Super-resolution lifetime imaging of single molecules surrounding gold bowtie nanoparticles
Loading...
Authors
Hallenbeck, Zachary
Issue Date
2022-05
Type
Electronic thesis
Thesis
Thesis
Language
en_US
Keywords
Physics
Alternative Title
Abstract
Interactions between light and matter serve as the basis of many of the technologies weuse, whether it be photon absorption, emission, or other transfers of energy. The quality of these
devices is thus inherently limited by the optical properties of their constituents, which are regularly
quite lacking in efficiency. Plasmonic nanoparticles serve as a highly versatile and tunable
platform for the enhancement of such optical properties when one of these optical transitions
occurs in their near-field. However, the near-field nature of these effects has made thorough study
and understanding of these mechanisms difficult. Particularly, a study of molecular decay rate
enhancement in resonant plasmonic environments on this length scale has only recently been
performed, and with limitations on efficiency and resolution. In this dissertation, I describe a new
technique that combines super-resolution microscopy with fluorescence lifetime imaging
microscopy (FLIM) to study single-molecule decay rate enhancement in a single-measurement,
with spatial resolution on the order of 10 nm. Additionally, in the same measurement, we verify
the validity of this technique using autocorrelation to confirm that our data indeed originates from
individual molecules, avoiding ensemble averaging. This thesis provides further insight into the
various mechanisms of plasmon-enhanced emission, decoupled from absorption enhancement,
providing a platform for further study of emission mislocalization and the position-dependent
prominence of different decay pathways.
Description
May 2022
School of Science
School of Science
Full Citation
Publisher
Rensselaer Polytechnic Institute, Troy, NY