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Reactions probabilities, resonances, and thermal rate constants for the collinear reactins H + FH and D + FD on a low-barrier surface. Close-coupling and tunneling calculations, variational

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j150625a019· OSTI ID:5772105

We study the collinear H + FH ..-->.. HF + H and D + FD ..-->.. DF + D reactions on a potential-energy surface that has twin 1.75 kcal/mol saddle points. We present accurate quantal reaction probabilities over a wide energy range, including three resonance energies and three resonance widths for each isotopic case. From these we calculate accurate quantal rate constants at temperatures 75 to 7000 K for H + FH and 75 to 2400 K for D + FD; and we separate out the contributions of the lowest-energy resonance to the low-temperature rates. We present plots of S-matrix phases and eigenphases and Argand diagrams. The accurate quantal results are used to test a wide variety of approximate dynamical results: semiclassical and quantal resonance calculations based on the vibrationally adiabatic model; rate constants calculated by conventional transition-state theory, three versions of variational transition-state theory, and the unified statistical model; and vibrationally adiabaic transmission coefficients.

DOE Contract Number:
AC02-79ER10425
OSTI ID:
5772105
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 85:25; ISSN JPCHA
Country of Publication:
United States
Language:
English