Matthew Pelton

Triggered single photons from a quantum dot

We demonstrate a new method for generating triggered single photons. After a laser pulse generates excitons inside a single quantum dot, electrostatic interactions between them and the resulting spectral shifts allow a single emitted photon to be isolated. Correlation measurements show a reduction of the two-photon probability to 0.12 times the value for Poisson light. Strong antibunching persists when the emission is saturated. The emitted photons are also polarized.

Simple Approach for High-Contrast Optical Imaging and Characterization of Graphene-Based Sheets

A simple optical method is presented for identifying and measuring the effective optical properties of nanometer-thick, graphene-based materials, based on the use of substrates consisting of a thin dielectric layer on silicon. High contrast between the graphene-based materials and the substrate is obtained by choosing appropriate optical properties and thickness of the dielectric layer. The effective refractive index and optical absorption coefficient of graphene oxide, thermally reduced graphene oxide, and graphene are obtained by comparing the predicted and measured contrasts.

Low-Threshold Stimulated Emission Using Colloidal Quantum Wells

The use of colloidal semiconductor nanocrystals for optical amplification and lasing has been limited by the need for high input power densities. Here we show that colloidal nanoplatelets produce amplified spontaneous emission with thresholds as low as 6 μJ/cm(2) and gain as high as 600 cm(-1), both a significant improvement over colloidal nanocrystals; in addition, gain saturation occurs at pump fluences 2 orders of magnitude higher than the threshold. We attribute this exceptional performance to large optical cross-sections, slow Auger recombination rates, and narrow ensemble emission line widths.

Optical trapping and alignment of single gold nanorods by using plasmon resonances.

We demonstrate three-dimensional trapping and orientation of individual Au nanorods by using laser light slightly detuned from their longitudinal plasmon mode. Detuning to the long-wavelength side of the resonance allows stable trapping for several minutes, with an exponential dependence of trapping time on laser power (consistent with a Kramers escape process). Detuning to the short-wavelength side causes repulsion of the rods from the laser focus. Alignment of the long axis of the rods with the trapping laser polarization is observed as a suppression of rotational diffusion about the short axis.

Atomic layer lithography of wafer-scale nanogap arrays for extreme confinement of electromagnetic waves

Squeezing light through nanometre-wide gaps in metals can lead to extreme field enhancements, nonlocal electromagnetic effects and light-induced electron tunnelling. This intriguing regime, however, has not been readily accessible to experimentalists because of the lack of reliable technology to fabricate uniform nanogaps with atomic-scale resolution and high throughput. Here we introduce a new patterning technology based on atomic layer deposition and simple adhesive-tape-based planarization. Using this method, we create vertically oriented gaps in opaque metal films along the entire contour of a millimetre-sized pattern, with gap widths as narrow as 9.9 Å, and pack 150,000 such devices on a 4-inch wafer. Electromagnetic waves pass exclusively through the nanogaps, enabling background-free transmission measurements. We observe resonant transmission of near-infrared waves through 1.1-nm-wide gaps (λ/1,295) and measure an effective refractive index of 17.8. We also observe resonant transmission of millimetre waves through 1.1-nm-wide gaps (λ/4,000,000) and infer an unprecedented field enhancement factor of 25,000.

Damping of acoustic vibrations in gold nanoparticles

Studies of acoustic vibrations in nanometre-scale particles can provide fundamental insights into the mechanical properties of materials because it is possible to precisely characterize and control the crystallinity and geometry of such nanostructures. Metal nanoparticles are of particular interest because they allow the use of ultrafast laser pulses to generate and probe high-frequency acoustic vibrations, which have the potential to be used in a variety of sensing applications. So far, the decay of these vibrations has been dominated by dephasing due to variations in nanoparticle size. Such inhomogeneities can be eliminated by performing measurements on single nanoparticles deposited on a substrate, but unknown interactions between the nanoparticles and the substrate make it difficult to interpret the results of such experiments. Here, we show that the effects of inhomogeneous damping can be reduced by using bipyramidal gold nanoparticles with highly uniform sizes. The inferred homogeneous damping is due to the combination of damping intrinsic to the nanoparticles and the surrounding solvent; the latter is quantitatively described by a parameter-free model.

Propagation Lengths and Group Velocities of Plasmons in Chemically Synthesized Gold and Silver Nanowires

Recent advances in chemical synthesis have made it possible to produce gold and silver nanowires that are free of large-scale crystalline defects and surface roughness. Surface plasmons can propagate along the wires, allowing them to serve as optical waveguides with cross sections much smaller than the optical wavelength. Gold nanowires provide improved chemical stability as compared to silver nanowires, but at the cost of higher losses for the propagating plasmons. In order to characterize this trade-off, we measured the propagation length and group velocity of plasmons in both gold and silver nanowires. Propagation lengths are measured by fluorescence imaging of the plasmonic near fields. Group velocities are deduced from the spacing of fringes in the spectrum of coherent light transmitted by the wires. In contrast to previous work, we interpret these fringes as arising from a far-field interference effect. The measured propagation characteristics agree with numerical simulations, indicating that propagation in these wires is dominated by the material properties of the metals, with additional losses due to scattering from roughness or grain boundaries providing at most a minor contribution. The propagation lengths and group velocities can also be described by a simple analytical model that considers only the lowest-order waveguide mode in a solid metal cylinder, showing that this single mode dominates in real nanowires. Comparison between experiments and theory indicates that widely used tabulated values for dielectric functions provide a good description of plasmons in gold nanowires but significantly overestimate plasmon losses in silver nanowires.

Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

Fluorescence blinking in nanocrystal quantum dots is known to exhibit power-law dynamics, and several different mechanisms have been proposed to explain this behavior. We have extended the measurement of quantum-dot blinking by characterizing fluctuations in the fluorescence of single dots over time scales from microseconds to seconds. The power spectral density of these fluctuations indicates a change in the power-law statistics that occurs at a time scale of several milliseconds, providing an important constraint on possible mechanisms for the blinking. In particular, the observations are consistent with the predictions of models wherein blinking is controlled by diffusion of the energies of electron or hole trap states.

Plasmon resonance-based optical trapping of single and multiple Au nanoparticles

The plasmon resonance-based optical trapping (PREBOT) method is used to achieve stable trapping of metallic nanoparticles of different shapes and composition, including Au bipyramids and Au/Ag core/shell nanorods. In all cases the longitudinal plasmon mode of these anisotropic particles is used to enhance the gradient force of an optical trap, thereby increasing the strength of the trap potential. Specifically, the trapping laser is slightly detuned to the long-wavelength side of the longitudinal plasmon resonance where the sign of the real component of the polarizability leads to an attractive gradient force. A second (femtosecond pulsed) laser is used to excite two-photon fluorescence for detection of the trapped nanoparticles. Two-photon fluorescence time trajectories are recorded for up to 20 minutes for single and multiple particles in the trap. In the latter case, a stepwise increase reflects sequential loading of single Au bipyramids. The nonlinearity of the amplitude and noise with step number are interpreted as arising from interactions or enhanced local fields amongst the trapped particles and fluctuations in the arrangements thereof.

Quantum-dot-induced transparency in a nanoscale plasmonic resonator

We investigate the near-field optical coupling between a single semiconductor nanocrystal (quantum dot) and a nanometer-scale plasmonic metal resonator using rigorous electrodynamic simulations. Our calculations show that the quantum dot produces a dip in both the extinction and scattering spectra of the surface-plasmon resonator, with a particularly strong change for the scattering spectrum. A phenomenological coupled-oscillator model is used to fit the calculation results and provide physical insight, revealing the roles of Fano interference and hybridization. The results indicate that it is possible to achieve nearly complete transparency as well as enter the strong-coupling regime for a single quantum dot in the near field of a metal nanostructure.