differential cross sections in the reactions of Cl + aligned-CHD3(v1=1,jK)→DCl(v=0)+CHD2(v1=1) is reported here for two different, rotationally polarized states with j = 1: specifically the jK=10 state prepared via the R(0) excitation and the 1±1 state via Q(1). In stark contrast to the complicated situation of the HCl(v) + CD3(v = 0) channel reported in Paper-I, the stereo-requirement of this isotopic channel for both polarized reactants appears quite straightforward and consistent with a direct rebound mechanism. The extent of steric effects is moderate and relatively smaller than the alternative H-atom abstraction channel. All major findings reported here can qualitatively be understood by first noting that the present reaction invokes abstracting a D-atom, which is the spectator in the IR-excitation process. Next, it is recognized that the directional properties of two polarized states of CHD3(v1=1, jK) should manifest primarily in the IR-excited C–H bond, leaving secondary imprints in the unexcited CD3-moiety. The stereo-specificity of the DCl + CHD2 product channel is further reduced by the fact that the abstraction can occur with any one of the three spatially distinct D-atoms.
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enlarging the reactive cone of acceptance by exciting the c h bond in the o 3p chd3 reaction
Chemical Science, 2010Co-Authors: Fengyan Wang, Kopin LiuAbstract:The effects of the CH stretching vibration of methane on the O(3P) + CHD3 reaction are elucidated in a crossed-beam imaging experiment. For the H-atom abstraction channel, the ground state reaction leads mainly to the vibrational ground states of products, OH(v = 0) + CD3(v = 0). When the reactant CHD3 is prepared with one-quantum excitation of CH stretching vibration (v1 = 1), more than 90% of OH coproducts that formed concomitantly with the CD3(v = 0) product are in v = 1. Significant vibrational enhancement in the reaction rate is observed, and the product angular distribution shifts from a backward-dominance in O(3P) + CHD3(v = 0) to a sideways-peaking upon CH stretching excitation. As to the D-atom abstraction channel, the C–H bond excitation, despite being conserved in the CHD2 product, unexpectedly hinders the overall reactivity of the unexcited C–D bond. We interpret the experimental findings as the result of enlarging the reactive cone of acceptance in abstracting the H atom at the expense of the cone for the D-atom transfer channel.
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Enlarging the reactive cone of acceptance by exciting the C–H bond in the O(3P) + CHD3 reaction
Chemical Science, 2010Co-Authors: Fengyan Wang, Kopin LiuAbstract:The effects of the CH stretching vibration of methane on the O(3P) + CHD3 reaction are elucidated in a crossed-beam imaging experiment. For the H-atom abstraction channel, the ground state reaction leads mainly to the vibrational ground states of products, OH(v = 0) + CD3(v = 0). When the reactant CHD3 is prepared with one-quantum excitation of CH stretching vibration (v1 = 1), more than 90% of OH coproducts that formed concomitantly with the CD3(v = 0) product are in v = 1. Significant vibrational enhancement in the reaction rate is observed, and the product angular distribution shifts from a backward-dominance in O(3P) + CHD3(v = 0) to a sideways-peaking upon CH stretching excitation. As to the D-atom abstraction channel, the C–H bond excitation, despite being conserved in the CHD2 product, unexpectedly hinders the overall reactivity of the unexcited C–D bond. We interpret the experimental findings as the result of enlarging the reactive cone of acceptance in abstracting the H atom at the expense of the cone for the D-atom transfer channel.
Gábor Czakó - One of the best experts on this subject based on the ideXlab platform.
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correlated dynamics of the o 3p chd3 v 0 reaction a joint crossed beam and quasiclassical trajectory study
Journal of Physical Chemistry A, 2015Co-Authors: Bailin Zhang, Kopin Liu, Gábor CzakóAbstract:Crossed beam experiments and quasiclassical trajectory computations on an ab initio potential energy surface are performed for the O(3P) + CHD3(v=0) → OH(v′=0) + CD3(v2=0,2) and OD(v′=0,1) + CHD2(v=0) reactions. Both experiment and theory show that the excitation functions display a concave-up behavior and the angular distributions are backward scattered, indicating a direct rebound mechanism and a tight-bend transition state. The reaction produces mainly ground-state products showing the dominance of a vibrationally adiabatic reaction pathway. The standard histogram binning cannot reproduce the observed vibrational adiabaticity, whereas Gaussian binning gives good agreement with experiment.
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Correlated Dynamics of the O(3P) + CHD3(v=0) Reaction: A Joint Crossed-Beam and Quasiclassical Trajectory Study
The Journal of Physical Chemistry A, 2014Co-Authors: Bailin Zhang, Kopin Liu, Gábor CzakóAbstract:Crossed beam experiments and quasiclassical trajectory computations on an ab initio potential energy surface are performed for the O(3P) + CHD3(v=0) → OH(v′=0) + CD3(v2=0,2) and OD(v′=0,1) + CHD2(v=0) reactions. Both experiment and theory show that the excitation functions display a concave-up behavior and the angular distributions are backward scattered, indicating a direct rebound mechanism and a tight-bend transition state. The reaction produces mainly ground-state products showing the dominance of a vibrationally adiabatic reaction pathway. The standard histogram binning cannot reproduce the observed vibrational adiabaticity, whereas Gaussian binning gives good agreement with experiment.
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Communication: Experimental and theoretical investigations of the effects of the reactant bending excitations in the F+CHD3 reaction
The Journal of Chemical Physics, 2010Co-Authors: Gábor Czakó, Kopin Liu, Quan Shuai, Joel M. BowmanAbstract:The effects of the reactant bending excitations in the F+CHD3 reaction are investigated by crossed molecular beam experiments and quasiclassical trajectory (QCT) calculations using a high-quality ab initio potential energy surface. The collision energy (Ec) dependence of the cross sections of the F+CHD3(vb=0,1) reactions for the correlated product pairs HF(v′)+CD3(v2=0,1) and DF(v′)+CHD2(v4=0,1) is obtained. Both experiment and theory show that the bending excitation activates the reaction at low Ec and begins to inactivate at higher Ec. The experimental F+CHD3(vb=1) excitation functions display surprising peak features, especially for the HF(v′=3)+CD3(v2=0,1) channels, indicating reactive resonances (quantum effects), which cannot be captured by quasiclassical calculations. The reactant state-specific QCT calculations predict that the v5(e) bending mode excitation is the most efficient to drive the reaction and the v6(e) and v5(e) modes enhance the DF and HF channels, respectively.
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Quasiclassical trajectory calculations of correlated product distributions for the F+CHD3(v1=0,1) reactions using an ab initio potential energy surface
The Journal of Chemical Physics, 2009Co-Authors: Gábor Czakó, Joel M. BowmanAbstract:We report quasiclassical trajectory (QCT) calculations of the correlated product distributions and branching ratios of the reactions F+CHD3(v1=0,1)→HF(v)+CD3(v) and DF(v)+CHD2(v) using a recently published ab initio-based full-dimensional global potential energy surface [G. Czako et al., J. Chem. Phys. 130, 084301 (2009)]. Harmonic normal mode analysis is done for the methyl products to determine the classical actions of each normal mode and then standard histogram binning and Gaussian binning (GB) methods are employed to obtain quantum state-resolved probabilities of the products. QCT calculations have been performed for both the vibrationally ground state and the CH stretching excited F+CHD3(v1=0,1) reactions at eight different collision energies in the 0.5–7.0 kcal/mol range. HF and DF vibrationally state-resolved rotational and angular distributions, CD3 and CHD2 mode-specific vibrational distributions, and correlated vibrationally state-specific distributions for the product pairs have been obtained ...
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quasiclassical trajectory calculations of correlated product distributions for the f chd3 v1 0 1 reactions using an ab initio potential energy surface
Journal of Chemical Physics, 2009Co-Authors: Gábor Czakó, Joel M. BowmanAbstract:We report quasiclassical trajectory (QCT) calculations of the correlated product distributions and branching ratios of the reactions F+CHD3(v1=0,1)→HF(v)+CD3(v) and DF(v)+CHD2(v) using a recently published ab initio-based full-dimensional global potential energy surface [G. Czako et al., J. Chem. Phys. 130, 084301 (2009)]. Harmonic normal mode analysis is done for the methyl products to determine the classical actions of each normal mode and then standard histogram binning and Gaussian binning (GB) methods are employed to obtain quantum state-resolved probabilities of the products. QCT calculations have been performed for both the vibrationally ground state and the CH stretching excited F+CHD3(v1=0,1) reactions at eight different collision energies in the 0.5–7.0 kcal/mol range. HF and DF vibrationally state-resolved rotational and angular distributions, CD3 and CHD2 mode-specific vibrational distributions, and correlated vibrationally state-specific distributions for the product pairs have been obtained ...