dc.creator Perry, David S. en_US dc.creator Martens, Jonathan en_US dc.creator Herman, Michel en_US dc.creator Amyay, Badr en_US dc.date.accessioned 2011-07-12T17:26:50Z dc.date.available 2011-07-12T17:26:50Z dc.date.issued 2011 en_US dc.identifier 2011-RD-06 en_US dc.identifier.uri http://hdl.handle.net/1811/49307 dc.description Author Institution: Department of Chemistry, The University of Akron, OH 44325-3601; Laboratoire de Chimie quantique et Photophysique, Universite libre de Bruxelles, B-1050, Belgium en_US dc.description.abstract The rotation-vibration Hamiltonian of acetylene is known in detail up to 13,000 cm$^{-1}$ in the electronic ground state, allows the calculation of time-dependent dynamics for postulated excitations of certain bright states. Three different measures of phase space exploration are examined including the participation number, Gruebele's dispersion, and the Shannon entropy. The time scales for phase space exploration span the range from 20 fs to 10 ps. The volume of phase space explored by the dynamics increases with energy and the rotational quantum number, $J$ reaching about 90\% of the (GOE) statistical limit at 12,000 cm$^{-1}$ and $J$ = 100. At low and intermediate $J$, the extent of phase space exploration is reduced for the local bender and counter-rotator bright states as compared to their normal mode counterparts. However, the phase space exploration of the local mode CH stretch state is similar to that of the corresponding normal mode vibration. These calculations shed light on the applicability of the energy randomization assumption that is at the heart of the Rice-Rampsberger-Kassel-Marcus (RRKM) theory of unimolecular reactions. en_US dc.language.iso en en_US dc.publisher Ohio State University en_US dc.title PHASE SPACE EXPLORATION OF ACETYLENE AT ENERGIES UP TO 13,000 cm$^{-1}$ en_US dc.type Article en_US dc.type Image en_US dc.type Presentation en_US
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