This paper describes the application of a relatively simple, but computationally tractable, particle-on-a-sphere (POS) model for quantum-mechanical calculation of large-amplitude, H atom dynamics in polyatomic hydrides (XHn), based on radially relaxed, two-dimensional angular motion of H atoms on the surface of a sphere. This work focuses on systems with many degrees of freedom, i.e., XH4 (eight dimensional) and XH5 (ten dimensional), with corresponding molecular analogs of CH4 and CH5+ and is applicable to rovibrationally excited states with J >= 0. A pairwise-additive potential fit for CH5+, which yields remarkable agreement with geometries, energies, and barrier heights on the full-dimensional surface of Brown [J. Chem. Phys. 121, 4105 (2004)] is presented. Comparisons with experimental data and diffusion quantum Monte Carlo (DMC) methods test convergence for the POS model and provide insight into multidimensional quantum rovibrational dynamics. In particular, POS energy-level patterns for a series of scaled CH5+ potentials indicate an absence of strong tunneling behavior, consistent with the highly delocalized wave functions, large zero-point energies, and small interconversion barriers noted in previous DMC studies of Brown et al. (C) 2008 American Institute of Physics.
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