Publications

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Spectral linewidths are used to assess a variety of physical properties, even as spectral overlap makes quantitative extraction difficult owing to uncertainty. Uncertainty, in turn, can be minimized with the choice of appropriate experimental conditions used in spectral collection. In response, we assess the experimental factors dictating uncertainty in the quantification of linewidth from a Raman experiment highlighting the comparative influence of (1) spectral resolution, (2) signal to noise, and (3) relative peak intensity (RPI) of the overlapping peaks. Practically, Raman spectra of SiGe thin films were obtained experimentally and simulated virtually under a variety of conditions. RPI is found to be the most impactful parameter in specifying linewidth followed by the spectral resolution and signal to noise. While developed for Raman experiments, the results are generally applicable to spectroscopic linewidth studies illuminating the experimental trade-offs inherent in quantification.

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We study semiconductor hyperbolic metamaterials (SHMs) at the quantum limit experimentally using spectroscopic ellipsometry as well as theoretically using a new microscopic theory. The theory is a combination of microscopic density matrix approach for the material response and Green’s function approach for the propagating electric field. Our approach predicts absorptivity of the full multilayer system and for the first time allows the prediction of in-plane and out-of-plane dielectric functions for every individual layer constructing the SHM as well as effective dielectric functions that can be used to describe a homogenized SHM.

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We experimentally demonstrated an actively tunable optical filter that controls the amplitude of reflected long-wave-infrared light in two separate spectral regions concurrently. Our device exploits the dependence of the excitation energy of plasmons in a continuous and unpatterned sheet of graphene on the Fermi-level, which can be controlled via conventional electrostatic gating. The filter enables simultaneous modification of two distinct spectral bands whose positions are dictated by the device geometry and graphene plasmon dispersion. Within these bands, the reflected amplitude can be varied by over 15% and resonance positions can be shifted by over 90 cm-1. Electromagnetic simulations verify that tuning arises through coupling of incident light to graphene plasmons by a grating structure. Importantly, the tunable range is determined by a combination of graphene properties, device structure, and the surrounding dielectrics, which dictate the plasmon dispersion. Thus, the underlying design shown here isapplicable across a broad range of infrared frequencies.

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In situ Raman microscopy was used to study polysulfide speciation in the bulk ether electrolyte during the discharge and charge of a Li-S electrochemical cell to assess the complex interplay between chemical and electrochemical reactions in solution. During discharge, long chain polysulfides and the S₃^- radical appear in the electrolyte at 2.4 V indicating a rapid equilibrium of the dissociation reaction to form S₃^-. When charging, however, an increase in the concentration of all polysulfide species was observed. This highlights the importance of the electrolyte to sulfur ratio and suggests a loss in the useful sulfur inventory from the cathode to the electrolyte.