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Makri, Nancy Liu, Jian 2015-09-25T22:13:24Z 2015-09-25T22:13:24Z 10000-01-01 2005 2005 The forward-backward semiclassical dynamics (FBSD) approximation provides a rigorous and practically useful methodology for simulating the dynamics of condensed phase systems that exhibit quantum mechanical effects. It is shown that FBSD autocorrelation functions of momentum and position-dependent operators satisfy rigorously the time symmetry relation of the quantum mechanical expression. The detailed balance condition follows from this symmetry in the special case where the density is given by the Boltzmann operator. The characteristics of phase space distributions in FBSD calculations are investigated. By virtue of Liouville's theorem and energy conservation, the volume of the negative regions is rigorously conserved and the energy distribution is invariant during time evolution. Thus, while the phase space density is not invariant under FBSD, exhibiting a weak time dependence mostly in its wings, it retains its quantum mechanical characteristics and does not revert to a classical Boltzmann distribution at long times. Illustrative applications on liquid neon are presented. Made available in DSpace on 2015-09-25T22:13:24Z (GMT). No. of bitstreams: 2 license.txt: 4848 bytes, checksum: 96035ab3f5e1c23cc7138a224ce498bd (MD5) 3199071.pdf: 6496445 bytes, checksum: 4f3d35784a6701e386ce290cd7dda408 (MD5) Previous issue date: 2005 Embargo set by: Seth Robbins for item 85473 Lift date: Forever Reason: Restricted to the U of I community idenfinitely during batch ingest of legacy ETDs Restricted to the U of I community idenfinitely during batch ingest of legacy ETDs U of I Only 333 p. Thesis (Ph.D.)--University of Illinois at Urbana-Champaign, 2005. http://hdl.handle.net/2142/84192 (MiAaPQ)AAI3199071 eng Chemistry, Physical Quantum Dynamics With Classical and Quantum Trajectories text Chemistry Chemistry University of Illinois at Urbana-Champaign Dissertation Ph.D.