DOI: 10.1063/1.2768948. Theoretical investigation of the dissociation dynamics of vibrationally excited vinyl bromide on an <i>ab initio</i> potential-energy surface obtained using modified novelty sampling and feedforward neural networks. II. Numerical application of the method

Theoretical investigation of the dissociation dynamics of vibrationally excited vinyl bromide on an ab initio potential-energy surface obtained using modified novelty sampling and feedforward neural networks. II. Numerical application of the method

10.1063/1.2768948

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

A previously reported method for conducting molecular dynamics simulations of gas-phase chemical dynamics on ab initio potential-energy surfaces using modified novelty sampling and feedforward neural networks is applied to the investigation of the unimolecular dissociation of vinyl bromide. The neural network is fitted to a database comprising the MP4(SDQ) energies computed for 71 969 nuclear configurations using an extended basis set. Dissociation rate coefficients and branching ratios at an internal excitation energy of 6.44eV for all six open reaction channels are reported. The distribution of vibrational energy in HBr formed in three-center dissociation is computed and found to be in excellent accord with experimental measurements. Computational requirements for the electronic structure calculations, neural network training, and trajectory calculations are given. The weight and bias matrices required for implementation of the neural network potential are made available through the Supplementary Material.

Bibliography

Malshe, M., Raff, L. M., Rockley, M. G., Hagan, M., Agrawal, P. M., & Komanduri, R. (2007). Theoretical investigation of the dissociation dynamics of vibrationally excited vinyl bromide on an ab initio potential-energy surface obtained using modified novelty sampling and feedforward neural networks. II. Numerical application of the method. The Journal of Chemical Physics, 127(13).

Authors 6

M. Malshe (first)
L. M. Raff (additional)
M. G. Rockley (additional)
M. Hagan (additional)
Paras M. Agrawal (additional)
R. Komanduri (additional)

References 27 Referenced 53

10.1063/1.2162170 / J. Chem. Phys. (2006)
10.1063/1.2264051 / J. Chem. Phys. (2006)
10.1063/1.466801 / J. Chem. Phys. (1994)
10.1063/1.469296 / J. Chem. Phys. (1995)
10.1039/a808154i / Phys. Chem. Chem. Phys. (1999)
10.1063/1.477643 / J. Chem. Phys. (1998)
10.1039/a606038b / J. Chem. Soc., Faraday Trans. (1997)
10.1063/1.479937 / J. Chem. Phys. (1999)
10.1063/1.475655 / J. Chem. Phys. (1998)
10.1063/1.479368 / J. Chem. Phys. (1999)
10.1063/1.472977 / J. Chem. Phys. (1996)
10.1021/jp9924575 / J. Phys. Chem. (2000)
10.1063/1.1617271 / J. Chem. Phys. (2003)
10.1063/1.1777572 / J. Chem. Phys. (2004)
10.1063/1.1667458 / J. Chem. Phys. (2004)
10.1063/1.2162170 / J. Chem. Phys. (2006)
10.1063/1.476259 / J. Chem. Phys. (1998)
10.1063/1.1559480 / J. Chem. Phys. (2003)
10.1021/jp001695t / J. Phys. Chem. A (2001)
10.1021/jp001696l / J. Phys. Chem. (2001)
10.1063/1.455575 / J. Chem. Phys. (1988)
10.1063/1.456347 / J. Chem. Phys. (1989)
10.1063/1.1850458 / J. Chem. Phys. (2005)
10.1021/j100010a005 / J. Phys. Chem. (1995)
{'first-page': '414', 'volume-title': 'Vibrational Spectra of Polyatomic Molecules', 'year': '1973', 'key': '2023071506535916800_c23'} / Vibrational Spectra of Polyatomic Molecules (1973)
10.1063/1.1382812 / J. Chem. Phys. (2001)
See EPAPS Document No. E-JCPSA6-127-023732 for specification of the nature of the input vector, transfer functions, upper and lower limits for the input data, and the weight and bias matrices for each layer of the NN for vinyl bromide. This document can be reached via a direct link in the online article’s HTML reference section or via the EPAPS homepage (http://www.aip.org/pubservs/epaps.html).

Dates

Type	When
Created	17 years, 10 months ago (Oct. 4, 2007, 6:37 p.m.)
Deposited	2 years, 1 month ago (July 15, 2023, 2:54 a.m.)
Indexed	3 weeks, 4 days ago (July 30, 2025, 6:49 a.m.)
Issued	17 years, 10 months ago (Oct. 4, 2007)
Published	17 years, 10 months ago (Oct. 4, 2007)
Published Online	17 years, 10 months ago (Oct. 4, 2007)
Published Print	17 years, 10 months ago (Oct. 7, 2007)

Funders 0

None

BibTeX

@article{Malshe_2007, title={Theoretical investigation of the dissociation dynamics of vibrationally excited vinyl bromide on an ab initio potential-energy surface obtained using modified novelty sampling and feedforward neural networks. II. Numerical application of the method}, volume={127}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.2768948}, DOI={10.1063/1.2768948}, number={13}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Malshe, M. and Raff, L. M. and Rockley, M. G. and Hagan, M. and Agrawal, Paras M. and Komanduri, R.}, year={2007}, month=oct }

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