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From Excited Charge Dynamics to Cluster Diffusion: Development and Application of Techniques Beyond DFT and KMC

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Date Issued:
2018
Abstract/Description:
This dissertation focuses on developing reliable and accurate computational techniques which enable the examination of static and dynamic properties of various activated phenomena using deterministic and stochastic approaches. To explore ultrafast electron dynamics in materials with strong electron-electron correlation, under the influence of a laser pulse, an ab initio electronic structure method based on time-dependent density functional theory (TDDFT) in combination with dynamical mean field theory (DMFT) is developed and applied to: 1) single-band Hubbard model; 2) multi-band metal Ni; and 3) multi-band insulator MnO. The ultrafast demagnetization in Ni reveal the importance of memory and correlation effects, leading to much better agreement with experimental data than previously obtained, while for MnO the main channels of charge response are identified. Furthermore, an analytical form of the exchange-correlation kernel is obtained for future applications, saving tremendous computational cost. In another project, size-dependent temporal and spatial evolution of homo- and hetero-epitaxial adatom islands on fcc(111) transition metals surfaces are investigated using the self-learning kinetic Monte Carlo (SLKMC) method that explores long-time dynamics unbiased by apriori selected diffusion processes. Novel multi-atom diffusion processes are revealed. Trends in the diffusion coefficients point to the relative role of adatom lateral interaction and island-substrate binding energy in determining island diffusivity. Moreover, analysis of the large data-base of the activation energy barriers generated for multitude of diffusion processes for variety of systems allows extraction of a set of descriptors that in turn generate predictive models for energy barrier evaluation. Finally, the kinetics of the industrially important methanol partial oxidation reaction on a model nanocatalyst is explored using KMC supplemented by DFT energetics. Calculated thermodynamics explores the active surface sites for reaction components including different intermediates and energetics of competing probable reaction pathways, while kinetic study attends to the selectivity of products and its variation with external factors.
Title: From Excited Charge Dynamics to Cluster Diffusion: Development and Application of Techniques Beyond DFT and KMC.
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Name(s): Acharya, Shree Ram, Author
Rahman, Talat, Committee Chair
Chow, Lee, Committee Member
Stolbov, Sergey, Committee Member
Wu, Annie, Committee Member
University of Central Florida, Degree Grantor
Type of Resource: text
Date Issued: 2018
Publisher: University of Central Florida
Language(s): English
Abstract/Description: This dissertation focuses on developing reliable and accurate computational techniques which enable the examination of static and dynamic properties of various activated phenomena using deterministic and stochastic approaches. To explore ultrafast electron dynamics in materials with strong electron-electron correlation, under the influence of a laser pulse, an ab initio electronic structure method based on time-dependent density functional theory (TDDFT) in combination with dynamical mean field theory (DMFT) is developed and applied to: 1) single-band Hubbard model; 2) multi-band metal Ni; and 3) multi-band insulator MnO. The ultrafast demagnetization in Ni reveal the importance of memory and correlation effects, leading to much better agreement with experimental data than previously obtained, while for MnO the main channels of charge response are identified. Furthermore, an analytical form of the exchange-correlation kernel is obtained for future applications, saving tremendous computational cost. In another project, size-dependent temporal and spatial evolution of homo- and hetero-epitaxial adatom islands on fcc(111) transition metals surfaces are investigated using the self-learning kinetic Monte Carlo (SLKMC) method that explores long-time dynamics unbiased by apriori selected diffusion processes. Novel multi-atom diffusion processes are revealed. Trends in the diffusion coefficients point to the relative role of adatom lateral interaction and island-substrate binding energy in determining island diffusivity. Moreover, analysis of the large data-base of the activation energy barriers generated for multitude of diffusion processes for variety of systems allows extraction of a set of descriptors that in turn generate predictive models for energy barrier evaluation. Finally, the kinetics of the industrially important methanol partial oxidation reaction on a model nanocatalyst is explored using KMC supplemented by DFT energetics. Calculated thermodynamics explores the active surface sites for reaction components including different intermediates and energetics of competing probable reaction pathways, while kinetic study attends to the selectivity of products and its variation with external factors.
Identifier: CFE0006965 (IID), ucf:52910 (fedora)
Note(s): 2018-05-01
Ph.D.
Sciences, Physics
Doctoral
This record was generated from author submitted information.
Subject(s): island diffusion -- reaction kinetics -- ultrafast dynamics -- density functional theory -- mean field theory -- kinetic monte carlo
Persistent Link to This Record: http://purl.flvc.org/ucf/fd/CFE0006965
Restrictions on Access: public 2018-05-15
Host Institution: UCF

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