Tyler Roschuk

Controlling Light Localization and Light-Matter Interactions with Nanoplasmonics

Nanoplasmonics is the emerging research field that studies light-matter interactions mediated by resonant excitations of surface plasmons in metallic nanostructures. It allows the manipulation of the flow of light and its interaction with matter at the nanoscale (10(-9) m). One of the most promising characteristics of plasmonic resonances is that they occur at frequencies corresponding to typical electronic excitations in matter. This leads to the appearance of strong interactions between localized surface plasmons and light emitters (such as molecules, dyes, or quantum dots) placed in the vicinity of metals. Recent advances in nanofabrication and the development of novel concepts in theoretical nanophotonics have opened the way to the design of structures aimed to reduce the lifetime and enhance the decay rate and quantum efficiency of available emitters. In this article, some of the most relevant experimental and theoretical achievements accomplished over the last several years are presented and analyzed.

X-ray-diffraction study of crystalline Si nanocluster formation in annealed silicon-rich silicon oxides

The formation and subsequent growth of crystalline silicon nanoclusters (Si-ncs) in annealed silicon-rich silicon oxides (SRSOs) were studied by glancing angle x-ray diffraction. SRSO samples with Si concentrations (y) of 0.40, 0.42, and 0.45 were grown by inductively coupled plasma-enhanced chemical-vapor deposition (PECVD). Samples with y=0.42 grown by electron-cyclotron-resonance PECVD were also studied. Annealing treatments were performed at temperatures (T) of 900, 1000, and 1100 °C for times (t) between 0.5 and 3 h in flowing Ar. As-grown SRSO films did not present signs of Si clusters (amorphous or crystalline); however, (111), (220), and (311) Bragg peaks corresponding to c‐Si were clearly seen after annealing at 900 °C for the y=0.45 sample, but only barely seen for the y=0.42 and undetected for the y=0.40 samples. For T=1000°C, all studied SRSO samples clearly showed the c‐Si diffraction peaks, which became narrower with increasing t and T. From the width of the Si (111) peaks, the mean size of ...

High-order harmonic generation in graphite plasma plumes using ultrashort laser pulses: a systematic analysis of harmonic radiation and plasma conditions

High-order harmonic generation in graphite-ablated plasmas was systematically studied using ultrashort (3.5 and 30 fs) laser pulses. We observed the efficient frequency conversion of 3.5 fs Ti:sapphire laser pulses in the range of 15-26 eV. Stabilization of the harmonic yield at a 1 kHz pulse repetition rate was accomplished using a rotating graphite target. We also show the results of harmonic generation in carbon plasma using 1300 nm, 40 ps pulses, which allowed the extension of the harmonic cutoff while maintaining a comparable conversion efficiency to the case of 780 nm driving radiation. The time-of-flight mass spectrometric analysis of the plasma components and the scanning electron microscopy of plasma debris under optimal conditions for harmonic generation suggest the presence of small carbon clusters (C10-C30 )i n the plasma plume at the moment of femtosecond pulse propagation, which further aggregate on nearby substrates. We present the results of plasma spectroscopy obtained under unoptimized plasma conditions that elucidate the reduction in harmonic signal. We also present calculations of plasma concentration under different excitation conditions of the ablated graphite target. (Some figures may appear in colour only in the online journal)

The formation of light emitting cerium silicates in cerium-doped silicon oxides

Cerium-doped silicon oxides with cerium concentrations of up to 0.9 at. % were deposited by electron cyclotron resonance plasma enhanced chemical vapor deposition. Bright cerium related photoluminescence, easily seen even under room lighting conditions, was observed from the films and found to be sensitive to film composition and annealing temperature. The film containing 0.9 at. % Ce subjected to anneal in N2 at 1200 °C for 3 h showed the most intense cerium-related emission, easily visible under bright room lighting conditions. This is attributed to the formation of cerium silicate [Ce2Si2O7 or Ce4.667 (SiO4)3O], the presence of which was confirmed by high resolution transmission electron microscopy.

Precise attoliter temperature control of nanopore sensors using a nanoplasmonic bullseye.

Targeted temperature control in nanopores is greatly important in further understanding biological molecules. Such control would extend the range of examinable molecules and facilitate advanced analysis, including the characterization of temperature-dependent molecule conformations. The work presented within details well-defined plasmonic gold bullseye and silicon nitride nanopore membranes. The bullseye nanoantennae are designed and optimized using simulations and theoretical calculations for interaction with 632.8 nm laser light. Laser heating was monitored experimentally through nanopore conductance measurements. The precise heating of nanopores is demonstrated while minimizing the accumulation of heat in the surrounding membrane material.

Plasmon-Induced Optical Anisotropy in Hybrid Graphene–Metal Nanoparticle Systems

Hybrid plasmonic metal-graphene systems are emerging as a class of optical metamaterials that facilitate strong light-matter interactions and are of potential importance for hot carrier graphene-based light harvesting and active plasmonic applications. Here we use femtosecond pump-probe measurements to study the near-field interaction between graphene and plasmonic gold nanodisk resonators. By selectively probing the plasmon-induced hot carrier dynamics in samples with tailored graphene-gold interfaces, we show that plasmon-induced hot carrier generation in the graphene is dominated by direct photoexcitation with minimal contribution from charge transfer from the gold. The strong near-field interaction manifests as an unexpected and long-lived extrinsic optical anisotropy. The observations are explained by the action of highly localized plasmon-induced hot carriers in the graphene on the subresonant polarizability of the disk resonator. Because localized hot carrier generation in graphene can be exploited to drive electrical currents, plasmonic metal-graphene nanostructures present opportunities for novel hot carrier device concepts.

Effect of thermal treatment on the growth, structure and luminescence of nitride-passivated silicon nanoclusters

Silicon nanoclusters (Si-ncs) embedded in silicon nitride films have been studied to determine the effects that deposition and processing parameters have on their growth, luminescent properties, and electronic structure. Luminescence was observed from Si-ncs formed in silicon-rich silicon nitride films with a broad range of compositions and grown using three different types of chemical vapour deposition systems. Photoluminescence (PL) experiments revealed broad, tunable emissions with peaks ranging from the near-infrared across the full visible spectrum. The emission energy was highly dependent on the film composition and changed only slightly with annealing temperature and time, which primarily affected the emission intensity. The PL spectra from films annealed for duration of times ranging from 2 s to 2 h at 600 and 800°C indicated a fast initial formation and growth of nanoclusters in the first few seconds of annealing followed by a slow, but steady growth as annealing time was further increased. X-ray absorption near edge structure at the Si K- and L3,2-edges exhibited composition-dependent phase separation and structural re-ordering of the Si-ncs and silicon nitride host matrix under different post-deposition annealing conditions and generally supported the trends observed in the PL spectra.

Light Emission from Rare-Earth Doped Silicon Nanostructures

Rare earth (Tb or Ce)-doped silicon oxides were deposited by electron cyclotron resonance plasma-enhanced chemical vapour deposition (ECR-PECVD). Silicon nanocrystals (Si-ncs) were formed in the silicon-rich films during certain annealing processes. Photoluminescence (PL) properties of the films were found to be highly dependent on the deposition parameters and annealing conditions. We propose that the presence of a novel sensitizer in the Tb-doped oxygen-rich films is responsible for the indirect excitation of the Tb emission, while in the Tb-doped silicon-rich films the Tb emission is excited by the Si-ncs through an exciton-mediated energy transfer. In the Ce-doped oxygen-rich films, an abrupt increase of the Ce emission intensity was observed after annealing at 1200∘C. This effect is tentatively attributed to the formation of Ce silicate. In the Ce-doped silicon-rich films, the Ce emission was absent at annealing temperatures lower than 1100∘C due to the strong absorption of Si-ncs. Optimal film compositions and annealing conditions for maximizing the PL intensities of the rare earths in the films have been determined. The light emissions from these films were very bright and can be easily observed even under room lighting conditions.

Laser photoluminescence spectrometer based on charge-coupled device detection for silicon-based photonics

We describe and characterize a multichannel modular room temperature photoluminescence spectroscopy system. This low cost instrument offers minimization of size and complexity as well as good flexibility and acceptable spectral resolution. The system employs an efficient flexible front end optics and a sensitive spectrometer with a charge-coupled device array detector. The spectrometer has no moving parts and is more robust than a scanning system. The scientific motivation was to enable the photoluminescence study of various silicon photonics structures. Typical applications are presented for SiOx (x<2) films. It is demonstrated that high-quality steady state photoluminescence data with excellent signal to noise enhancement capability can be delivered besides the ability to perform simultaneous multiwavelength measurements in one shot. This instrument is shown to be useful for evaluating semiconductor wafers, including those intended for light emitting structures from silicon-based photonic crystals. The ...

Light emission from Si nanoclusters formed at low temperatures

Photoluminescence (PL) from amorphous Si nanoclusters (Si-ncls) formed by thin-film deposition via electron-cyclotron resonance plasma-enhanced chemical vapor deposition followed by annealing at temperatures ⩽875°C has been investigated. We find that Si-ncls grow very slowly after their initial nucleation at low temperatures. An increase in the size of Si-ncls, which can be controlled by the annealing temperature, induces a redshift in the Si-ncl PL peak. While the emitted optical power is more than 100 times smaller than that of Si nanocrystals formed in an identically deposited film, it is increased by a factor of up to approximately four times following hydrogen passivation. The incorporation of hydrogen causes a redshift in the PL peak position, suggesting a partial hydrogenation induced bond distortion of the Si-ncls. This redshift decreases with increasing hydrogen ambient annealing temperature.