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Excursions in Light-Dressed Matter Systems: From Floquet Engineering to Molecular Polaritonics
Excursions in Light-Dressed Matter Systems: From Floquet Engineering to Molecular Polaritonics
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211151123
- ISBN
- 9798384012672
- DDC
- 540
- 서명/저자
- Excursions in Light-Dressed Matter Systems: From Floquet Engineering to Molecular Polaritonics
- 발행사항
- [Sl] : University of California, San Diego, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 141 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
- 주기사항
- Advisor: Yuen Zhou, Joel.
- 학위논문주기
- Thesis (Ph.D.)--University of California, San Diego, 2024.
- 초록/해제
- 요약The detection and manipulation of matter with light is a ubiquitous goal of chemists and physicists. However, this endeavor faces inherent challenges due to the typically "weak" light-matter interaction and discrepancy in scale between molecules and the spatial variation of the electromagnetic field. Such limitations hinder the ability to differentiate between similar molecules and effectively modify their characteristics.In this dissertation, we seek to transcend the limitations of typical light-matter interactions by introducing innovative laser protocols and venturing into the realm of strong coupling. We aim to overcome the challenges attributed to natural and magnetically-induced optically activity and demystify phenomena intriguing to molecular polaritonic phenomena.We begin by proposing a laser setup to generate synthetic gauge fields within molecular aggregates to induce a molecular excitonic version of the Aharovon-Bohm effect. Even though the undriven system is achiral, this laser-induced effect generates a non-zero circular dichroism signal. Notably, an unfeasibly strong static magnetic field is needed to generate a similar effect in electronic systems.Next, we introduce a modified microwave three-wave mixing setup to achieve enantioselective topological frequency conversion. This approach, representing the first instance of a chiroptical spectroscopic signal directly linked to a topological invariant, underscores the potential of using topological principles to enhance the sensitivity and robustness of spectroscopic techniques for distinguishing between enantiomers.Transitioning into the realm of strong coupling, we explore the effects of molecular disorder on the linear response of molecular polaritons. We provide analytical expressions for the vacuum Rabi splitting observed in the absorption, transmission, and reflection spectra under conditions of weak disorder, addressing multiple disorder distributions. Additionally, we introduce a novel sum rule offering a universal methodology for extracting accurate collective light-matter coupling values from experimental data.Finally, we address the perplexing fact that classical linear optics can regularly describe polaritonic effects. We demonstrate that, in the thermodynamic limit, polaritonic transmission windows function as "optical filters", and many phenomena attributed to polaritons can be replicated in bare molecular systems using appropriately configured linear optical sources. This insight urges a reevaluation of certain "polaritonic" phenomena and identifies promising directions for future research to uncover genuinely novel polaritonic effects.
- 일반주제명
- Chemistry
- 일반주제명
- Electromagnetics
- 일반주제명
- Applied mathematics
- 키워드
- Light
- 기타저자
- University of California, San Diego Chemistry and Biochemistry
- 기본자료저록
- Dissertations Abstracts International. 86-02B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520250211151123
■006m o d
■007cr#unu||||||||
■020 ▼a9798384012672
■035 ▼a(MiAaPQ)AAI31146760
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aSchwennicke, Kai.
■24510▼aExcursions in Light-Dressed Matter Systems: From Floquet Engineering to Molecular Polaritonics
■260 ▼a[Sl]▼bUniversity of California, San Diego▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a141 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-02, Section: B.
■500 ▼aAdvisor: Yuen Zhou, Joel.
■5021 ▼aThesis (Ph.D.)--University of California, San Diego, 2024.
■520 ▼aThe detection and manipulation of matter with light is a ubiquitous goal of chemists and physicists. However, this endeavor faces inherent challenges due to the typically "weak" light-matter interaction and discrepancy in scale between molecules and the spatial variation of the electromagnetic field. Such limitations hinder the ability to differentiate between similar molecules and effectively modify their characteristics.In this dissertation, we seek to transcend the limitations of typical light-matter interactions by introducing innovative laser protocols and venturing into the realm of strong coupling. We aim to overcome the challenges attributed to natural and magnetically-induced optically activity and demystify phenomena intriguing to molecular polaritonic phenomena.We begin by proposing a laser setup to generate synthetic gauge fields within molecular aggregates to induce a molecular excitonic version of the Aharovon-Bohm effect. Even though the undriven system is achiral, this laser-induced effect generates a non-zero circular dichroism signal. Notably, an unfeasibly strong static magnetic field is needed to generate a similar effect in electronic systems.Next, we introduce a modified microwave three-wave mixing setup to achieve enantioselective topological frequency conversion. This approach, representing the first instance of a chiroptical spectroscopic signal directly linked to a topological invariant, underscores the potential of using topological principles to enhance the sensitivity and robustness of spectroscopic techniques for distinguishing between enantiomers.Transitioning into the realm of strong coupling, we explore the effects of molecular disorder on the linear response of molecular polaritons. We provide analytical expressions for the vacuum Rabi splitting observed in the absorption, transmission, and reflection spectra under conditions of weak disorder, addressing multiple disorder distributions. Additionally, we introduce a novel sum rule offering a universal methodology for extracting accurate collective light-matter coupling values from experimental data.Finally, we address the perplexing fact that classical linear optics can regularly describe polaritonic effects. We demonstrate that, in the thermodynamic limit, polaritonic transmission windows function as "optical filters", and many phenomena attributed to polaritons can be replicated in bare molecular systems using appropriately configured linear optical sources. This insight urges a reevaluation of certain "polaritonic" phenomena and identifies promising directions for future research to uncover genuinely novel polaritonic effects.
■590 ▼aSchool code: 0033.
■650 4▼aChemistry
■650 4▼aElectromagnetics
■650 4▼aApplied mathematics
■653 ▼aFloquet engineering
■653 ▼aMolecular polaritonics
■653 ▼aLight
■690 ▼a0485
■690 ▼a0607
■690 ▼a0364
■71020▼aUniversity of California, San Diego▼bChemistry and Biochemistry.
■7730 ▼tDissertations Abstracts International▼g86-02B.
■790 ▼a0033
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17160829▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.


