Relatively large gold nanoparticles (mean diameter of major axis 38.2 nm, mean aspect ratio 1.29) in aqueous solution were found to undergo shape transformations from ellipsoids to spheres at ca. 940 degrees C, which is much lower than their melting point, ca. 1060 degrees C. The shape transformation of gold nanoparticles induced by a single pulse of a Nd:YAG laser (lambda = 355 nm, pulse width = 30 ps) was directly observed by a transmission electron microscope (TEM). Analysis of the experimental data showed that the threshold energy for photothermally induced shape transformation was on the order of 40 fJ for a particle, which is smaller than the energy, 67 fJ, required for its complete melting. Estimations based on the heat balance and surface melting model revealed that the temperature which particles reach after a single laser pulse was about 940 degrees C, with the thickness of the liquid layer on the surface of the solid core being 1.4 nm. We also examined thermally induced shape transformation of gold nanoparticles on Si substrates; above 950 degrees C they changed their shapes to spheres, which supported our estimation. Due to the surface melting of particles, their shape transformation occurs at a temperature much lower than their melting point.

The mass accommodation (condensation) coefficient R of water vapor into liquid water was theoretically studied via two complementary approaches: by molecular dynamics (MD) scattering simulation and by computational fluid dynamics simulation of the droplet train/flow reactor experiment. The MD scattering simulation predicts R ∼ 1 at 273 K. The fluid dynamics simulation quantitatively interprets the gaseous resistance in the droplet train flow tube, which demonstrated that the results of the droplet train/flow reactor experiment [Li et al., J. Phys. Chem. A 2001, 105, 10627] are consistent with a value for the water R in the range between 0.2 and 1. Both methods are thus seen to be consistent and provide values for the mass accommodation coefficient of water in the ideal situation free from surface impurities and nonequilibrium latent heat production.

The evolution of size distributions of gold nanoparticles under pulsed laser irradiation (Nd:YAG, lambda = 355 nm, pulse width 30 ps) was carefully observed by transmission electron microscopy. Interestingly, the initial monomodal size distribution of gold nanoparticles turned into a bimodal one, with two peaks in the number of particles, one at 6 nm and the other at 16-24 nm. The sizes for small particles depended very little on the irradiated laser energy. This change is attributed to laser-induced size reduction of the initial gold nanoparticles followed by the formation of small particles. In our analysis, we extracted a characteristic value for the size-reduction rate per one pulse and revealed that laser-induced size reduction of gold nanoparticles occurred even below the boiling point. When laser energy is insufficient for the boiling of particles, formation of gold vapor around liquid gold drops is thought to cause the phenomenon. With enough laser energy for the boiling, the formation of gold vapor around and inside liquid gold drops is responsible for the phenomenon. We also observed particles with gold strings after one pulse irradiation with a laser energy of 43 mJ cm(-2) pulse(-1), which is sufficient energy for the boiling. It is considered that such particles with gold strings are formed by the projection of gaseous gold from liquid gold drops with some volume of liquid gold around the bubble. On the basis of comparison with previous work, picosecond laser pulses are thought to be the most efficient way to cause laser-induced size reduction of gold nanoparticles.

We illustrate the important trade-off between far-field scattering effects, which have the potential to provide increased optical path length over broad bands, and parasitic absorption due to the excitation of localized surface plasmon resonances in metal nanoparticle arrays. Via detailed comparison of photocurrent enhancements given by Au, Ag and Al nanostructures on thin-film GaAs devices we reveal that parasitic losses can be mitigated through a careful choice of scattering medium. Absorption at the plasmon resonance in Au and Ag structures occurs in the visible spectrum, impairing device performance. In contrast, exploiting Al nanoparticle arrays results in a blue shift of the resonance, enabling the first demonstration of truly broadband plasmon enhanced photocurrent and a 22% integrated efficiency enhancement.

The highest efficiency of 24.4% for the solar-to-hydrogen (STH) energy conversion was obtained in an outdoor field test by combining concentrator photovoltaic (CPV) modules with InGaP/GaAs/Ge three-junction cells and polymer-electrolyte electrochemical (EC) cells. The high efficiency was obtained by using the high-efficiency CPV modules (>31% under the present operation conditions) and the direct connection between the CPV modules and the EC cells with an almost optimized number of elements in series. The STH efficiency bottleneck was clarified to be the efficiency of the CPV modules, the over-potential of the EC cells, and matching of the operation point to the maximal-power point of the CPV modules.