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Spatially and Temporally Resolved Spectroscopy of Transition Metal Dichalcogenide Semiconductors
Spatially and Temporally Resolved Spectroscopy of Transition Metal Dichalcogenide Semicond...
Spatially and Temporally Resolved Spectroscopy of Transition Metal Dichalcogenide Semiconductors

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20250211152818
ISBN  
9798384012559
DDC  
541
저자명  
Scheeler, Jason.
서명/저자  
Spatially and Temporally Resolved Spectroscopy of Transition Metal Dichalcogenide Semiconductors
발행사항  
[Sl] : The University of Wisconsin - Madison, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
157 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-02, Section: B.
주기사항  
Advisor: Wright, John C.
학위논문주기  
Thesis (Ph.D.)--The University of Wisconsin - Madison, 2024.
초록/해제  
요약Coherent multidimensional spectroscopy (CMDS) is a powerful analytical technique for learning about the structure and dynamics of quantum states in a variety of sample systems. In this dissertation, we apply CMDS to investigate monolayers and heterobilayers of transition metal dichalcogenide (TMD) semiconductors, a materials system that shows promise in photovoltaic applications. Experiments use multiple 50-femtosecond laser pulses to interrogate the rich exciton diversity in TMDs as a function of frequency, time, and space. First, we motivate adding a widefield nonlinear microscope to our CMDS setup by describing how spatial heterogeneity within monolayer and heterobilayer TMDs affects their optical properties. We discuss the design principles for each component in the widefield nonlinear microscope and present proof of principle measurements on TMDs to validate the instrument. Next, we demonstrate that two-color sum frequency generation (SFG) spectroscopy is capable of probing high-energy conduction bands in monolayer WS2. We show the technique's general applicability by performing the SFG measurements on TMDs of various sample morphologies. We extract the ultrafast dynamics of charge carriers occupying the high-energy conduction bands throughout the Brillouin zone by preceding the SFG pulse sequence with a pump pulse. Finally, we suggest software improvements to the microscope that would allow it to speed up the camera frame rate and greatly improve the S/N for pump-probe experiments with strong probe fields. For the SFG measurements, we propose additional experiments to further confirm the peak assignments made for monolayer WS2 and suggest a strategy for directly probing the dynamics of high-energy conduction bands localized at the direct-gap momentum point. This work applies foundational optical principles to build a novel widefield nonlinear imaging system and provides a framework for developing highly selective, multidimensional probes of non-direct-bandgap states in materials systems with large excitonic transition dipoles.
일반주제명  
Physical chemistry
일반주제명  
Condensed matter physics
일반주제명  
Optics
키워드  
Microscopy
키워드  
Semiconductors
키워드  
Coherent multidimensional spectroscopy
키워드  
Transition metal dichalcogenide
키워드  
Sum frequency generation
기타저자  
The University of Wisconsin - Madison Chemistry
기본자료저록  
Dissertations Abstracts International. 86-02B.
전자적 위치 및 접속  
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MARC

 008250123s2024        us                              c    eng  d
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■020    ▼a9798384012559
■035    ▼a(MiAaPQ)AAI31558888
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a541
■1001  ▼aScheeler,  Jason.
■24510▼aSpatially  and  Temporally  Resolved  Spectroscopy  of  Transition  Metal  Dichalcogenide  Semiconductors
■260    ▼a[Sl]▼bThe  University  of  Wisconsin  -  Madison▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a157  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-02,  Section:  B.
■500    ▼aAdvisor:  Wright,  John  C.
■5021  ▼aThesis  (Ph.D.)--The  University  of  Wisconsin  -  Madison,  2024.
■520    ▼aCoherent  multidimensional  spectroscopy  (CMDS)  is  a  powerful  analytical  technique  for  learning  about  the  structure  and  dynamics  of  quantum  states  in  a  variety  of  sample  systems.  In  this  dissertation,  we  apply  CMDS  to  investigate  monolayers  and  heterobilayers  of  transition  metal  dichalcogenide  (TMD)  semiconductors,  a  materials  system  that  shows  promise  in  photovoltaic  applications.  Experiments  use  multiple  50-femtosecond  laser  pulses  to  interrogate  the  rich  exciton  diversity  in  TMDs  as  a  function  of  frequency,  time,  and  space.  First,  we  motivate  adding  a  widefield  nonlinear  microscope  to  our  CMDS  setup  by  describing  how  spatial  heterogeneity  within  monolayer  and  heterobilayer  TMDs  affects  their  optical  properties.  We  discuss  the  design  principles  for  each  component  in  the  widefield  nonlinear  microscope  and  present  proof  of  principle  measurements  on  TMDs  to  validate  the  instrument.  Next,  we  demonstrate  that  two-color  sum  frequency  generation  (SFG)  spectroscopy  is  capable  of  probing  high-energy  conduction  bands  in  monolayer  WS2.  We  show  the  technique's  general  applicability  by  performing  the  SFG  measurements  on  TMDs  of  various  sample  morphologies.  We  extract  the  ultrafast  dynamics  of  charge  carriers  occupying  the  high-energy  conduction  bands  throughout  the  Brillouin  zone  by  preceding  the  SFG  pulse  sequence  with  a  pump  pulse.  Finally,  we  suggest  software  improvements  to  the  microscope  that  would  allow  it  to  speed  up  the  camera  frame  rate  and  greatly  improve  the  S/N  for  pump-probe  experiments  with  strong  probe  fields.  For  the  SFG  measurements,  we  propose  additional  experiments  to  further  confirm  the  peak  assignments  made  for  monolayer  WS2  and  suggest  a  strategy  for  directly  probing  the  dynamics  of  high-energy  conduction  bands  localized  at  the  direct-gap  momentum  point.  This  work  applies  foundational  optical  principles  to  build  a  novel  widefield  nonlinear  imaging  system  and  provides  a  framework for  developing  highly  selective,  multidimensional  probes  of  non-direct-bandgap  states  in  materials  systems  with  large  excitonic  transition  dipoles.
■590    ▼aSchool  code:  0262.
■650  4▼aPhysical  chemistry
■650  4▼aCondensed  matter  physics
■650  4▼aOptics
■653    ▼aMicroscopy
■653    ▼aSemiconductors
■653    ▼aCoherent  multidimensional  spectroscopy
■653    ▼aTransition  metal  dichalcogenide
■653    ▼aSum  frequency  generation
■690    ▼a0494
■690    ▼a0611
■690    ▼a0752
■71020▼aThe  University  of  Wisconsin  -  Madison▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g86-02B.
■790    ▼a0262
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163988▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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