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Exploring the Interplay of Structure and Electronic Dynamics in Bimetallic Platinum Complexes
Exploring the Interplay of Structure and Electronic Dynamics in Bimetallic Platinum Complexes
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152839
- ISBN
- 9798346858171
- DDC
- 541
- 서명/저자
- Exploring the Interplay of Structure and Electronic Dynamics in Bimetallic Platinum Complexes
- 발행사항
- [Sl] : Northwestern University, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 230 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-06, Section: B.
- 주기사항
- Advisor: Chen, Lin X.
- 학위논문주기
- Thesis (Ph.D.)--Northwestern University, 2024.
- 초록/해제
- 요약To better engineer molecules for ideal photochemical outcomes, we require a deeper understanding of how nuclear parameters such as structure and quantum mechanical vibrations impact electronic behavior. This dissertation aims to further our understanding of these parameters through use of a tunable platinum(II) dimeric framework and a combination of ultrafast optical and x-ray spectroscopic techniques.Chapter 3 utilizes X-ray Transient Absorption (XTA) to track transient bond formation between the Pt(II) dimer centers or lack thereof. The study incorporates optical transient absorption (OTA) to track the excited state dynamics of the two systems studied and provide a correlation between optical and X-ray observations. This study provided the first structural evidence of the lack of Pt-Pt bond formation in the charge transfer band of a Pt(II) dimer with sufficiently separated metal centers while confirming the oxidation of the Pt(II) centers.Chapter 4 examines the nuclear wave packet dynamics along the Pt-Pt mode in a Pt(II) dimer donor acceptor complex using ultrafast transient x-ray solution scattering (TRXSS) to give a purely nuclear picture to the vibration and the bond contraction. This is supplemented with OTA to detail the excited electronic states of the complex. This study shows that Pt-Pt contraction is sufficiently slow enough to potentially modulate the rate of electron transfer during the contraction, as the transient bond formation moves the Pt centers closer together thus possibly altering the energy of the electronic states and the electron transfer driving force.Chapter 5 is a study of the electron transfer (ET) dynamics in two different Pt(II) dimer donor acceptors. Utilizing OTA, this study shows that the Pt(II) dimer offers a framework in which the optically resonant MLCT transitions can be tuned by bridge group bulkiness without altering ET dynamics. Chapter 6 utilizes broadband transient absorption (BBTA) two-dimensional electronic spectroscopy (2DES) to probe vibronic wave packets in the Pt(II) dimers. This study showed a unique result of decoherence and subsequent recoherence of the Pt-Pt stretching mode as the system undergoes intersystem crossing (ISC), shedding new light on the processes of spin-vibronic coupling through a short-lived intermediate triplet state en route to the lowest energy triplet state.
- 일반주제명
- Physical chemistry
- 일반주제명
- Materials science
- 일반주제명
- Optics
- 일반주제명
- Analytical chemistry
- 키워드
- Spectroscopy
- 키워드
- Platinum
- 기타저자
- Northwestern University Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-06B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520250211152839
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■007cr#unu||||||||
■020 ▼a9798346858171
■035 ▼a(MiAaPQ)AAI31562157
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a541
■1001 ▼aWeingartz, Nicholas P.▼0(orcid)0000-0002-1486-2918
■24510▼aExploring the Interplay of Structure and Electronic Dynamics in Bimetallic Platinum Complexes
■260 ▼a[Sl]▼bNorthwestern University▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a230 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-06, Section: B.
■500 ▼aAdvisor: Chen, Lin X.
■5021 ▼aThesis (Ph.D.)--Northwestern University, 2024.
■520 ▼aTo better engineer molecules for ideal photochemical outcomes, we require a deeper understanding of how nuclear parameters such as structure and quantum mechanical vibrations impact electronic behavior. This dissertation aims to further our understanding of these parameters through use of a tunable platinum(II) dimeric framework and a combination of ultrafast optical and x-ray spectroscopic techniques.Chapter 3 utilizes X-ray Transient Absorption (XTA) to track transient bond formation between the Pt(II) dimer centers or lack thereof. The study incorporates optical transient absorption (OTA) to track the excited state dynamics of the two systems studied and provide a correlation between optical and X-ray observations. This study provided the first structural evidence of the lack of Pt-Pt bond formation in the charge transfer band of a Pt(II) dimer with sufficiently separated metal centers while confirming the oxidation of the Pt(II) centers.Chapter 4 examines the nuclear wave packet dynamics along the Pt-Pt mode in a Pt(II) dimer donor acceptor complex using ultrafast transient x-ray solution scattering (TRXSS) to give a purely nuclear picture to the vibration and the bond contraction. This is supplemented with OTA to detail the excited electronic states of the complex. This study shows that Pt-Pt contraction is sufficiently slow enough to potentially modulate the rate of electron transfer during the contraction, as the transient bond formation moves the Pt centers closer together thus possibly altering the energy of the electronic states and the electron transfer driving force.Chapter 5 is a study of the electron transfer (ET) dynamics in two different Pt(II) dimer donor acceptors. Utilizing OTA, this study shows that the Pt(II) dimer offers a framework in which the optically resonant MLCT transitions can be tuned by bridge group bulkiness without altering ET dynamics. Chapter 6 utilizes broadband transient absorption (BBTA) two-dimensional electronic spectroscopy (2DES) to probe vibronic wave packets in the Pt(II) dimers. This study showed a unique result of decoherence and subsequent recoherence of the Pt-Pt stretching mode as the system undergoes intersystem crossing (ISC), shedding new light on the processes of spin-vibronic coupling through a short-lived intermediate triplet state en route to the lowest energy triplet state.
■590 ▼aSchool code: 0163.
■650 4▼aPhysical chemistry
■650 4▼aMaterials science
■650 4▼aOptics
■650 4▼aAnalytical chemistry
■653 ▼aSpectroscopy
■653 ▼aTransition metal complexes
■653 ▼aElectron transfer
■653 ▼aOptical transient absorption
■653 ▼aPlatinum
■690 ▼a0494
■690 ▼a0752
■690 ▼a0794
■690 ▼a0486
■71020▼aNorthwestern University▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g86-06B.
■790 ▼a0163
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17164168▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
