Coherent control of ballistic photocurrents in multilayer epitaxial graphene using quantum interference.

We report generation of ballistic electric currents in unbiased epitaxial graphene at 300 K via quantum interference between phase-controlled cross-polarized fundamental and second harmonic 220 fs pulses. The transient currents are detected via the emitted terahertz radiation. Because of graphene's special structure symmetry, the injected current direction can be well controlled by the polarization of the pump beam in epitaxial graphene. This all optical injection of current provides not only a noncontact way of injecting directional current in graphene but also new insight into optical and transport process in epitaxial graphene.

Real-time biomolecular binding detection using a sensitive photonic crystal biosensor.

Real-time measurement of specific biomolecular interactions is critical to many areas of biological research. A number of label-free techniques for directly monitoring biomolecular binding have been developed, but it is still challenging to measure the binding kinetics of very small molecules, to detect low concentrations of analyte molecules, or to detect low affinity interactions. In this study, we report the development of a highly sensitive photonic crystal biosensor for label-free, real-time biomolecular binding analysis. We characterize the performance of this biosensor using a standard streptavidin-biotin binding system. Optimization of the surface functionalization methods for streptavidin immobilization on the silica sensing surface is presented, and the specific binding of biotinylated analyte molecules ranging over 3 orders of magnitude in molecular weight, including very small molecules (<250 Da), DNA oligonucleotides, proteins, and antibodies (>150 000 Da), are detected in real time with a high signal-to-noise ratio. Finally, we document the sensor efficiency for low mass adsorption, as well as multilayered molecular interactions. By all important metrics for sensitivity, we anticipate this photonic crystal biosensor will provide new capabilities for highly sensitive measurements of biomolecular binding.

Spectroscopic measurement of interlayer screening in multilayer epitaxial graphene.

The substrate-induced charge-density profile in carbon face epitaxial graphene is determined using nondegenerate ultrafast midinfrared pump-probe spectroscopy. Distinct zero crossings in the differential transmission spectra are used to identify the Fermi levels of layers within the multilayer stack. Probing within the transmission window of the SiC substrate, we find the Fermi levels of the first four heavily doped layers to be, respectively, 360, 215, 140, and 93 meV above the Dirac point. The charge screening length is determined to be one graphene layer, in good agreement with theoretical predictions.

Time-reversal and model-based imaging in a THz waveguide.

We investigate two approaches to improving the resolution of time-reversal based THz imaging systems. First, we show that a substantial improvement in the reconstruction of time-reversed THz fields is achieved by increasing the system's numerical aperture via a waveguide technique adapted from ultrasound imaging. Second, a model-based reconstruction algorithm is developed as an alternative to time-reversal THz imaging and its performance is demonstrated for cases with and without a waveguide.

Sensitive molecular binding assay using a photonic crystal structure in total internal reflection.

A novel optical sensor for label-free biomolecular binding assay using a one-dimensional photonic crystal in a total-internal-reflection geometry is proposed and demonstrated. The simple configuration provides a narrow optical resonance to enable sensitive measurements of molecular binding, and at the same time employs an open interface to enable real-time measurements of binding dynamics. Ultrathin aminopropyltriethoxysilane/ glutaraldehyde films adsorbed on the interface were detected by measuring the spectral shift of the photonic crystal resonance and the intensity ratio change in a differential reflectance measurement. A detection limit of 6 x 10(-5) nm for molecular layer thickness was obtained, which corresponds to a detection limit for analyte adsorption of 0.06 pg/mm(2) or a refractive index resolution of 3 x 10(-8) RIU; this represents a significant improvement relative to state-of-the-art surface-plasmon-resonance-based systems.

Whole spectrum fluorescence detection with ultrafast white light excitation.

We have developed a new detection mechanism for ultrabroadband multicolor fluorescence detection using an ultrafast supercontinuum white light source without spectral filtering to simultaneously excite different fluorophores. A nonlinear photonic crystal fiber was utilized in conjunction with a femtosecond laser to generate the supercontinuum. A time-resolved detector was tested to detect the whole spectrum fluorescence while gating out the excitation white light in the time domain.

GaP waveguide emitters for high power broadband THz generation pumped by Yb-doped fiber lasers.

We demonstrate the generation of broadband THz pulses by optical rectification in GaP waveguides pumped by high power Yb-doped fiber amplifiers. The dispersion of the GaP emitter can be controlled via the geometry of the waveguide; the peak frequency of the emitted THz radiation is tuned by varying the waveguide cross-section. Most importantly, the use of a waveguide for the THz emission increases the coherent buildup length of the THz pulses and offers scalability to higher power; this was investigated by pumping a GaP waveguide emitter with a high power Yb-doped fiber laser system. A 25-MHz-repetition-rate pulse train of THz radiation with 120 muW average power was achieved using 14 W optical power, which represents the highest average power for a broadband THz source pumped by fiber lasers to date.

Power scalable compact THz system based on an ultrafast Yb-doped fiber amplifier.

A power-scalable approach for THz generation is demonstrated using optical rectification in GaP pumped by a high power ultrafast Yb-doped fiber amplifier operating at 1.055 mum. A 120-MHz-repetition-rate pulse train of single-cycle THz radiation with 6.5 muW average power is generated using 10 W from a parabolic fiber amplifier. Analysis of the THz power scalability indicates that due to the unique advantages offered by ultrafast optical rectification in GaP and due to the power scalability of fiber lasers, this approach has the potential to generate single-cycle THz pulse trains with average powers up to several mW.

Microscopic origins of the terahertz carrier relaxation and cooling dynamics in graphene.

The ultrafast dynamics of hot carriers in graphene are key to both understanding of fundamental carrier-carrier interactions and carrier-phonon relaxation processes in two-dimensional materials, and understanding of the physics underlying novel high-speed electronic and optoelectronic devices. Many recent experiments on hot carriers using terahertz spectroscopy and related techniques have interpreted the variety of observed signals within phenomenological frameworks, and sometimes invoke extrinsic effects such as disorder. Here, we present an integrated experimental and theoretical programme, using ultrafast time-resolved terahertz spectroscopy combined with microscopic modelling, to systematically investigate the hot-carrier dynamics in a wide array of graphene samples having varying amounts of disorder and with either high or low doping levels. The theory reproduces the observed dynamics quantitatively without the need to invoke any fitting parameters, phenomenological models or extrinsic effects such as disorder. We demonstrate that the dynamics are dominated by the combined effect of efficient carrier-carrier scattering, which maintains a thermalized carrier distribution, and carrier-optical-phonon scattering, which removes energy from the carrier liquid.

Electronic cooling via interlayer Coulomb coupling in multilayer epitaxial graphene.

In van der Waals bonded or rotationally disordered multilayer stacks of two-dimensional (2D) materials, the electronic states remain tightly confined within individual 2D layers. As a result, electron-phonon interactions occur primarily within layers and interlayer electrical conductivities are low. In addition, strong covalent in-plane intralayer bonding combined with weak van der Waals interlayer bonding results in weak phonon-mediated thermal coupling between the layers. We demonstrate here, however, that Coulomb interactions between electrons in different layers of multilayer epitaxial graphene provide an important mechanism for interlayer thermal transport, even though all electronic states are strongly confined within individual 2D layers. This effect is manifested in the relaxation dynamics of hot carriers in ultrafast time-resolved terahertz spectroscopy. We develop a theory of interlayer Coulomb coupling containing no free parameters that accounts for the experimentally observed trends in hot-carrier dynamics as temperature and the number of layers is varied.

Label-free biosensing using a photonic crystal structure in a total-internal-reflection geometry.

A novel optical biosensor using a one-dimensional photonic crystal structure in a total-internal-reflection geometry (PC-TIR) is presented and investigated for label-free biosensing applications. This simple configuration forms a micro Fabry-Perot resonator in the top layer which provides a narrow optical resonance to enable label-free, highly sensitive measurements for the presence of analytes on the sensing surface or the refractive index change of the surrounding medium in the enhanced evanescent field; and at the same time it employs an open sensing surface for real-time biomolecular binding detection. The high sensitivity of the sensor was experimentally demonstrated by bulk solvent refractive index changes, ultrathin molecular films adsorbed on the sensing surface, and real-time analytes binding, measuring both the spectral shift of the photonic crystal resonance and the change of the intensity ratio in a differential reflectance measurement. Detection limits of 7x10(-8) RIU for bulk solvent refractive index, 6x10(-5) nm for molecular layer thickness and 24 fg/mm(2) for mass density were obtained, which represent a significant improvement relative to state-of-the-art surface-plasmon-resonance (SPR)-based systems. The PC-TIR sensor is thus seen to be a promising technology platform for high sensitivity and accurate biomolecular detection.

Ultrafast relaxation of excited Dirac fermions in epitaxial graphene using optical differential transmission spectroscopy.

We investigate the ultrafast relaxation dynamics of hot Dirac fermionic quasiparticles in multilayer epitaxial graphene using ultrafast optical differential transmission spectroscopy. We observe differential transmission spectra which are well described by interband transitions with no electron-hole interaction. Following the initial thermalization and emission of high-energy phonons, the electron cooling is determined by electron-acoustic phonon scattering, found to occur on the time scale of 1 ps for highly doped layers, and 4-11 ps in undoped layers. The spectra also provide strong evidence for the multilayer structure and doping profile of thermally grown epitaxial graphene on SiC.

Generation of radially polarized terahertz pulses via velocity-mismatched optical rectification.

We demonstrate the generation of radially polarized terahertz pulses via optical rectification in a Cherenkov geometry exploiting velocity mismatch, contrary to the traditional approach for generating linearly polarized terahertz beams. A compact system is implemented using 001-cut ZnTe pumped by an ultrafast Yb-doped fiber amplifier.