Gan, Xing Yee
(2021)
Understanding the Emergence, Tunability, and Performance of Plasmonic Copper Selenide Semiconductor Nanoparticles.
Doctoral Dissertation, University of Pittsburgh.
(Unpublished)
Abstract
The phenomena of localized surface plasmon resonances (LSPRs) has been broadly studied and is a property of nanomaterials that can be used to enhance or enable a wide variety of technologies including cancer treatment, light-driven catalysis, and ultrasensitive detection. While most widely-observed and studied in noble metal nanomaterials, there is significant interest in earth-abundant plasmonic materials. However, whether or not their performance can match or even surpass their noble metal counterparts remains to be established. An important first step in determining the extent of their versatility is to understand basic aspects of their plasmonic features. We first synthesize and demonstrate the LSPR energy tunability of air-stable degenerately doped copper selenide (Cu2Se) NPs (Chapter 2.0). We quantitatively access the LSPR and correlate its spectral features with changes in the nanoparticle structure that can be controlled chemically. Our next step is to understand the surface chemistry of Cu2Se NPs, which clarifies the site of potential catalytic behavior (Chapter 3.0). We then establish their molar extinction coefficient, which is an important readout for the LSPR intensity and showcases our ability to control such intensity with NP size (Chapter 4.0). Importantly, we determine that size-dependent increases in molar extinction coefficients behave much like their noble metal analogues, as the trend mimics the Mie theory predictions. In Chapter 5.0, we demonstrate the first plasmon-driven chemical conversion on the surface of this new plasmonic material class. Finally, we establish a reaction-insensitive, material-specific design rule to prepare multicomponent nanostructures starting from Cu2Se (Chapter 6.0). Taken together, these results give a promising outlook towards rational designs and implementations of technology-relevant and earth-abundant materials.
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Details
| Item Type: |
University of Pittsburgh ETD
|
| Status: |
Unpublished |
| Creators/Authors: |
|
| ETD Committee: |
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| Date: |
3 May 2021 |
| Date Type: |
Publication |
| Defense Date: |
25 March 2021 |
| Approval Date: |
3 May 2021 |
| Submission Date: |
22 February 2021 |
| Access Restriction: |
2 year -- Restrict access to University of Pittsburgh for a period of 2 years. |
| Number of Pages: |
275 |
| Institution: |
University of Pittsburgh |
| Schools and Programs: |
Dietrich School of Arts and Sciences > Chemistry |
| Degree: |
PhD - Doctor of Philosophy |
| Thesis Type: |
Doctoral Dissertation |
| Refereed: |
Yes |
| Uncontrolled Keywords: |
localized surface plasmon resonance, nanomaterials, chemistry, degenerately-doped semiconductor nanoparticles |
| Date Deposited: |
03 May 2021 14:42 |
| Last Modified: |
03 May 2023 05:15 |
| URI: |
http://d-scholarship.pitt.edu/id/eprint/40283 |
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