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Staircase patterns of nuclear fluxes during coherent tunneling in excited doublets of symmetric double well potentials

Liu, ChunMei and Manz, Jörn and Yang, Yonggang – 2016

Tunneling isomerization of molecules with symmetric double well potentials are associated with periodic nuclear fluxes, from the reactant R to the product P and back to R. Halfway between R and P the fluxes achieve their maximum values at the potential barrier. For molecules in the lowest tunneling doublet (v = 0) the rises and falls to and from the maximum values are approximately bell-shaped. Upon excitation to higher tunneling doublets v = 1, 2, etc., however, this shape is replaced by symmetric “staircase patterns” of the fluxes, with v + 1 stepping up and down in the domains of R and P, respectively. The quantum derivation of the phenomenon is universal. It is demonstrated here for a simple model of nuclear fluxes during tunneling isomerization of ammonia along the umbrella inversion mode, with application to separation of isotopomers.

Title
Staircase patterns of nuclear fluxes during coherent tunneling in excited doublets of symmetric double well potentials
Author
Liu, ChunMei and Manz, Jörn and Yang, Yonggang
Date
2016
Identifier
DOI: 10.1039/c5cp06935a
Source(s)
Citation
Phys. Chem. Chem. Phys., 2016,18, 5048-5055