James P. Long

Low-Loss, Extreme Subdiffraction Photon Confinement via Silicon Carbide Localized Surface Phonon Polariton Resonators

Plasmonics provides great promise for nanophotonic applications. However, the high optical losses inherent in metal-based plasmonic systems have limited progress. Thus, it is critical to identify alternative low-loss materials. One alternative is polar dielectrics that support surface phonon polariton (SPhP) modes, where the confinement of infrared light is aided by optical phonons. Using fabricated 6H-silicon carbide nanopillar antenna arrays, we report on the observation of subdiffraction, localized SPhP resonances. They exhibit a dipolar resonance transverse to the nanopillar axis and a monopolar resonance associated with the longitudinal axis dependent upon the SiC substrate. Both exhibit exceptionally narrow linewidths (7-24 cm(-1)), with quality factors of 40-135, which exceed the theoretical limit of plasmonic systems, with extreme subwavelength confinement of (λ(res)3/V(eff))1/3 = 50-200. Under certain conditions, the modes are Raman-active, enabling their study in the visible spectral range. These observations promise to reinvigorate research in SPhP phenomena and their use for nanophotonic applications.

A room-temperature semiconductor spaser operating near 1.5 μm

Room temperature spasing of surface plasmon polaritons at 1.46 μm wavelength has been demonstrated by sandwiching a gold-film plasmonic waveguide between optically pumped InGaAs quantum-well gain media. The spaser exhibits gain narrowing, the expected transverse-magnetic polarization, and mirror feedback provided by cleaved facets in a 1-mm long cavity fabricated with a flip-chip approach. The 1.06-μm pump-threshold of ~60 kW/cm2 is in good agreement with calculations. The architecture is readily adaptable to all-electrical operation on an integrated microchip.

Characterization of reconstructed SiC(100) surfaces using soft‐x‐ray photoemission spectroscopy

The surface quality of βSiC films grown on Si(100) by chemical vapor deposition has been assessed through synchrotron photoemission measurements of the valence band and of the linewidths and surface‐induced structure in Si 2p core‐level spectra. For these n‐type samples, band bending is small on the c(2×2) and (3×2) surfaces but larger on the (2×1), which also exhibits an increased Si 2p linewidth and evidence of elemental Si patches. All three reconstructions show emission from gap states extending from the valence band maximum to the Fermi level.

Mie resonance-enhanced light absorption in periodic silicon nanopillar arrays.

Mie-resonances in vertical, small aspect-ratio and subwavelength silicon nanopillars are investigated using visible bright-field µ-reflection measurements and Raman scattering. Pillar-to-pillar interactions were examined by comparing randomly to periodically arranged arrays with systematic variations in nanopillar diameter and array pitch. First- and second-order Mie resonances are observed in reflectance spectra as pronounced dips with minimum reflectances of several percent, suggesting an alternative approach to fabricating a perfect absorber. The resonant wavelengths shift approximately linearly with nanopillar diameter, which enables a simple empirical description of the resonance condition. In addition, resonances are also significantly affected by array density, with an overall oscillating blue shift as the pitch is reduced. Finite-element method and finite-difference time-domain simulations agree closely with experimental results and provide valuable insight into the nature of the dielectric resonance modes, including a surprisingly small influence of the substrate on resonance wavelength. To probe local fields within the Si nanopillars, µ-Raman scattering measurements were also conducted that confirm enhanced optical fields in the pillars when excited on-resonance.

A New Methodology for Quantitative LSPR Biosensing and Imaging

A new quantitative analysis methodology for localized surface plasmon resonance (LSPR) biosensing which determines surface-receptor fractional occupancy, as well as an LSPR imaging technique for the spatiotemporal mapping of binding events, is presented. Electron beam nanolithography was used to fabricate 20 × 20 arrays of gold nanostructures atop glass coverslips. A single biotinylated array was used to measure the association kinetics of neutravidin to the surface by spectroscopically determining the fractional occupancy as a function of time. By regenerating the same array, a reliable comparison of the kinetics could be made between control samples and neutravidin concentrations ranging from 1 μM to 50 nM. CCD-based imagery of the array, taken simultaneously with the spectroscopic measurements, reveals the binding of neutravidin to the surface as manifested by enhanced scattering over the majority of the resonance peak. The temporal resolution of the LSPR imaging technique was 200 ms and the spatial resolution was 8 μm(2).

Quantitative imaging of protein secretions from single cells in real time.

Protein secretions from individual cells create spatially and temporally varying concentration profiles in the extracellular environment, which guide a wide range of biological processes such as wound healing and angiogenesis. Fluorescent and colorimetric probes for the detection of single cell secretions have time resolutions that range from hours to days, and as a result, little is known about how individual cells may alter their protein secretion rates on the timescale of minutes or seconds. Here, we present a label-free technique based upon nanoplasmonic imaging, which enabled the measurement of individual cell secretions in real time. When applied to the detection of antibody secretions from single hybridoma cells, the enhanced time resolution revealed two modes of secretion: one in which the cell secreted continuously and another in which antibodies were released in concentrated bursts that coincided with minute-long morphological contractions of the cell. From the continuous secretion measurements we determined the local concentration of antibodies at the sensing array closest to the cell and from the bursts we estimated the diffusion constant of the secreted antibodies through the extracellular media. The design also incorporates transmitted light and fluorescence microscopy capabilities for monitoring cellular morphological changes and intracellular fluorescent labels. We anticipate that this technique can be adapted as a general tool for the quantitative study of paracrine signaling in both adherent and nonadherent cell lines.

Surface passivation of InAs(001) with thioacetamide

We describe the passivation of InAs(001) surfaces with thioacetamide (CH3CSNH2 or TAM) as an alternative to the standard sulfur passivation using inorganic sulfide (NH4)2Sx. Quantitative comparison using x-ray photoelectron spectroscopy (XPS) demonstrates that TAM passivation dramatically improves the stability against reoxidation in air compared with the inorganic sulfide, with little to no etching during the treatment. We find that TAM passivation preserves the intrinsic surface charge accumulation layer, as directly confirmed with laser-induced photoemission. Overall, TAM appears to provide superior passivation for electronic device and sensing applications.

Evidence for charge-carrier mediated magnetic-field modulation of electroluminescence in organic light-emitting diodes

Electroluminescence (EL) from organic light-emitting diodes can be surprisingly sensitive (∼20%) to modest magnetic fields B (0–2T). The origin of this magnetic-field effect has not been clearly identified, although the magnetic-field effect in some devices resembles that of delayed fluorescence in anthracene, which originates from magnetic-field-dependent singlet-exciton production via triplet-triplet annihilation (TTA). Here, we test the role of TTA at low magnetic fields (∼80mT) by measuring transient EL and by employing dc drive levels so low that the bimolecular rate of TTA is unimportant. Under these conditions, we find enhancements of EL exceeding 14% at the lowest drives, which excludes TTA-mediated magnetic-field effects and indicates a role for charge-carrier pair states.

Photoemission and C 1s near-edge absorption from photopolymerized C60 films

Abstract Valence band and C 1s X-ray photoemission and near-edge absorption spectroscopy have been used to characterize C 60 photopolymerization induced by pulsed laser irradiation of 2.43 eV photons. Photoemission spectroscopy at various photon energies detected the reduced amplitude and broadening of the HOMO and HOMO −1 bands upon polymerization, and the appearance of two additional photoinduced features. In the C 1s NEXAFS, the unoccupied bands of C 60 were broadened upon photopolymerization with a small shift (≈0.1 eV) toward higher energy. The dependence of the photopolymerization rate on the incident laser intensity was sublinear for instantaneous laser intensities 70–800 kW/cm 2 .

Photoelectron spectroscopy of laser-excited states in semiconductors

When solids are exposed to intense pulsed laser radiation, highly excited electronic states are created that are of both practical and theoretical interest. Time-resolved photoelectron spectroscopic methods developed in recent years provide an effective approach to this problem and have yielded considerable information, particularly on semiconductors. The experiment reported on here uses a short, strongly absorbed laser pulse to excite electrons to intermediate states. Then a probe pulse that may be coincident or delayed relative to the exciting pulse and may have the same or higher photon energy ejects electrons whose energy distribution is measured. This distribution can be related directly to the distribution in the intermediate states. We describe applications of the general technique to observe normally unoccupied states between the Fermi level and vacuum level, to measure dynamics of surface space charge layers and surface recombination, to measure hot-electron temperatures, and to determine the rates of electron energy relaxation processes. Results on Si(111) 7 x 7 and cleaved ZnTe(110) and CdTe(110) surfaces are described.