Abstract

This thesis investigates the role of non-Gaussian thermostatting mechanisms in controlling structural and dynamical properties of supercooled Lennard--Jones liquids using molecular dynamics simulations. Conventional thermostats such as Nose--Hoover and Langevin enforce Maxwell--Boltzmann velocity statistics and therefore strictly sample canonical ensembles. In contrast, we introduce and analyze heavy-tailed stochastic thermostats that generate controlled deviations from Gaussian velocity distributions. The resulting non-equilibrium steady states exhibit enhanced velocity kurtosis, tunable through a heavy-tail parameter $\overline{A}$, which acts as a control knob for crystallization and dynamical arrest. By systematically varying thermostat noise statistics, polydispersity, and quench protocols, we quantify the impact of excess kurtosis $\kappa$ on bond-orientational order parameters, radial distribution functions $g(r)$, and intermediate scattering functions $F(q,t)$. We further show that heavy-tailed thermostatting modifies nucleation pathways and shifts the balance between crystallization and supercooling without altering the underlying pair interaction potential. A statistical-mechanical framework where effective inverse temperatures follow a Gamma distribution, provides a theoretical interpretation of the observed non-Gaussian velocity and provides a link between non-equilibrium statistics and relaxation slow-down in supercooled systems. These results establish non-Gaussian thermostatting as a principled method for engineering metastability and glass formation in model liquids, offering new insight into the interplay between microscopic velocity statistics and emergent structural order in MD systems.

Committee Chair

Zohar Nussinov

Committee Members

Alex Seidel; Erik Henriksen; Li Yang; Rohan Mishra

Degree

Doctor of Philosophy (PhD)

Author's Department

Physics

Author's School

Graduate School of Arts and Sciences

Document Type

Dissertation

Date of Award

4-22-2026

Language

English (en)

Available for download on Wednesday, April 21, 2027

Included in

Physics Commons

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