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Investigating the Underlying Factors of Excited-State Dynamics in Model Organic Chromophore Systems Using Ultrafast Spectroscopy
Investigating the Underlying Factors of Excited-State Dynamics in Model Organic Chromophore Systems Using Ultrafast Spectroscopy
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152840
- ISBN
- 9798346858324
- DDC
- 540
- 서명/저자
- Investigating the Underlying Factors of Excited-State Dynamics in Model Organic Chromophore Systems Using Ultrafast Spectroscopy
- 발행사항
- [Sl] : Northwestern University, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 326 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-06, Section: B.
- 주기사항
- Advisor: Wasielewski, Michael R.
- 학위논문주기
- Thesis (Ph.D.)--Northwestern University, 2024.
- 초록/해제
- 요약Understanding the various forces that drive electron dynamics following photoexcitation is of high interest to the fields of solar energy and quantum information. Here, these drivers are disentangled and then further related to each other using spectroscopic experiments aimed at studying the underlying physical principles that exist within settings where real-world applications are expected to take place. By utilizing two-dimensional electronic spectroscopy (2DES) to study the excited state evolution of carefully designed organic chromophore systems, the ultrafast sub-ps time dynamics can be probed to inform on the contexts that govern electronic, vibrational, and vibronic couplings.Fluctuations in temperature and solvation media are found to have major controllable effects on the electronic pathway of a photoexcited spiro-fused terrylene-3,4:11,12-bis(dicarboximide) (TDI) dimer (sTDI2), where imposed structural rigidity afforded study of how external environment changes independently affect photophysics. A subsequent study on a simplified julolidine-BODIPY (Jul-BD) donor-acceptor system elevated these findings by elucidating the effect of intramolecular twisting and compression on electron transfer characteristics, outlining synthetic design parameters to inhibit or favor certain vibrational motions in pursuit of targeted responses. The asymmetry of molecular interfaces - known to persist in virtually all practical device settings - was investigated via a perylene-perylenediimide-perylenediimide (PerPDI2) slip-stacked donor-acceptor-acceptor system. Results show even minor changes in chromophore solvation and chromophore π-stacking have major effects on excited-state dynamics. Finally, the assumption that any one principle can dictate photophysics alone was challenged through study of cofacial PDI dimer systems with either 1,7-bis(pyrrolidin-1'-yl) (5PDI2) or bis-1,7-(3',5'-di-t-butylphenoxy) substituents (PPDI2) at the bay positions. Herein, a convolution of multiple underlying factors is demonstrated to affect the energetic properties of the systems, mirroring real-world contexts.To better parse out the forces that drive photoexcitation and subsequent energetic evolution, several alterations were carried out to improve the capabilities of a 2DES instrument. Pump capabilities were enhanced by construction and incorporation of a water flow cell apparatus to generate supercontinuum pulses extending from the near ultraviolet to near infrared spectral ranges. Integration of a microscope into the 2DES setup extended its experimental reach into the solid state, where the ordering of crystalline materials offers great insights.
- 일반주제명
- Chemistry
- 일반주제명
- Physical chemistry
- 일반주제명
- Organic chemistry
- 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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■006m o d
■007cr#unu||||||||
■020 ▼a9798346858324
■035 ▼a(MiAaPQ)AAI31562656
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a540
■1001 ▼aO'Connor, James Patrick.▼0(orcid)0000-0002-8586-9842
■24510▼aInvestigating the Underlying Factors of Excited-State Dynamics in Model Organic Chromophore Systems Using Ultrafast Spectroscopy
■260 ▼a[Sl]▼bNorthwestern University▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a326 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-06, Section: B.
■500 ▼aAdvisor: Wasielewski, Michael R.
■5021 ▼aThesis (Ph.D.)--Northwestern University, 2024.
■520 ▼aUnderstanding the various forces that drive electron dynamics following photoexcitation is of high interest to the fields of solar energy and quantum information. Here, these drivers are disentangled and then further related to each other using spectroscopic experiments aimed at studying the underlying physical principles that exist within settings where real-world applications are expected to take place. By utilizing two-dimensional electronic spectroscopy (2DES) to study the excited state evolution of carefully designed organic chromophore systems, the ultrafast sub-ps time dynamics can be probed to inform on the contexts that govern electronic, vibrational, and vibronic couplings.Fluctuations in temperature and solvation media are found to have major controllable effects on the electronic pathway of a photoexcited spiro-fused terrylene-3,4:11,12-bis(dicarboximide) (TDI) dimer (sTDI2), where imposed structural rigidity afforded study of how external environment changes independently affect photophysics. A subsequent study on a simplified julolidine-BODIPY (Jul-BD) donor-acceptor system elevated these findings by elucidating the effect of intramolecular twisting and compression on electron transfer characteristics, outlining synthetic design parameters to inhibit or favor certain vibrational motions in pursuit of targeted responses. The asymmetry of molecular interfaces - known to persist in virtually all practical device settings - was investigated via a perylene-perylenediimide-perylenediimide (PerPDI2) slip-stacked donor-acceptor-acceptor system. Results show even minor changes in chromophore solvation and chromophore π-stacking have major effects on excited-state dynamics. Finally, the assumption that any one principle can dictate photophysics alone was challenged through study of cofacial PDI dimer systems with either 1,7-bis(pyrrolidin-1'-yl) (5PDI2) or bis-1,7-(3',5'-di-t-butylphenoxy) substituents (PPDI2) at the bay positions. Herein, a convolution of multiple underlying factors is demonstrated to affect the energetic properties of the systems, mirroring real-world contexts.To better parse out the forces that drive photoexcitation and subsequent energetic evolution, several alterations were carried out to improve the capabilities of a 2DES instrument. Pump capabilities were enhanced by construction and incorporation of a water flow cell apparatus to generate supercontinuum pulses extending from the near ultraviolet to near infrared spectral ranges. Integration of a microscope into the 2DES setup extended its experimental reach into the solid state, where the ordering of crystalline materials offers great insights.
■590 ▼aSchool code: 0163.
■650 4▼aChemistry
■650 4▼aPhysical chemistry
■650 4▼aOrganic chemistry
■653 ▼aQuantum information
■653 ▼aTwo-dimensional electronic spectroscopy
■653 ▼aJulolidine-BODIPY
■653 ▼aCrystalline materials
■690 ▼a0485
■690 ▼a0494
■690 ▼a0490
■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=T17164181▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
