Method to deterministically study photonic nanostructures in different experimental instruments.

We describe an experimental method to recover a single, deterministically fabricated nanostructure in various experimental instruments without the use of artificially fabricated markers, with the aim to study photonic structures. Therefore, a detailed map of the spatial surroundings of the nanostructure is made during the fabrication of the structure. These maps are made using a series of micrographs with successively decreasing magnifications.

Large photonic strength of highly tunable resonant nanowire materials.

We demonstrate that highly tunable nanowire arrays with optimized diameters, volume fractions, and alignment form one of the strongest optical scattering materials to date. Using a new broad-band technique, we explore the scattering strength of the nanowires by varying systematically their diameter and alignment on the substrate. We identify strong Mie-type internal resonances of the nanowires which can be tuned over the entire visible spectrum.

Effect of confinement on proton-transfer reactions in water nanopools.

Proton transfer from the photoacid 8-hydroxy-1,3,6-pyrenetrisulfonic acid (HPTS) to water is studied in reverse micelles with ionic (AOT=sodium dioctyl sulfosuccinate) and non-ionic (BRIJ-30=polyoxyethylene(4)lauryl ether) surfactants. The dynamics are studied by probing the transient electronic absorption and transient vibrational absorption, both with sub-picosecond resolution. The reverse micelle sizes range from approximately 1.

Influence of ions on aqueous acid-base reactions.

We study the effects of bromide salts on the rate and mechanism of the aqueous proton/deuteron-transfer reaction between the photoacid 8-hydroxy-1,3,6-pyrenetrisulfonic acid (HPTS) and the base acetate. The proton/deuteron release is triggered by exciting HPTS with 400 nm femtosecond laser pulses. Probing the electronic and vibrational resonances of the photoacid, the conjugate photobase, the hydrated proton/deuteron and the accepting base with femtosecond visible and mid-infrared pulses monitors the proton transfer.

Long-range surface polaritons in ultra-thin films of silicon.

We present an experimental and theoretical study of the optical excitation of long-range surface polaritons supported by thin layers of amorphous silicon (a-Si). The large imaginary part of the dielectric constant of a-Si at visible and ultraviolet (UV) frequencies allows the excitation of surface polariton modes similar to long-range surface plasmon polaritons on metals. Propagation of these modes along considerable distances is possible because the electric field is largely excluded from the absorbing thin film.

Two regimes of slow-light losses revealed by adiabatic reduction of group velocity.

The losses in a photonic crystal waveguide were measured with a near-field microscope in the group velocity range of c/7 down to c/200. Our measurements show that the losses scale proportional to v{g};{-2} for group velocities above c/30. Below c/30, the losses are no longer described by the same power-law dependence on v{g} and the modal pattern becomes irregular, indicative of multiple scattering.

Design of light scattering in nanowire materials for photovoltaic applications.

We experimentally investigate the optical properties of layers of InP, Si, and GaP nanowires, relevant for applications in solar cells. The nanowires are strongly photonic, resulting in a significant coupling mismatch with incident light due to multiple scattering. We identify a design principle for the effective suppression of reflective losses, based on the ratio of the nondiffusive absorption and diffusive scattering lengths.

Full characterization of anisotropic diffuse light.

We demonstrate a method for fully characterizing diffuse transport of light in a statistically anisotropic opaque material. Our technique provides a simple means of determining all parameters governing anisotropic diffusion. Anisotropy in the diffusion constant, the mean free path, and the extrapolation length are, for the first time, determined independently.

Local and anisotropic excitation of surface plasmon polaritons by semiconductor nanowires.

We demonstrate a novel functionality of semiconductor nanowires as local sources for surface plasmon polaritons (SPPs). Photoexcited semiconductor nanowires decay non-radiatively exciting SPPs when they are on top of a metallic surface. We have investigated the anisotropic excitation of SPPs by nanowires by placing individual InP nanowires inside gold bullseye gratings.

Broadband enhanced backscattering spectroscopy of strongly scattering media.

We report on a new experimental method for enhanced backscattering spectroscopy (EBS) of strongly scattering media over a bandwidth from 530-1000 nm. The instrument consists of a supercontinuum light source and an angle-dependent detection system using a fiber-coupled grating spectrometer. Using a combination of two setups, the backscattered intensity is obtained over a large angular range and using circularly polarized light.

Nanofocusing in laterally tapered plasmonic waveguides.

We investigate the focusing of surface plasmon polaritons (SPPs) excited with 1.5 microm light in a tapered Au waveguide on a planar dielectric substrate by experiments and simulations. We find that nanofocusing can be obtained when the asymmetric bound mode at the substrate side of the metal film is excited.

Structural properties of opals grown with vertical controlled drying.

We have grown thin opals of self-assembled silica colloids by the well-known vertically controlled drying method. The volume fraction at the start of the growth and the temperature were systematically varied. We have quantitatively characterized the lateral domain sizes by scanning electron microscopy.

Ultrafast energy transfer dynamics of a bioinspired dyad molecule.

A caroteno-purpurin dyad molecule was studied by steady-state and pump-probe spectroscopies to resolve the excited-state deactivation dynamics of the different energy levels as well as the connecting energy flow pathways and corresponding rate constants. The data were analyzed with a two-step multi-parameter global fitting procedure that makes use of an evolutionary algorithm. We found that following ultrafast excitation of the donor (carotenoid) chromophore to its S2 state, the energy flows via two channels: energy transfer (70%) and internal conversion (30%) with time constants of 54 and 110 fs, respectively.

Novel instrument for surface plasmon polariton tracking in space and time.

We describe the realization of a phase-sensitive and ultrafast near-field microscope, optimized for investigation of surface plasmon polariton propagation. The apparatus consists of a homebuilt near-field microscope that is incorporated in Mach-Zehnder-type interferometer which enables heterodyne detection. We show that this microscope is able to measure dynamical properties of both photonic and plasmonic systems with phase sensitivity.

Direct determination of the sign of the NO dipole moment.

We report a novel approach for determining the sign of permanent dipole moments, using nitric oxide [NO(v=0)] as an example. State-selected NO (j=|m|=|Omega=1/2) molecules are focused using a hexapole and oriented in a strong dc electric field. The angular distributions of ionic fragments resulting from extreme ultraviolet single-photon and multiphoton dissociative ionization at 400 and 800 nm are measured and indicate that the dipole moment is negative (corresponding to N-O+).

Optical scattering resonances of single and coupled dimer plasmonic nanoantennas.

The optical resonances of individual plasmonic dimer antennas are investigated using confocal darkfield spectroscopy. Experiments on an array of antennas with varying arm lengths and interparticle gap sizes show large spectral shifts of the plasmon modes due to a combination of geometrical resonances and plasmon hybridization. The resonances of the coupled-dimer antennas are considerably broadened compared to those of single nanorods, which is attributed to a superradiant damping of the coupled antenna modes.

Direct observation of plasmonic modes in au nanowires using high-resolution cathodoluminescence spectroscopy.

We use cathodoluminescence imaging spectroscopy to excite and investigate plasmonic eigenmodes of Au nanowires with lengths of 500-1200 nm and approximately 100 nm width. We observe emission patterns along the Au nanowire axis that are symmetric and strongly wavelength dependent. Different patterns correspond to different resonant modes of the nanowire.

Calcium-induced phospholipid ordering depends on surface pressure.

The effect of sodium and calcium ions on zwitterionic and anionic phospholipids monolayers is investigated using vibrational sum-frequency generation in conjunction with surface pressure measurements and fluorescence microscopy. Sodium ions only subtly affect the monolayer structure, while the effect of calcium is large and depends strongly on the surface pressure. At low surface pressures (approximately 5 mN/m), the presence on Ca2+ results in the unexpected appearance of ordered domains.

Strong enhancement of the radiative decay rate of emitters by single plasmonic nanoantennas.

We demonstrate a strong, 5-fold enhancement of the radiative decay rate from highly efficient fluorescent dye molecules around resonant optical nanoantennas. The plasmonic modes of individual gold dimer antennas are tuned by the particle length and the antenna gap, providing control over both the spectral resonance position and the near-field mode profile of the nanoantenna. Resonant enhancement of the radiative and nonradiative decay rates of a fluorescent dye is observed, resulting in an increase of the internal quantum efficiency from 40% up to 53% for single antennas, and up to 59% for antenna clusters.

Modification of the photoluminescence anisotropy of semiconductor nanowires by coupling to surface plasmon polaritons.

We demonstrate efficient modification of the polarized light emission from single semiconductor nanowires by coupling this emission to surface plasmon polaritons on a metal grating. The polarization anisotropy of the emitted photoluminescence from single nanowires is compared for wires deposited on silica, a flat gold film, and a shallow gold grating. By varying the orientation of the nanowire with respect to the grating grooves, the large intrinsic polarization anisotropy can be either suppressed or enhanced.

Low-noise rotating sample holder for ultrafast transient spectroscopy at cryogenic temperatures.

We present the design and testing of a rotating device that fits within a commercial helium cryostat and is capable of providing at 4 K a fresh sample surface for subsequent shots of a 1-10 kHz amplified pulsed laser. We benchmark this rotator in a transient-absorption experiment on molecular switches. After showing that the device introduces only a small amount of additional noise, we demonstrate how the effect of signal degradation due to high fluence is completely resolved.

Enhanced nonlinear optical effects with a tapered plasmonic waveguide.

Infrared surface plasmon polaritons (SPPs) are concentrated in a laterally tapered planar Ag waveguide. The near field of SPPs excited with 1490 nm light at a Ag-sapphire interface is probed using the photoluminescence of upconverted Er ions at 550 and 660 nm. SPP interference patterns are observed that exhibit clear evidence of SPP concentration toward the taper end.

Disulfide bond cleavages observed in SORI-CID of three nonapeptides complexed with divalent transition-metal cations.

Tandem MS sequencing of peptides that contain a disulfide bond is often hampered when using a slow heating technique. We show that complexation of a transition-metal ion with a disulfide-bridge-containing nonapeptide yields very rich tandem mass spectra, including fragments that involve the cleavage of the disulfide bond up to 56% of the total product ion intensity. On the contrary, MS/MS of the corresponding protonated nonapeptides results predominantly in fragments from the region that is not involved in the disulfide bond.