Photoinduced Force Mapping of Plasmonic Nanostructures.

The ability to image the optical near-fields of nanoscale structures, map their morphology, and concurrently obtain spectroscopic information, all with high spatiotemporal resolution, is a highly sought-after technique in nanophotonics. As a step toward this goal, we demonstrate the mapping of electromagnetic forces between a nanoscale tip and an optically excited sample consisting of plasmonic nanostructures with an imaging platform based on atomic force microscopy. We present the first detailed joint experimental-theoretical study of this type of photoinduced force microscopy.

Direct Plasmon-Driven Photoelectrocatalysis.

Harnessing the energy from hot charge carriers is an emerging research area with the potential to improve energy conversion technologies.1-3 Here we present a novel plasmonic photoelectrode architecture carefully designed to drive photocatalytic reactions by efficient, nonradiative plasmon decay into hot carriers. In contrast to past work, our architecture does not utilize a Schottky junction, the commonly used building block to collect hot carriers.

Light trapping for solar fuel generation with Mie resonances.

The implementation of solar fuel generation as a clean, terawatt-scale energy source is critically dependent on the development of high-performance, inexpensive photocatalysts. Many candidate materials, including for example α-Fe2O3 (hematite), suffer from very poor charge transport with minority carrier diffusion lengths that are significantly shorter (nanometer scale) than the absorption depth of light (micrometer scale near the band edge). As a result, most of the photoexcited carriers recombine rather than participate in water-splitting reactions.

Self-assembly based plasmonic arrays tuned by atomic layer deposition for extreme visible light absorption.

Achieving complete absorption of visible light with a minimal amount of material is highly desirable for many applications, including solar energy conversion to fuel and electricity, where benefits in conversion efficiency and economy can be obtained. On a fundamental level, it is of great interest to explore whether the ultimate limits in light absorption per unit volume can be achieved by capitalizing on the advances in metamaterial science and nanosynthesis. Here, we combine block copolymer lithography and atomic layer deposition to tune the effective optical properties of a plasmonic array at the atomic scale.

Plasmon enhanced solar-to-fuel energy conversion.

Future generations of photoelectrodes for solar fuel generation must employ inexpensive, earth-abundant absorber materials in order to provide a large-scale source of clean energy. These materials tend to have poor electrical transport properties and exhibit carrier diffusion lengths which are significantly shorter than the absorption depth of light. As a result, many photoexcited carriers are generated too far from a reactive surface and recombine instead of participating in solar-to-fuel conversion.

Polarization-dependent scanning photoionization microscopy: ultrafast plasmon-mediated electron ejection dynamics in single Au nanorods.

This work investigates plasmon-enhanced multiphoton scanning photoelectron emission microscopy (SPIM) of single gold nanorods under vacuum conditions. Striking differences in their photoemission properties are observed for nanorods deposited either on 2 nm thick Pt films or 10 nm thick indium tin oxide (ITO) films. On a Pt support, the Au nanorods display fourth-order photoionization when excited at 800 nm, a wavelength corresponding to their plasmon resonance in aqueous solution.

Direct measurement of the angular dependence of the single-photon ionization of aligned N2 and CO2.

By combining a state-of-the-art high-harmonic ultrafast soft X-ray source with field-free dynamic alignment, we map the angular dependence of molecular photoionization yields for the first time for a nondissociative molecule. The observed modulation in ion yield as a function of molecular alignment is attributed to the molecular frame transition dipole moment of single-photon ionization to the X, A and B states of N2(+) and CO2(+). Our data show that the transition dipoles for single-photon ionization of N2 and CO2 at 43 eV have larger perpendicular components than parallel ones.

Long-term carrier-envelope phase stability from a grating-based, chirped pulse amplifier.

We demonstrate a carrier-envelope phase (CEP) stabilized, chirped pulse laser amplifier that exhibits greatly improved intrinsic long-term CEP stability compared with that of other amplifiers. This system employs a grating-based stretcher and compressor and a cryogenically cooled laser amplifier. Single-shot carrier envelope phase noise measurements are also presented that avoid underestimation of this parameter caused by fringe averaging and represent a rigorously accurate upper limit on CEP noise.

Investigation of a grating-based stretcher/compressor for carrier-envelope phase stabilized fs pulses.

In this work, we experimentally investigate the effect of a grating based pulse stretcher/compressor on the carrier-envelope phase stability of femtosecond pulses. Grating based stretcher-compressor (SC) setups have been avoided in past demonstrations of chirped pulse amplification (CPA) of carrier envelope phase (CEP) stabilized femtosecond pulses, because they were expected to introduce significantly stronger CEP fluctuations than material-based SC systems. Using a microstructure fiber-based detection setup, we measure CEP fluctuations of PhiCE,SC = 340 milliradians rms for a frequency range from 63 mHz to 102 kHz for pulses propagating through the SC setup.

Broadband phase-coherent optical frequency synthesis with actively linked Ti:sapphire and Cr:forsterite femtosecond lasers.

We link the output spectra of a Ti:sapphire and a Cr:forsterite femtosecond laser phase coherently to form a continuous frequency comb with a wavelength coverage of 0.57-1.45 microm at power levels of 1 nW to 40 microW per frequency mode.

Chromium-doped forsterite: dispersion measurement with white-light interferometry.

Using a Michelson white-light interferometer, we measure the group-delay dispersion and third-order dispersion coefficients, d2(phi)/d(omega)2 and d3(phi)/d(omega)3, of chromium-doped forsterite (Cr:Mg2SiO4) over wavelengths of 1050-1600 nm for light polarized along both the c and b crystal axes. In this interval, the second-order dispersion for the c axis ranges from 35 fs2/mm to -14 fs2/mm, and the third-order dispersion ranges from 36 fs3/mm to 142 fs3/mm. For the b axis the second-order dispersion ranges from 35 fs2/mm to -15 fs2/mm and the third-order from 73 fs3/mm to 185 fs3/mm.