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Attosecond Noncollinear Four-Wave Mixing Spectroscopy of Ultrafast Quantum Dynamics
Attosecond Noncollinear Four-Wave Mixing Spectroscopy of Ultrafast Quantum Dynamics
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20260202104842
- ISBN
- 9798297600690
- DDC
- 540
- 서명/저자
- Attosecond Noncollinear Four-Wave Mixing Spectroscopy of Ultrafast Quantum Dynamics
- 발행사항
- [Sl] : University of California, Berkeley, 2025
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2025
- 형태사항
- 175 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 87-04, Section: B.
- 주기사항
- Advisor: Leone, Stephen R.;Neumark, Daniel M.
- 학위논문주기
- Thesis (Ph.D.)--University of California, Berkeley, 2025.
- 초록/해제
- 요약Attosecond noncollinear four-wave mixing (FWM) spectroscopy with extreme ultraviolet (XUV) and near-infrared (NIR) pulses enables background-free, time-resolved measurements of ultrafast quantum dynamics. This technique generates spatially isolated FWM signals in order to probe correlation-driven electronic decay in a quantum-state-specific manner. The experimental apparatus is designed to compress the NIR pulses to the few-cycle regime, generate XUV pulses via table-top high-harmonic generation, and configure the three-pulses in a noncollinear, cross-beam geometry to produce FWM signals at wavevector, phase-matched angles. Attosecond noncollinear FWM accesses the dynamics of both optically allowed and forbidden excited states relative to the ground state, providing a more complete picture of electronic interactions during relaxation processes.This thesis explores fundamental electron-electron interactions via the study of autoionization decay lifetime dynamics across a series of experiments conducted in noble gases. In helium, doubly excited states show longer lifetimes with increasing principal quantum number n, consistent with the Rydberg scaling law. In neon, inner-valence excited states exhibit longer lifetimes with greater angular momentum of the orbital quantum number l, reflecting decreased spatial overlap with the core hole. In xenon, core-excited states decay via a spectator mechanism with lifetimes largely independent of principal quantum number n and orbital quantum number l. Unexpectedly long-lived dark-state signals are attributed to NIR coupling to nearby multi-electronic states. Together, these results offer new insight into how electronic structure and coupling shape decay dynamics governed by electron correlation during excited state decay processes.Future iterations of attosecond noncollinear FWM will extend this technique to the soft x-ray regime, revealing the electronic dynamics underpinning biologically-significant molecules, condensed-phase materials, and chemical reactions.
- 일반주제명
- Chemistry
- 일반주제명
- Physical chemistry
- 일반주제명
- Atomic physics
- 일반주제명
- Quantum physics
- 일반주제명
- Optics
- 키워드
- Ultraviolet
- 키워드
- Quantum number
- 기타저자
- University of California, Berkeley Chemistry
- 기본자료저록
- Dissertations Abstracts International. 87-04B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520260202104842
■006m o d
■007cr#unu||||||||
■020 ▼a9798297600690
■035 ▼a(MiAaPQ)AAI32173140
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aPuskar, Nicolette Gabrielle.
■24510▼aAttosecond Noncollinear Four-Wave Mixing Spectroscopy of Ultrafast Quantum Dynamics
■260 ▼a[Sl]▼bUniversity of California, Berkeley▼c2025
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2025
■300 ▼a175 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 87-04, Section: B.
■500 ▼aAdvisor: Leone, Stephen R.;Neumark, Daniel M.
■5021 ▼aThesis (Ph.D.)--University of California, Berkeley, 2025.
■520 ▼aAttosecond noncollinear four-wave mixing (FWM) spectroscopy with extreme ultraviolet (XUV) and near-infrared (NIR) pulses enables background-free, time-resolved measurements of ultrafast quantum dynamics. This technique generates spatially isolated FWM signals in order to probe correlation-driven electronic decay in a quantum-state-specific manner. The experimental apparatus is designed to compress the NIR pulses to the few-cycle regime, generate XUV pulses via table-top high-harmonic generation, and configure the three-pulses in a noncollinear, cross-beam geometry to produce FWM signals at wavevector, phase-matched angles. Attosecond noncollinear FWM accesses the dynamics of both optically allowed and forbidden excited states relative to the ground state, providing a more complete picture of electronic interactions during relaxation processes.This thesis explores fundamental electron-electron interactions via the study of autoionization decay lifetime dynamics across a series of experiments conducted in noble gases. In helium, doubly excited states show longer lifetimes with increasing principal quantum number n, consistent with the Rydberg scaling law. In neon, inner-valence excited states exhibit longer lifetimes with greater angular momentum of the orbital quantum number l, reflecting decreased spatial overlap with the core hole. In xenon, core-excited states decay via a spectator mechanism with lifetimes largely independent of principal quantum number n and orbital quantum number l. Unexpectedly long-lived dark-state signals are attributed to NIR coupling to nearby multi-electronic states. Together, these results offer new insight into how electronic structure and coupling shape decay dynamics governed by electron correlation during excited state decay processes.Future iterations of attosecond noncollinear FWM will extend this technique to the soft x-ray regime, revealing the electronic dynamics underpinning biologically-significant molecules, condensed-phase materials, and chemical reactions.
■590 ▼aSchool code: 0028.
■650 4▼aChemistry
■650 4▼aPhysical chemistry
■650 4▼aAtomic physics
■650 4▼aQuantum physics
■650 4▼aOptics
■653 ▼aFour-wave mixing spectroscopy
■653 ▼aNear-infrared pulses
■653 ▼aUltraviolet
■653 ▼aUltrafast quantum dynamics
■653 ▼aQuantum number
■690 ▼a0485
■690 ▼a0494
■690 ▼a0748
■690 ▼a0752
■690 ▼a0599
■71020▼aUniversity of California, Berkeley▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g87-04B.
■790 ▼a0028
■791 ▼aPh.D.
■792 ▼a2025
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17359155▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
