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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 Polarito...
Excursions in Light-Dressed Matter Systems: From Floquet Engineering to Molecular Polaritonics

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자료유형  
 학위논문 서양
최종처리일시  
20250211151123
ISBN  
9798384012672
DDC  
540
저자명  
Schwennicke, Kai.
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  
Floquet engineering
키워드  
Molecular polaritonics
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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■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.

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