Spatially and Temporally Resolved Spectroscopy of Transition Metal Dichalcogenide Semiconductors
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
- 기타저자
- The University of Wisconsin - Madison Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-02B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■006m o d
■007cr#unu||||||||
■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.


