S. Pochon

Optical control of gallium nanoparticle growth

The study of metallic nanoparticles has a long tradition in linear and nonlinear optics [1], with current emphasis on the ultrafast dynamics, size, shape and collective effects in their optical response [2-6]. Nanoparticles also represent the ultimate confined geometry:high surface-to-volume ratios lead to local field enhancements and a range of dramatic modifications of the materials properties and phase diagram [7-9]. Confined gallium has become a subject of special interest as the light-induced structural phase transition recently observed in gallium films [10, 11] has allowed for the demonstration of all-optical switching devices that operate at low laser power [12]. Spontaneous self-assembly has been the main approach to the preparation of nanoparticles (for a review see 13). Here we report that light can dramatically influence the nanoparticle self-assembly process: illumination of a substrate exposed to a beam of gallium atoms results in the formation of nanoparticles with a relatively narrow size distribution. Very low light intensities, below the threshold for thermally-induced evaporation, exert considerable control over nanoparticle formation through non-thermal atomic desorption induced by electronic excitation.We report that low-intensity light can dramatically influence and regulate the nanoparticle self-assembly process: Illumination of a substrate exposed to a beam of gallium atoms results in the formation of gallium nanoparticles with a relatively narrow size distribution. Very low light intensities, below the threshold for thermally induced evaporation, exert considerable control over nanoparticle formation.

Phase Coexistence in Gallium Nanoparticles Controlled by Electron Excitation

In gallium nanoparticles 100 nm in diameter grown on the tip of an optical fiber from an atomic beam we observed equilibrium coexistence of gamma, beta, and liquid structural phases that can be controlled by e-beam excitation in a highly reversible and reproducible fashion. With 2 keV electrons only 1 pJ of excitation energy per nanoparticle is needed to exercise control, with the equilibrium phase achieved in less than a few tenths of a microsecond. The transformations between coexisting phases are accompanied by a continuous change in the nanoparticle films reflectivity.

Controlling the coexistence of structural phases and the optical properties of gallium nanoparticles with optical excitation

We have observed reversible structural transformations, induced by optical excitation at 1.55 μm, between the β, γ and liquid phases of gallium in self-assembled gallium nanoparticles, with a narrow size distribution around 50 nm, on the tip of an optical fiber. Only a few tens of nanowatts of optical excitation per particle are required to control the transformations, which take the form of a dynamic phase coexistence and are accompanied by substantial changes in the optical properties of the nanoparticle film. The time needed to achieve phase equilibrium is in the microsecond range, and increases sharply near the transition temperatures.

Electron-beam induces reversible changes in the optical properties of gallium nanoparticles

The paper reports, for the first time, a beam of electrons which can be instrumental in switching the structural phase of gallium nanoparticles between solid and liquid phases, and between two different solid phases. Such change of the phase develops as a surface-driven, fully reversible phase transformation that drives changes in the optical properties of the nanoparticles and leads to reversible changes in the nanoparticle films reflectivity.

First observation of light-controlled self-assembly of gallium nanoparticles with narrow size dispersion

Summary form only given. We report growth processes that control the shape and size of particles as they form, through non-thermal processes, using a low-power (/spl sim/ few mW) infrared diode laser. We study nanoparticle formation on the ends of optical fibers exposed to a gallium atomic-beam source under high vacuum. The results of the experiments and numerical modeling indicate that the growth of gallium nanoparticles in a laser-illuminated area is controlled through non-thermal laser-induced processes. We expect that by changing the deposition conditions (atomic beam flux, substrate temperature, etc.) and laser parameters (wavelength, power, etc.), the size, shape and spatial distribution of nanoparticles could be varied.

Nanoscale photonics of structural transformations in gallium

We have found recently that Gallium, confined at an interface with silica, responds dramatically to low power optical excitation when held at temperatures close to its melting point (29.8oC). Intensities of just a few kW/cm2 can reversibly modulate the intensity (by up to 40%) and phase (by as much as several degrees) of reflected light as the result of a light-induced structural transition occurring in a layer of gallium of only a few nm thick. Here, we report that this concept - of achieving a nonlinearity via a light-induced transformation in a confined solid at a temperature close to a phase transition temperature - can also be applied to gallium nanoparticles. We present the transient all-optical switching characteristics of gallium nanoparticle films comprising particles, typically 80 nm in diameter, which were formed directly on the ends of optical fibers using a new light-assisted self-assembly technique. We also report, for the first time, that this light-induced structural transition in gallium confined at an interface with silica underlies a new mechanism for photoconductivity. In our opinion, the exploitation of the light-induced phase transition in gallium may be a means of enabling the development of nanoscale photonic devices.