Nanoparticle probes based on metal carbonyl chemical species for biological sensing with infrared spectroscopy

The development of probes that enable the measurement of target molecular species with high specificity is essential to studying complex biological systems. Bright, non-interfering, and easily distinguishable labels for infrared spectroscopies are necessary to perform more advanced studies using these techniques. This dissertation examines the rational design, synthesis, characterization, and application of candidate IR probes, IR emitting Quantum Dots and metal carbonyl-based probes for infrared micro spectroscopy. Our results suggest that these probes enable infrared spectroscopy with biomolecular specificity. The use of probes for infrared spectroscopy is an emerging area of research and the development of bright, compact, and non-interfering probes is needed for further advancement in the field. Transition metal carbonyls are organometallic compounds consisting of carbon monoxide moieties coordinated to a metal center. Their large infrared cross-sections and non-interference with infrared spectroscopy of functional groups of biological materials make them an ideal candidate as probes for vibrational spectroscopy. Through the work described in this dissertation, their utility for vibrational spectroscopic imaging has been further expanded. Probes composed of a polymeric nanoparticle impregnated with transition metal carbonyls were employed because they localize large numbers of carbonyl functional groups to the nanoparticle interior and provide surface sites for chemical modification and attachment of targeting molecules.These properties have led to their applications in bio-imaging and -sensing, in particular through Raman, surface-enhanced Raman spectroscopy (SERS) and more recently Infrared spectroscopic imaging. The emerging use of affinity-based probes for vibrational spectroscopies has spurred the need for probes with strong absorption cross sections and with signatures that lie outside of biologically significant spectral windows. We report on the formation of an IR nanoprobe comprised of a polymeric nanoparticle doped with a metal carbonyl species using a tractable swelling and diffusion process that meets these requirements for the development of probes for IR microscopy.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Bioengineering

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2023

Author dc:creator

• Richard, Craig A.

Contributors dc:contributor

• Bhargava, Rohit
• Smith, Andrew
• Irudayaraj, Joseph
• Nie, Shuming

• Infrared Nanoprobe
• Metal Carbonyl
• Nanoparticle
• Infrared Spectroscopic Imaging

Statement dc:rights

• Copyright 2023 Craig Richard

Language dc:language

en, eng

Handle dc:identifier

https://hdl.handle.net/2142/121996

OAI record oai:identifier

https://www.ideals.illinois.edu/oai-pmh?verb=GetRecord&metadataPrefix=etdms&identifier=oai%3Awww.ideals.illinois.edu%3A2142%2F121996