Michael F. Becker

FEMTOSECOND LASER EXCITATION OF THE SEMICONDUCTOR-METAL PHASE TRANSITION IN VO2

We have measured the subpicosecond optical response of a solid‐state, semiconductor‐to‐metal phase transition excited by femtosecond laser pulses. We have determined the dynamic response of the complex refractive index of VO2 thin films by making pump‐probe optical transmission and reflection measurements at 780 nm. The phase transition was found to be largely prompt with the optical properties of the high‐temperature metallic state being attained within 5 ps. The ultrafast change in complex refractive index enables ultrafast optical switching devices in VO2.

Metal nanoparticles generated by laser ablation

Abstract We study a new method for producing ultrafine metal particles (nanopartides) that employs Laser Ablation of Microparticles (LAM). Pulsed excimer laser radiation at 248 nm wavelength was used to ablate ~2 μm feedstock of silver, gold, andpermalloy (Ni 81 %:Fe 19% ) under both normal atmospheric conditions and in other gases and pressures. A model for nanoparticle formation by LAM is proposed that includes plasma breakdown and shock-wave propagation through the initial microparticle. Behind the shock a large fraction of the original microparticle mass is converted to nanoparticles that diffuse to silicon substrates and TEM grids for collection and analysis. Nanoparticle morphologies are spherical except for gold nanoparticles >100 nm that are generally cubes. Electron micrographs of the samples were analyzed by computer-aided image processing to determine the effect of irradiation conditions on the nanoparticle size distribution. The results showed that mean particle diameters were normally in the range from 10 to 100 nm and that the particle size distributions were generally log-normal, with dispersion (diameter/standard deviation) ranging from 0.2 to 0.5. For metallic microparticle feedstock, the mean size of the produced nanoparticles generally increased with increasing laser fluence and were smallest for fluences not too far above the breakdown threshold.

FEMTOSECOND LASER EXCITATION DYNAMICS OF THE SEMICONDUCTOR-METAL PHASE TRANSITION IN VO2

We have measured the subpicosecond optical response of a solid‐state, semiconductor‐to‐metal phase transition excited by femtosecond laser pulses. We have determined the dynamic response of the complex refractive index of polycrystalline VO2 thin‐films by making pump‐probe optical transmission and reflection measurements at 780 nm. The phase transition was found to be largely prompt with the optical properties very close to the high‐temperature metallic state being attained within about 5 ps. The equilibration of the metallic state after femtosecond excitation was modeled by non‐exponentially decaying perturbations in the metallic state electron density and collision frequency. The decay of both these plasma parameters was well fit by a 1/√t time dependence. This indicated that a diffusion process governed the equilibration of the metallic phase of VO2.

Large-scale production of nanocrystals by laser ablation of microparticles in a flowing aerosol

We experimentally demonstrate the production of nanoparticles by laser ablation of microparticles entrained at high density in a flowing aerosol. The currently measured production rate of 20 grams per hour could be scaled to industrially useful rates. We have characterized the size distribution of particles and found nearly monodisperse distributions where mean sizes were smaller and varied less with laser fluence than was observed for ablation of microparticles held on flat plates. Mean size was controlled from 4–20 nm by varying the type and pressure of carrier gas. We found Ag and CdSe nanoparticles were crystalline having few dislocations. Materials tested included metals (Ag, Au, and W), semiconductors (Si, CdSe, GaN, and ZnO), ceramics (WC, SiC, and YBa2Cu3O7), and a ferroelectric. Two types of collection processes are described that preserve the nonagglomerated nature of the particles, even at high mass densities.

Electromagnetic scattering of two-dimensional surface-relief dielectric gratings

We employed the rigorous vector coupled-wave theory [J. Opt. Soc. Am. 73, 1105 (1983)] to analyze the electromagnetic scattering from two dimensional (2-D) surface-relief dielectric gratings. A shoot-back method was developed for the numerical solution of the resulting coupled differential equations. This method allowed numerical solutions to be found for grating structures of arbitrary profiles and relatively deep grooves. It was most suitable where the grating medium refractive index was not too large and where only a small number of propagating orders existed. Experiments confirmed the numerically predicted reflectivities for 2-D surface-relief dielectric sinusoidal gratings. Reflectivity measurements were made on 2-D sinusoidal gratings fabricated on photoresist and on polycarbonate. The grating periodicities were of the order of 3000 lines/mm such that only the zero-order diffracted waves were propagating in the incident region, and possibly a few forward orders in the transmission region. The embossing technique that was used for replicating the grating patterns from photoresist onto polycarbonate proved to be a feasible method for the production of such gratings.

Some problems of the material choice for the first mirrors of plasma diagnostics in a fusion reactor

We present the results of simulation experiments on the effect of the fusion reactor environment on the optical properties of the first mirrors for spectroscopy and laser diagnostics. We found the greatest effect on the degradation of mirror optical properties was due to charge exchange atoms. These atoms can affect mirror quality in two ways: by sputtering and by redeposition of material sputtered from other inner components of the vacuum chamber. The degradation rates of mirrors made of different metals and subjected to long-term bombardment by ions from hydrogen or deuterium plasmas are compared. From analysis of all data, we concluded that special experiments will have to be conducted in order to make a correct choice of a first mirror material. These tests should include the following: (1) study the role of swelling on mirror surface modification; (2) find the multimillion shot laser-induced-damage threshold of metal mirrors; and (3) develop and test methods to protect the first mirrors from redeposi...

Light-Directed Reversible Assembly of Plasmonic Nanoparticles Using Plasmon-Enhanced Thermophoresis

Reversible assembly of plasmonic nanoparticles can be used to modulate their structural, electrical, and optical properties. Common and versatile tools in nanoparticle manipulation and assembly are optical tweezers, but these require tightly focused and high-power (10-100 mW/μm2) laser beams with precise optical alignment, which significantly hinders their applications. Here we present light-directed reversible assembly of plasmonic nanoparticles with a power intensity below 0.1 mW/μm2. Our experiments and simulations reveal that such a low-power assembly is enabled by thermophoretic migration of nanoparticles due to the plasmon-enhanced photothermal effect and the associated enhanced local electric field over a plasmonic substrate. With software-controlled laser beams, we demonstrate parallel and dynamic manipulation of multiple nanoparticle assemblies. Interestingly, the assemblies formed over plasmonic substrates can be subsequently transported to nonplasmonic substrates. As an example application, we selected surface-enhanced Raman scattering spectroscopy, with tunable sensitivity. The advantages provided by plasmonic assembly of nanoparticles are the following: (1) low-power, reversible nanoparticle assembly, (2) applicability to nanoparticles with arbitrary morphology, and (3) use of simple optics. Our plasmon-enhanced thermophoretic technique will facilitate further development and application of dynamic nanoparticle assemblies, including biomolecular analyses in their native environment and smart drug delivery.

High-precision laser beam shaping using a binary-amplitude spatial light modulator

We have achieved high-precision laser beam shaping by using a binary-amplitude spatial light modulator, a digital micromirror device (DMD), followed by an imaging telescope that contains a pinhole low-pass filter (LPF). An error diffusion algorithm was used to design the initial DMD pixel pattern based on the measured input beam profile. This pattern was iteratively refined by simulating the optically low-pass filtered DMD image and changing DMD pixels to lift valleys and suppress peaks. We noted the gap between the experimental result of 1.4% root-mean-square (RMS) error and the simulated result for the same DMD pattern of 0.3% RMS error. Therefore, we deemed it necessary to introduce iterative refinement based on actual measurements of the output image to further improve the uniformity of the beam. Using this method, we have demonstrated the ability to shape raw, non-spatially filtered laser beams (quasi-Gaussian beams) into beams with precisely controlled profiles that have an unprecedented level of RMS error with respect to the target profile. We have shown that our iterative refinement process is able to improve the light intensity uniformity to around 1% RMS error in a raw camera image for both 633 and 1064 nm laser beams. The use of a digital LPF on the camera image is justified in that it matches the performance of the pinhole filter in the experimental setup. The digital low-pass filtered results reveal that the actual optical beam profiles have RMS error down to 0.23%. Our approach has also demonstrated the ability to produce a range of target profiles as long as they have similar spatial-frequency content (i.e., a slowly varying beam profile). Circular and square cross-section flat-top beams and beams with a linear intensity variation within a circular and square cross section were produced with similarly low RMS errors. The measured errors were about twice the ultimate limit of 0.1% RMS error based on the number of binary DMD pixels that participate in the beam-formation process.

1.5% root-mean-square flat-intensity laser beam formed using a binary-amplitude spatial light modulator

We demonstrate a digital micromirror device (DMD)-based optical system that converts a spatially noisy quasi-Gaussian to an eighth-order super-Lorentzian flat-top beam. We use an error-diffusion algorithm to design the binary pattern for the Texas Instruments DLP device. Following the DMD, a telescope with a pinhole low-pass filters the beam and scales it to the desired sized image. Experimental measurements show a 1% root-mean-square (RMS) flatness over a diameter of 0.28 mm in the center of the flat-top beam and better than 1.5% RMS flatness over its entire 1.43 mm diameter. The power conversion efficiency is 37%. We develop an alignment technique to ensure that the DMD pattern is correctly positioned on the incident beam. An interferometric measurement of the DMD surface flatness shows that phase uniformity is maintained in the output beam. Our approach is highly flexible and is able to produce not only flat-top beams with different parameters, but also any slowly varying target beam shape. It can be used to generate the homogeneous optical lattice required for Bose-Einstein condensate cold atom experiments.

Bimodal Nanoparticle Size Distributions Produced by Laser Ablation of Microparticles in Aerosols

Silver nanoparticles were produced by laser ablation of a continuously flowing aerosol of microparticles in nitrogen at varying laser fluences. Transmission electron micrographs were analyzed to determine the effect of laser fluence on the nanoparticle size distribution. These distributions exhibited bimodality with a large number of particles in a mode at small sizes (3–6-nm) and a second, less populated mode at larger sizes (11–16-nm). Both modes shifted to larger sizes with increasing laser fluence, with the small size mode shifting by 35% and the larger size mode by 25% over a fluence range of 0.3–4.2-J/cm2. Size histograms for each mode were found to be well represented by log-normal distributions. The distribution of mass displayed a striking shift from the large to the small size mode with increasing laser fluence. These results are discussed in terms of a model of nanoparticle formation from two distinct laser–solid interactions. Initially, laser vaporization of material from the surface leads to condensation of nanoparticles in the ambient gas. Material evaporation occurs until the plasma breakdown threshold of the microparticles is reached, generating a shock wave that propagates through the remaining material. Rapid condensation of the vapor in the low-pressure region occurs behind the traveling shock wave. Measurement of particle size distributions versus gas pressure in the ablation region, as well as, versus microparticle feedstock size confirmed the assignment of the larger size mode to surface-vaporization and the smaller size mode to shock-formed nanoparticles.