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dc.contributor.authorChurch, Matthew Steven
dc.date.accessioned2019-10-15T15:28:45Z
dc.date.available2019-10-15T15:28:45Z
dc.date.issued2019-05-30
dc.identifier.otherChurch_cornellgrad_0058F_11376
dc.identifier.otherhttp://dissertations.umi.com/cornellgrad:11376
dc.identifier.otherbibid: 11050242
dc.identifier.urihttps://hdl.handle.net/1813/67261
dc.description.abstractSemiclassical (SC) theory offers a pedagogically rich connection between quantum and classical perspectives of nature, and, furthermore, is a promising approach to incorporating quantum effects into molecular dynamics simulations. However, a variety of numerical challenges associated with SC methods, such as the cumbersome search for special trajectories, or the integration of highly oscillatory functions (i.e. the SC ``sign problem"), generally renders SC theory impractical for all but very simple, low-dimensional systems. In this dissertation we derive a variety of mixed quantum-classical (MQC) representations of the real-time correlation function within the SC initial value representation (SC-IVR) using the modified Filinov filtration (MFF) technique. The most promising of these methods are subsequently tested on a number of low- and high-dimensional systems. Each of these methods have three significant advantages. (1) They offer a significant improvement upon the SC-IVR ``sign problem." (2) They offer mode-specific quantization in a dynamically consistent framework. And (3) they are significantly easier to implement than other leading SC-IVR methodologies. The extension of these methods to nonadiabatic systems is made as well. We conclude that, in future studies of a variety of non-equilibrium molecular systems, particularly those that exhibit strong nuclear quantum effects such as interference, the novel SC-IVR methods presented here should prove to be very powerful.
dc.language.isoen_US
dc.subjectQuantum Mechanics
dc.subjectPhysical chemistry
dc.subjectComputational Chemistry
dc.subjectchemical physics
dc.subjectinitial value representation
dc.subjectsemiclassical dynamics
dc.subjecttheoretical chemistry
dc.titleSemiclassical Approaches to Complex Chemical Simulation in Real Time
dc.typedissertation or thesis
thesis.degree.disciplineChemistry and Chemical Biology
thesis.degree.grantorCornell University
thesis.degree.levelDoctor of Philosophy
thesis.degree.namePh.D., Chemistry and Chemical Biology
dc.contributor.chairAnanth, Nandini
dc.contributor.committeeMemberLoring, Roger F.
dc.contributor.committeeMemberEzra, Gregory Sion
dcterms.licensehttps://hdl.handle.net/1813/59810
dc.identifier.doihttps://doi.org/10.7298/fys0-3128


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