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First Principles Study of Nonequilibrium Electron Dynamics in Complex Extended Systems Using Time-Dependent Maximally Localized Wannier Functions
First Principles Study of Nonequilibrium Electron Dynamics in Complex Extended Systems Using Time-Dependent Maximally Localized Wannier Functions
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211151141
- ISBN
- 9798382715612
- DDC
- 540
- 서명/저자
- First Principles Study of Nonequilibrium Electron Dynamics in Complex Extended Systems Using Time-Dependent Maximally Localized Wannier Functions
- 발행사항
- [Sl] : The University of North Carolina at Chapel Hill, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 230 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
- 요약Developing a complete picture of the underlying electron dynamics is essential for understanding the details of numerous physical processes, including electronic stopping and optical excitation, among others. First-principles approaches offer a pathway to unravel the quantum details of these processes without reliance on any empirical data. Real-time time-dependent density functional theory (RT-TDDFT) stands out as a proficient tool, adept at accurately and efficiently simulating electron dynamics across diverse systems. Nonetheless, the molecular-level details of many electronic excitation processes remain unknown, especially for extended systems.In this dissertation we investigate the molecular-level details of various electronic dynamic phenomena using RT-TDDFT. Much of this dissertation is centered on electronic stopping in complex extended biological systems, with a specific emphasis on its application to ion beam therapy. Electronic stopping entails the transfer of energy from high energy ions, such as protons, to the electrons of a target material. The energy deposition profile is highly localized, leading to considerable attention from the medical physics community and beam therapies emergence as a viable alternative to traditional X-ray oncology cancer treatments. Using RT-TDDFT simulation we examine the electronic stopping process in both liquid water and solvated DNA to understand and build a complete picture of the ultrafast electronic response. We unveil key details of the stopping process, including how the primary excitation by an irradiating proton in liquid water precedes the formation of cationic holes. With the help of supercomputers, we compare the electronic stopping process in solvated DNA under proton, α-particle, and carbon ion irradiation. We show how significantly more energy is deposited on the sugar-phosphate side chains through the formation of highly energetic holes, leading to DNA strand damage and cell death.The concluding section of this dissertation covers technical advancements in RT-TDDFT, focusing primarily on accelerating calculations utilizing exact exchange through the implementation of time-dependent maximally localized Wannier functions (TD-MLWFs). Additionally, we detail several related advancements, including the refinement procedure for TD-MLWFs, comparison of the velocity and length gauge approaches for modeling an electric field, and usage of a complex absorbing potential for modeling isolated systems in the planewave-pseudopotential formalism of RT-TDDFT.
- 일반주제명
- Chemistry
- 일반주제명
- Physics
- 일반주제명
- Physical chemistry
- 키워드
- Energetic holes
- 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
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■00520250211151141
■006m o d
■007cr#unu||||||||
■020 ▼a9798382715612
■035 ▼a(MiAaPQ)AAI31149462
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aShepard, Christopher.
■24510▼aFirst Principles Study of Nonequilibrium Electron Dynamics in Complex Extended Systems Using Time-Dependent Maximally Localized Wannier Functions
■260 ▼a[Sl]▼bThe University of North Carolina at Chapel Hill▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a230 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 ▼aDeveloping a complete picture of the underlying electron dynamics is essential for understanding the details of numerous physical processes, including electronic stopping and optical excitation, among others. First-principles approaches offer a pathway to unravel the quantum details of these processes without reliance on any empirical data. Real-time time-dependent density functional theory (RT-TDDFT) stands out as a proficient tool, adept at accurately and efficiently simulating electron dynamics across diverse systems. Nonetheless, the molecular-level details of many electronic excitation processes remain unknown, especially for extended systems.In this dissertation we investigate the molecular-level details of various electronic dynamic phenomena using RT-TDDFT. Much of this dissertation is centered on electronic stopping in complex extended biological systems, with a specific emphasis on its application to ion beam therapy. Electronic stopping entails the transfer of energy from high energy ions, such as protons, to the electrons of a target material. The energy deposition profile is highly localized, leading to considerable attention from the medical physics community and beam therapies emergence as a viable alternative to traditional X-ray oncology cancer treatments. Using RT-TDDFT simulation we examine the electronic stopping process in both liquid water and solvated DNA to understand and build a complete picture of the ultrafast electronic response. We unveil key details of the stopping process, including how the primary excitation by an irradiating proton in liquid water precedes the formation of cationic holes. With the help of supercomputers, we compare the electronic stopping process in solvated DNA under proton, α-particle, and carbon ion irradiation. We show how significantly more energy is deposited on the sugar-phosphate side chains through the formation of highly energetic holes, leading to DNA strand damage and cell death.The concluding section of this dissertation covers technical advancements in RT-TDDFT, focusing primarily on accelerating calculations utilizing exact exchange through the implementation of time-dependent maximally localized Wannier functions (TD-MLWFs). Additionally, we detail several related advancements, including the refinement procedure for TD-MLWFs, comparison of the velocity and length gauge approaches for modeling an electric field, and usage of a complex absorbing potential for modeling isolated systems in the planewave-pseudopotential formalism of RT-TDDFT.
■590 ▼aSchool code: 0153.
■650 4▼aChemistry
■650 4▼aPhysics
■650 4▼aPhysical chemistry
■653 ▼aElectronic stopping
■653 ▼aFirst principles simulations
■653 ▼aWannier functions
■653 ▼aElectron dynamics
■653 ▼aEnergetic holes
■690 ▼a0485
■690 ▼a0605
■690 ▼a0494
■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=T17160958▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
