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Quantum Trajectory Surface Hopping: Theory and Its Inner Workings
Quantum Trajectory Surface Hopping: Theory and Its Inner Workings
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152137
- ISBN
- 9798384498759
- DDC
- 540
- 서명/저자
- Quantum Trajectory Surface Hopping: Theory and Its Inner Workings
- 발행사항
- [Sl] : University of California, Irvine, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 239 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
- 주기사항
- Advisor: Martens, Craig C.
- 학위논문주기
- Thesis (Ph.D.)--University of California, Irvine, 2024.
- 초록/해제
- 요약Quantum trajectory surface hopping (QTSH) is a trajectory surface hopping method that is rigorously derived from the quantum-classical Liouville equation, developed to study nonadiabatic molecular dynamics of multistate systems. This work explores the unique features of QTSH - energy conservation on the ensemble level without the imposition of ad hoc momentum rescaling, and its rigorous derivation in both the diabatic and adiabatic representations - that distinguish it from the widely used fewest switches trajectory surface hopping method (FSSH). We show that in the limit of complete and localized population transfer in the adiabatic representation, the work done by the quantum force that characterizes QTSH is akin to the strict classical energy conserving momentum 'jumps' of FSSH. Our numerical results show that the feedback between nuclear and electronic degrees of freedom, mediated by the quantum forces that work to conserve the quantum-classical energy on average, is well-incorporated in QTSH. By transforming the QTSH results for the elements of the Wigner distribution and forces from one representation to another, we conclude that QTSH is representation invariant. By analyzing the classical and quantum forces for non-adiabatic processes in both the diabatic and adiabatic representations, we found that highly non-classical processes in the adiabatic representation are, conversely, highly classical in the diabatic representation. Since errors due to inconsistencies in surface hopping are larger when significant population transfers occur, it allows us to conclude that QTSH results for the highly non-classical processes in the adiabatic representation are less accurate than for the corresponding more classical processes in the diabatic representation. We exploit the representation invariance of QTSH to obtain more accurate results for the population dynamics in the adiabatic representation.
- 일반주제명
- Chemistry
- 일반주제명
- Physical chemistry
- 일반주제명
- Computational chemistry
- 일반주제명
- Energy
- 키워드
- Quantum forces
- 기타저자
- University of California, Irvine Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-04B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■020 ▼a9798384498759
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■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aHuang, Miaoyu Dorothy.
■24510▼aQuantum Trajectory Surface Hopping: Theory and Its Inner Workings
■260 ▼a[Sl]▼bUniversity of California, Irvine▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a239 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-04, Section: B.
■500 ▼aAdvisor: Martens, Craig C.
■5021 ▼aThesis (Ph.D.)--University of California, Irvine, 2024.
■520 ▼aQuantum trajectory surface hopping (QTSH) is a trajectory surface hopping method that is rigorously derived from the quantum-classical Liouville equation, developed to study nonadiabatic molecular dynamics of multistate systems. This work explores the unique features of QTSH - energy conservation on the ensemble level without the imposition of ad hoc momentum rescaling, and its rigorous derivation in both the diabatic and adiabatic representations - that distinguish it from the widely used fewest switches trajectory surface hopping method (FSSH). We show that in the limit of complete and localized population transfer in the adiabatic representation, the work done by the quantum force that characterizes QTSH is akin to the strict classical energy conserving momentum 'jumps' of FSSH. Our numerical results show that the feedback between nuclear and electronic degrees of freedom, mediated by the quantum forces that work to conserve the quantum-classical energy on average, is well-incorporated in QTSH. By transforming the QTSH results for the elements of the Wigner distribution and forces from one representation to another, we conclude that QTSH is representation invariant. By analyzing the classical and quantum forces for non-adiabatic processes in both the diabatic and adiabatic representations, we found that highly non-classical processes in the adiabatic representation are, conversely, highly classical in the diabatic representation. Since errors due to inconsistencies in surface hopping are larger when significant population transfers occur, it allows us to conclude that QTSH results for the highly non-classical processes in the adiabatic representation are less accurate than for the corresponding more classical processes in the diabatic representation. We exploit the representation invariance of QTSH to obtain more accurate results for the population dynamics in the adiabatic representation.
■590 ▼aSchool code: 0030.
■650 4▼aChemistry
■650 4▼aPhysical chemistry
■650 4▼aComputational chemistry
■650 4▼aEnergy
■653 ▼aEnergy conservation
■653 ▼aQuantum forces
■653 ▼aWigner distribution
■653 ▼aAdiabatic representation
■690 ▼a0485
■690 ▼a0494
■690 ▼a0219
■690 ▼a0791
■71020▼aUniversity of California, Irvine▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g86-04B.
■790 ▼a0030
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163122▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
