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Capturing Nuclear Quantum Effects at Classical Efficiency: a Path-Integral Approach


Tao, Xuecheng (2022) Capturing Nuclear Quantum Effects at Classical Efficiency: a Path-Integral Approach. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/s929-5x12.


Quantum mechanical effects of nuclei are ubiquitous in chemistry. For a typical example, zero-point energies and tunneling effects of the nuclei shift the chemical equilibrium and manipulate the reaction rate. However, theoretical investigation of such nuclear quantum effects in chemical reactions remains a challenge due to the heavy computation cost. To this end, imaginary-time path-integral based approximate methods have been previously introduced, which allows the inclusion of nuclear quantization in real-time chemical dynamics simulations at the efficiency of classical Newtonian dynamics. In the dissertation, we further extend the applicability of those path-integral methods and exploit the methods for practical chemical investigations. Specifically, we introduce novel dynamics approaches based on ring-polymer molecular dynamics methodology to incorporate nuclear quantum effects in the simulations of excited state dynamics and microcanonical scattering processes, and to examine the nuclear quantum effects in Hydrogen/Deuterium sticking to the graphene surface.

Item Type:Thesis (Dissertation (Ph.D.))
Subject Keywords:nuclear quantum effects, ring-polymer molecular dynamics, chemical dynamics, rate theory, isotope effects
Degree Grantor:California Institute of Technology
Division:Chemistry and Chemical Engineering
Major Option:Chemistry
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Miller, Thomas F.
Thesis Committee:
  • Chan, Garnet K. (chair)
  • Okumura, Mitchio
  • Wei, Lu
  • Miller, Thomas F.
Defense Date:22 March 2022
Record Number:CaltechTHESIS:03282022-213805038
Persistent URL:
Related URLs:
URLURL TypeDescription adapted for Chapter 2 adapted for Chapter 3 adapted for Chapter 4 adapted for Chapter 5 related to the thesis
Tao, Xuecheng0000-0003-2907-3839
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:14531
Deposited By: Xuecheng Tao
Deposited On:20 Apr 2022 19:42
Last Modified:13 Jul 2022 22:54

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