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Classical and Quantum Effects in Plasmonic Metals

Citation

Brown, Ana Maii (2016) Classical and Quantum Effects in Plasmonic Metals. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/Z9QV3JHT. http://resolver.caltech.edu/CaltechTHESIS:04242016-093536420

Abstract

The field of plasmonics exploits the unique optical properties of metallic nanostructures to concentrate and manipulate light at subwavelength length scales. Metallic nanostructures get their unique properties from their ability to support surface plasmons– coherent wave-like oscillations of the free electrons at the interface between a conductive and dielectric medium. Recent advancements in the ability to fabricate metallic nanostructures with subwavelength length scales have created new possibilities in technology and research in a broad range of applications.

In the first part of this thesis, we present two investigations of the relationship between the charge state and optical state of plasmonic metal nanoparticles. Using experimental bias-dependent extinction measurements, we derive a potential- dependent dielectric function for Au nanoparticles that accounts for changes in the physical properties due to an applied bias that contribute to the optical extinction. We also present theory and experiment for the reverse effect– the manipulation of the carrier density of Au nanoparticles via controlled optical excitation. This plasmoelectric effect takes advantage of the strong resonant properties of plasmonic materials and the relationship between charge state and optical properties to eluci- date a new avenue for conversion of optical power to electrical potential.

The second topic of this thesis is the non-radiative decay of plasmons to a hot-carrier distribution, and the distribution’s subsequent relaxation. We present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. We also preform ab initio calculations of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We extend these first-principle methods to calculate the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions. Finally, we combine these first-principles calculations of carrier dynamics and optical response to produce a complete theoretical description of ultrafast pump-probe measurements, free of any fitting parameters that are typical in previous analyses.

Item Type:Thesis (Dissertation (Ph.D.))
Subject Keywords:Plasmonics
Degree Grantor:California Institute of Technology
Division:Engineering and Applied Science
Major Option:Applied Physics
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Atwater, Harry Albert
Thesis Committee:
  • Vahala, Kerry J. (chair)
  • Minnich, Austin J.
  • Faraon, Andrei
  • Atwater, Harry Albert
Defense Date:20 April 2016
Funders:
Funding AgencyGrant Number
NSFUNSPECIFIED
Link Energy FoundationUNSPECIFIED
DOE ‘Light-Material Interactions in Energy Conversion’ Energy Frontier Research CenterDE- SC0001293
Record Number:CaltechTHESIS:04242016-093536420
Persistent URL:http://resolver.caltech.edu/CaltechTHESIS:04242016-093536420
DOI:10.7907/Z9QV3JHT
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1126/science.1258405DOIArticle adapted for Ch. 1
http://dx.doi.org/10.1021/ph500358qDOIArticle adapted for Ch. 2
http://dx.doi.org/10.1021/acsnano.5b06199DOIArticle adapted for Ch. 3
ORCID:
AuthorORCID
Brown, Ana Maii0000-0003-3008-2310
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:9684
Collection:CaltechTHESIS
Deposited By: Ana Brown
Deposited On:10 May 2016 19:43
Last Modified:26 Oct 2016 20:46

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