Inelastic F–H<sub>2</sub>scattering

Faubel, Manfred; Rusin, L. Yu.; Sondermann, F.; Tappe, U.; Toennies, J. P.

doi:10.1039/ft9938901475

Cited by 47 publications

(77 citation statements)

References 14 publications

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“…Whereas the experimental integral cross section summed on v' increases by a factor of 2.15 as the collision energy is increased from 78.9 to 144 meV, the QCT one grows only by a factor of 1.85. Figure 4 shows a comparison between the present QCT results and the recent experimental measurements of Faubel et a1.32, 35 The QCT and the experimentally deduced cm differential cross sections are represented in the top panel. In this case, the experimental LAB angular range restricted the cm scattering angles to be greater than about 110".…”

Section: Resultsmentioning

confidence: 73%

“…The collision energy is only slightly different than the one of the experiment of Neumark et a1.,2 but the rotational temperature of the D2 molecules is lower. In spite of these differences, the angular dependence of the two experimental cross sections is quite similar over the range of angles where they can be compared (see Figure 14 of ref 35). The QCT angular distributions portrayed in Figure 4 take explicitly into account the rotational populations of the D2 molecules in the experiment.…”

Section: Resultsmentioning

confidence: 91%

“…The simulation of the laboratory (LAB) time-of-flight (TOF) spectra is carried out by means of a Monte Carlo procedure, transforming the cm DCS into the LAB system using the appropriate Jacobian factors39 and sampling the reagents' beam velocities arid divergences from the experimental distributions given in ref 35.…”

Section: Methodsmentioning

confidence: 99%

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Quasi-Classical Trajectory Study of the F + D2 .fwdarw. DF + D Reaction on a New ab Initio Potential Energy Surface. Comparison with Molecular Beam Experimental Results

Aoiz¹,

Bañares²,

Herrero³

et al. 1994

J. Phys. Chem.

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The F + D2 reaction dynamics has been studied by means of quasi-classical trajectory calculations on a new a b initio potential energy surface. In general, there is a remarkably good agreement between the calculated and experimental vibrationally resolved differential and integral cross sections for all the collision energies studied experimentally. As in the experiments, production of DF in the v' = 3 vibrational state dominates, with smaller fractions in v' = 1, v' = 2, and v' = 4. A forward peak appears selectively for v' = 4 at the highest collision energy, in good accordance with the experimental findings.

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Section: Resultsmentioning

confidence: 73%

Section: Resultsmentioning

confidence: 91%

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Quasi-Classical Trajectory Study of the F + D2 .fwdarw. DF + D Reaction on a New ab Initio Potential Energy Surface. Comparison with Molecular Beam Experimental Results

Aoiz¹,

Bañares²,

Herrero³

et al. 1994

J. Phys. Chem.

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“…1 The high-quality ab initio potential energy surface of Stark and Werner ͑SW͒ 2 has been used in a number of quantum-scattering calculations, 3-10 quasiclassical trajectory studies, 4,11 and other investigations of the properties of the FH 2 system. [12][13][14] This theoretical work has successfully reproduced the major features seen in both the photodetachment spectrum of the FH 2 Ϫ ion 3,12 and the molecular-beam scattering studies of the reaction of F with H 2 , 9 D 2 , 15 and HD. 16 The approach of the H 2 molecule to the F atom splits the degeneracy of the 2 P state.…”

Section: Introductionmentioning

confidence: 85%

“…The molecular-beam, differential scattering studies mentioned above 15,23 indicate that the reactivity of the excited spin-orbit state is below the sensitivity level of these experiments at collision energies below 2 kcal/mol. ͑The barrier on the SW PES with the full spin-orbit Hamiltonian included, but uncorrected for zero-point effects, is Ϸ1.9 kcal/mol.…”

Section: Introductionmentioning

confidence: 98%

An investigation of the F+H2 reaction based on a full ab initio description of the open-shell character of the F(2P) atom

Alexander

Manolopoulos

Werner

2000

The Journal of Chemical Physics

257

202

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Expanding on an earlier Communication [M. H. Alexander, H.-J. Werner, and D. E. Manolopoulos, J. Chem. Phys. 109, 5710 (1998)], we present here the full framework for the quantum treatment of reactions of the fluorine atom with molecular hydrogen. This involves four potential energy surfaces (PESs) and two, coordinate-dependent spin–orbit interaction terms, all of which were fitted to the results of ab initio calculations. Quantum scattering calculations, based on a time-independent method formulated in hyperspherical coordinates, were carried out to determine initial and final state-resolved reactive cross sections, for reaction of F in its ground (2P3/2) and excited (2P1/2) spin–orbit state with H2 in j=0 and j=2(pH2) and j=1(oH2). The overall reactivity of the excited state of F, which can occur only through nonadiabatic transitions, is found to be small, at most 25% of the reactivity of the ground spin–orbit state, which is adiabatically allowed. In addition, when compared with results of earlier calculations, based on a single, electronically adiabatic, PES, our calculations show that even fine details of the dynamics of the F+H2 reaction will be well described by calculations on a single PES. The contribution of the excited spin–orbit state can be seen most clearly in the formation of HF products in the v=3 vibrational manifold, which are nearly thermoneutral (or even slightly endoergic) in the reaction of ground-state F atoms. The cross section for the near resonant electronic-rotational process [F*+H2(j=0)→F+H2(j=2)] is found to be large, in confirmation of earlier work.

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Ab initio calculations and modeling of three‐dimensional adiabatic and diabatic potential energy surfaces of F(²P)···H₂(¹Σ⁺) Van der Waals complex

Kłos

Chałasiński

Szczȩśniak

2002

Int J of Quantum Chemistry

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Three lowest diabatic potential energy surfaces for the F( 2 P) ϩ H 2 Van der Waals complex are derived from accurate ab initio calculations of the T-shaped (C 2v ) and collinear geometries (C ϱv ), at the coupled-cluster single, double, and noniterative triple excitations [CCSD(T)] level of theory with a large basis set. For the intermediate geometries the angular dependence is modeled by a simple Legendrepolynomial interpolation. The nonadiabatic coupling (off-diagonal derivative) matrix element, and the fourth, off-diagonal, diabatic surface are determined by separate multireference configuration interaction (MR-CI) calculations with a somewhat smaller basis set. Three adiabatic potential energy surfaces (PESs) are also obtained, by diagonalizing the total Hamiltonian in the diabatic basis. Both the nonrelativistic and relativistic (including spin-orbit coupling) PESs are evaluated. They are found to be in very good agreement with the entrance channel of the ASW PESs (Alexander, Manolopoulos, and Werner, J Chem Phys 2000, 113, 11084

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Inelastic F–H₂scattering

Cited by 47 publications

References 14 publications

Quasi-Classical Trajectory Study of the F + D2 .fwdarw. DF + D Reaction on a New ab Initio Potential Energy Surface. Comparison with Molecular Beam Experimental Results

Quasi-Classical Trajectory Study of the F + D2 .fwdarw. DF + D Reaction on a New ab Initio Potential Energy Surface. Comparison with Molecular Beam Experimental Results

An investigation of the F+H2 reaction based on a full ab initio description of the open-shell character of the F(2P) atom

Ab initio calculations and modeling of three‐dimensional adiabatic and diabatic potential energy surfaces of F(²P)···H₂(¹Σ⁺) Van der Waals complex

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Inelastic F–H2scattering

Cited by 47 publications

References 14 publications

Quasi-Classical Trajectory Study of the F + D2 .fwdarw. DF + D Reaction on a New ab Initio Potential Energy Surface. Comparison with Molecular Beam Experimental Results

Quasi-Classical Trajectory Study of the F + D2 .fwdarw. DF + D Reaction on a New ab Initio Potential Energy Surface. Comparison with Molecular Beam Experimental Results

An investigation of the F+H2 reaction based on a full ab initio description of the open-shell character of the F(2P) atom

Ab initio calculations and modeling of three‐dimensional adiabatic and diabatic potential energy surfaces of F(2P)···H2(1Σ+) Van der Waals complex

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Product

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Inelastic F–H₂scattering

Ab initio calculations and modeling of three‐dimensional adiabatic and diabatic potential energy surfaces of F(²P)···H₂(¹Σ⁺) Van der Waals complex