자료유형  

 학위논문

Control Number  

0017164181

International Standard Book Number  

9798346858324

Dewey Decimal Classification Number  

540

Main Entry-Personal Name  

O'Connor, James Patrick.

Publication, Distribution, etc. (Imprint  

[S.l.] : Northwestern University., 2024

Publication, Distribution, etc. (Imprint  

Ann Arbor : ProQuest Dissertations & Theses, 2024

Physical Description  

326 p.

General Note  

Source: Dissertations Abstracts International, Volume: 86-06, Section: B.

General Note  

Advisor: Wasielewski, Michael R.

Dissertation Note  

Thesis (Ph.D.)--Northwestern University, 2024.

Summary, Etc.  

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.

Subject Added Entry-Topical Term  

Chemistry.

Subject Added Entry-Topical Term  

Physical chemistry.

Subject Added Entry-Topical Term  

Organic chemistry.

Index Term-Uncontrolled  

Quantum information

Index Term-Uncontrolled  

Two-dimensional electronic spectroscopy

Index Term-Uncontrolled  

Julolidine-BODIPY

Index Term-Uncontrolled  

Crystalline materials

Added Entry-Corporate Name  

Northwestern University Chemistry

Host Item Entry  

Dissertations Abstracts International. 86-06B.

Electronic Location and Access  

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Control Number  

joongbu:653888