Semiclassical Approaches to Complex Chemical Simulation in Real Time
| dc.contributor.author | Church, Matthew Steven | |
| dc.contributor.chair | Ananth, Nandini | |
| dc.contributor.committeeMember | Loring, Roger F. | |
| dc.contributor.committeeMember | Ezra, Gregory Sion | |
| dc.date.accessioned | 2019-10-15T15:28:45Z | |
| dc.date.available | 2019-10-15T15:28:45Z | |
| dc.date.issued | 2019-05-30 | |
| dc.description.abstract | Semiclassical (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.identifier.doi | https://doi.org/10.7298/fys0-3128 | |
| dc.identifier.other | Church_cornellgrad_0058F_11376 | |
| dc.identifier.other | http://dissertations.umi.com/cornellgrad:11376 | |
| dc.identifier.other | bibid: 11050242 | |
| dc.identifier.uri | https://hdl.handle.net/1813/67261 | |
| dc.language.iso | en_US | |
| dc.subject | Quantum Mechanics | |
| dc.subject | Physical chemistry | |
| dc.subject | Computational Chemistry | |
| dc.subject | chemical physics | |
| dc.subject | initial value representation | |
| dc.subject | semiclassical dynamics | |
| dc.subject | theoretical chemistry | |
| dc.title | Semiclassical Approaches to Complex Chemical Simulation in Real Time | |
| dc.type | dissertation or thesis | |
| dcterms.license | https://hdl.handle.net/1813/59810 | |
| thesis.degree.discipline | Chemistry and Chemical Biology | |
| thesis.degree.grantor | Cornell University | |
| thesis.degree.level | Doctor of Philosophy | |
| thesis.degree.name | Ph.D., Chemistry and Chemical Biology |
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