Henry O. Everitt

Aluminum for Plasmonics

Unlike silver and gold, aluminum has material properties that enable strong plasmon resonances spanning much of the visible region of the spectrum and into the ultraviolet. This extended response, combined with its natural abundance, low cost, and amenability to manufacturing processes, makes aluminum a highly promising material for commercial applications. Fabricating Al-based nanostructures whose optical properties correspond with theoretical predictions, however, can be a challenge. In this work, the Al plasmon resonance is observed to be remarkably sensitive to the presence of oxide within the metal. For Al nanodisks, we observe that the energy of the plasmon resonance is determined by, and serves as an optical reporter of, the percentage of oxide present within the Al. This understanding paves the way toward the use of aluminum as a low-cost plasmonic material with properties and potential applications similar to those of the coinage metals.

Aluminum Plasmonic Nanoantennas

The use of aluminum for plasmonic nanostructures opens up new possibilities, such as access to short-wavelength regions of the spectrum, complementary metal-oxide-semiconductor (CMOS) compatibility, and the possibility of low-cost, sustainable, mass-producible plasmonic materials. Here we examine the properties of individual Al nanorod antennas with cathodoluminescence (CL). This approach allows us to image the local density of optical states (LDOS) of Al nanorod antennas with a spatial resolution less than 20 nm and to identify the radiative modes of these nanostructures across the visible and into the UV spectral range. The results, which agree well with finite difference time domain (FDTD) simulations, lay the groundwork for precise Al plasmonic nanostructure design for a variety of applications.

Enhancement of spontaneous recombination rate in a quantum well by resonant surface plasmon coupling

Using time-resolved photoluminescence measurements, the recombination rate in an

Refractive indices and absorption coefficients of MgxZn1−xO alloys

{\mathrm{In}}_{0.18}{\mathrm{Ga}}_{0.82}\mathrm{N}/\mathrm{GaN}

Stimulated emission and time-resolved photoluminescence in rf-sputtered ZnO thin films

quantum well (QW) is shown to be greatly enhanced when spontaneous emission is resonantly coupled to a silver surface plasmon. The rate of enhanced spontaneous emission into the surface plasmon was as much as 92 times faster than QW spontaneous emission into free space. A calculation, based on Fermis golden rule, reveals that the enhancement is very sensitive to silver thickness and indicates even greater enhancements are possible for QWs placed closer to the surface metal coating.

Aluminum Nanocrystals as a Plasmonic Photocatalyst for Hydrogen Dissociation

Indices of refraction for MgxZn1−xO epitaxial films grown by pulsed-laser deposition on sapphire substrates with x up to 0.36 were determined in the range of wavelength 457–968 nm by analysis of optical transmission spectra and prism-coupled waveguide measurements. The dispersion follows the first-order Sellmeier dispersion equation. Absorption coefficients, exciton energy gaps, and binding energies of MgxZn1−xO alloys were determined by transmission spectroscopy. The excitonic absorption features were clearly visible at room temperature despite alloy broadening. These results provide important information for the design and modeling of ZnO/MgZnO heterostructure optoelectronic devices.

Fano Resonant Aluminum Nanoclusters for Plasmonic Colorimetric Sensing

Stimulated emission (SE) was measured from ZnO thin films grown on c-plane sapphire by rf sputtering. Free exciton transitions were clearly observed at 10 K in the photoluminescence (PL), transmission, and reflection spectra of the sample annealed at 950 °C. SE resulting from both exciton-exciton scattering and electron hole plasma formation was observed in the annealed samples at moderate excitation energy densities. The SE threshold energy density decreased with increasing annealing temperature up to ∼950 °C. The observation of low threshold exciton-exciton scattering-induced SE showed that excitonic laser action could be obtained in rf-sputtered ZnO thin films. At excitation densities below the SE threshold, time-resolved PL revealed very fast recombination times of ∼74 ps at room temperature, and no significant change at 85 K. The decay time for the SE-induced PL was below the system resolution of <45 ps.

Shallow acceptor complexes in p-type ZnO

Hydrogen dissociation is a critical step in many hydrogenation reactions central to industrial chemical production and pollutant removal. This step typically utilizes the favorable band structure of precious metal catalysts like platinum and palladium to achieve high efficiency under mild conditions. Here we demonstrate that aluminum nanocrystals (Al NCs), when illuminated, can be used as a photocatalyst for hydrogen dissociation at room temperature and atmospheric pressure, despite the high activation barrier toward hydrogen adsorption and dissociation. We show that hot electron transfer from Al NCs to the antibonding orbitals of hydrogen molecules facilitates their dissociation. Hot electrons generated from surface plasmon decay and from direct photoexcitation of the interband transitions of Al both contribute to this process. Our results pave the way for the use of aluminum, an earth-abundant, nonprecious metal, for photocatalysis.

Shape matters: plasmonic nanoparticle shape enhances interaction with dielectric substrate.

Aluminum is an abundant and high-quality material for plasmonics with potential for large-area, low-cost photonic technologies. Here we examine aluminum nanoclusters with plasmonic Fano resonances that can be tuned from the near-UV into the visible region of the spectrum. These nanoclusters can be designed with specific chromaticities in the blue-green region of the spectrum and exhibit a remarkable spectral sensitivity to changes in the local dielectric environment. We show that such structures can be used quite generally for colorimetric localized surface plasmon resonance (LSPR) sensing, where the presence of analytes is detected by directly observable color changes rather than through photodetectors and spectral analyzers. To quantify our results and provide a metric for optimization of such structures for colorimetric LSPR sensing, we introduce a figure of merit based on the color perception ability of the human eye.

Ordinary and extraordinary refractive indices for AlxGa1−xN epitaxial layers

We show that N-doped ZnO films grown on sapphire can exhibit significant (∼1018 cm−3) room-temperature p-type behavior when sufficient nitrogen (N) is incorporated and the material is annealed appropriately. Substitutional N on the oxygen (O) sublattice is a deep acceptor; however, shallow acceptor complexes involve N, H, and zinc vacancies (VZn). Combining secondary ion mass spectrometry, Raman-scattering, photoluminescence, and Hall-effect data, we establish the evolution of N from its initial incorporation on a Zn site to a final shallow acceptor complex VZn_NO_H+ with an ionization energy of ca. 130 meV. This complex is responsible for the observed p-type behavior.