서브메뉴
검색
First-Principles Theoretical Study of Non-Equilibrium Electron Dynamics and Electronic Excitation
First-Principles Theoretical Study of Non-Equilibrium Electron Dynamics and Electronic Excitation
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211151153
- ISBN
- 9798382630090
- DDC
- 540
- 저자명
- Zhou, Ruiyi.
- 서명/저자
- First-Principles Theoretical Study of Non-Equilibrium Electron Dynamics and Electronic Excitation
- 발행사항
- [Sl] : The University of North Carolina at Chapel Hill, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 245 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
- 주기사항
- Advisor: Kanai, Yosuke.
- 학위논문주기
- Thesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2024.
- 초록/해제
- 요약Exploring non-equilibrium electron dynamics is pivotal for developing predictive insights into molecular and material behavior. Understanding electronic excitations is essential to decipher non-equilibrium processes such as optical absorption, electron transport, and relaxation mechanisms. Quantum mechanics-based first-principles methods are highly effective in modeling the relationship between atomic structure and electron dynamics, eliminating the need for empirical fitting and ensuring quantitative accuracy in properties related to excited states.This dissertation delves into first-principles simulations of non-equilibrium electron dynamics and electronic excitation within condensed matter systems from a chemistry standpoint. The first portion of my dissertation presents nonequilibrium electron dynamics studies via real-time, time-dependent density functional theory (RT-TDDFT). Firstly, we extend natural transition orbitals within RT-TDDFT, so called, "dynamical transition orbital" offering a particle-hole perspective for non-equilibrium electron dynamics simulations. And then, we delve into the nonequilibrium phenomenon of "Floquet topological pumping" within condensed matter physics. We demonstrate the nonadiabatic Thouless pumping of electrons in trans-polyacetylene through Floquet engineering, utilizing first-principles theory. Our approach employs time-dependent maximally localized Wannier functions in real-time density functional theory simulations, linking the winding number-a topological invariant-to an molecular-level understanding of quantized pumping. Also, we identify a single dynamical transition orbital as crucial for quantized pumping, which transitions from π bonding to resonance and antibonding character during the drive cycle. Furthermore, we examine how molecular-level alterations impact the Floquet topological phase of trans-polyacetylene, particularly focusing on how chemical substitutions influence electronic structure properties, including mesmeric, inductive, and electron conjugation effects. Last, we also examine the robustness of this quantum phenomenon at ambient conditions, factoring in the dynamical electron-ion coupling and thermal fluctuations.The final portion of this dissertation comprises advanced method developments of technical methodologies for calculating electronic excited states in extended systems. We implement the Bethe-Salpeter equation in the formulism of all-electron numeric atomic orbital for periodic systems. This advancement in methodology eliminates the uncertainties stemming from the use of non-local pseudopotentials, enabling quantum chemists to leverage recent progress in Green's function theory methods.
- 일반주제명
- Chemistry
- 일반주제명
- Physical chemistry
- 일반주제명
- Condensed matter physics
- 일반주제명
- Quantum physics
- 기타저자
- The University of North Carolina at Chapel Hill Chemistry
- 기본자료저록
- Dissertations Abstracts International. 85-11B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
008250123s2024 us c eng d■001000017161037
■00520250211151153
■006m o d
■007cr#unu||||||||
■020 ▼a9798382630090
■035 ▼a(MiAaPQ)AAI31236006
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aZhou, Ruiyi.
■24510▼aFirst-Principles Theoretical Study of Non-Equilibrium Electron Dynamics and Electronic Excitation
■260 ▼a[Sl]▼bThe University of North Carolina at Chapel Hill▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a245 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 85-11, Section: B.
■500 ▼aAdvisor: Kanai, Yosuke.
■5021 ▼aThesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2024.
■520 ▼aExploring non-equilibrium electron dynamics is pivotal for developing predictive insights into molecular and material behavior. Understanding electronic excitations is essential to decipher non-equilibrium processes such as optical absorption, electron transport, and relaxation mechanisms. Quantum mechanics-based first-principles methods are highly effective in modeling the relationship between atomic structure and electron dynamics, eliminating the need for empirical fitting and ensuring quantitative accuracy in properties related to excited states.This dissertation delves into first-principles simulations of non-equilibrium electron dynamics and electronic excitation within condensed matter systems from a chemistry standpoint. The first portion of my dissertation presents nonequilibrium electron dynamics studies via real-time, time-dependent density functional theory (RT-TDDFT). Firstly, we extend natural transition orbitals within RT-TDDFT, so called, "dynamical transition orbital" offering a particle-hole perspective for non-equilibrium electron dynamics simulations. And then, we delve into the nonequilibrium phenomenon of "Floquet topological pumping" within condensed matter physics. We demonstrate the nonadiabatic Thouless pumping of electrons in trans-polyacetylene through Floquet engineering, utilizing first-principles theory. Our approach employs time-dependent maximally localized Wannier functions in real-time density functional theory simulations, linking the winding number-a topological invariant-to an molecular-level understanding of quantized pumping. Also, we identify a single dynamical transition orbital as crucial for quantized pumping, which transitions from π bonding to resonance and antibonding character during the drive cycle. Furthermore, we examine how molecular-level alterations impact the Floquet topological phase of trans-polyacetylene, particularly focusing on how chemical substitutions influence electronic structure properties, including mesmeric, inductive, and electron conjugation effects. Last, we also examine the robustness of this quantum phenomenon at ambient conditions, factoring in the dynamical electron-ion coupling and thermal fluctuations.The final portion of this dissertation comprises advanced method developments of technical methodologies for calculating electronic excited states in extended systems. We implement the Bethe-Salpeter equation in the formulism of all-electron numeric atomic orbital for periodic systems. This advancement in methodology eliminates the uncertainties stemming from the use of non-local pseudopotentials, enabling quantum chemists to leverage recent progress in Green's function theory methods.
■590 ▼aSchool code: 0153.
■650 4▼aChemistry
■650 4▼aPhysical chemistry
■650 4▼aCondensed matter physics
■650 4▼aQuantum physics
■653 ▼aBethe-Salpeter equation
■653 ▼aFirst-principles simulation
■653 ▼aMany-body perturbation theory
■653 ▼aTime-dependent density functional theory
■653 ▼aElectronic excitation
■690 ▼a0485
■690 ▼a0494
■690 ▼a0599
■690 ▼a0611
■71020▼aThe University of North Carolina at Chapel Hill▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g85-11B.
■790 ▼a0153
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17161037▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
