Controlling the Environmental Sensitivity of Small Molecule Fluorophores for Cellular Imaging
Open Access
- Author:
- Hoelzel, Conner
- Graduate Program:
- Chemistry
- Degree:
- Doctor of Philosophy
- Document Type:
- Dissertation
- Date of Defense:
- March 31, 2021
- Committee Members:
- Xin Zhang, Dissertation Advisor/Co-Advisor
Xin Zhang, Committee Chair/Co-Chair
Emily E Weinert, Outside Member
Elizabeth A Elacqua, Committee Member
Squire J Booker, Committee Member
Philip C Bevilacqua, Program Head/Chair - Keywords:
- fluorescence
solvatochromism
brightness
excited state
non-radiative decay
internal conversion
external conversion
twisted intramolecular charge transfer
rhodamine
proteostasis
cell imaging
protein misfolding
aggregation
neurodegenerative disease
microscopy - Abstract:
- The spatiotemporal information derived from the employment of small molecule, organic fluorophores has made their employment in the chemical and biological sciences nearly ubiquitous. Small molecule fluorophores commonly exhibit an environmental sensitive behavior, with differences in emission properties arising from changes in the polarity of the local microenvironment. This phenomenon, known as solvatochromism, can act both deleteriously by attenuating fluorescent signal and beneficially to differentiate between the physicochemical properties of separate localities in a heterogeneous system. To this end, this report details efforts to understand and control the excited state dynamics of these dyes in order to produce more effective and more functional probes for the purpose of cellular imaging. We address this objective through three individual aims: 1) control excited state dynamics to mitigate the deleterious effects of solvatochromism, 2) understand mechanistic origins of environmental sensitivity in non-canonical platforms, 3) apply solvent-dependent photophysical and chemical properties of small molecule fluorophores towards the development of novel imaging methodologies.