One of the major motivators of this work is the Mercury Project, which is a 1 kW scalable diode-pumped solid-state laser system under development at Lawrence Livermore National Laboratory (LLNL). Major goals include 100 J pulses, 10% wallplug efficiency, 10 Hz repetition rate, and a 5 times diffraction limited beam. To achieve these goals the Mercury laser incorporates ytterbium doped Sr{sub 5}(PO{sub 4}){sub 3}F (S-FAP) as the amplifier gain medium. The primary focus of this thesis is a full understanding of the properties of this material which are necessary for proper design and modeling of the system. Ytterbium doped fluorapatites, which were previously investigated at LLNL, were found to be ideal candidate materials for a high power amplifier systems providing high absorption and emission cross sections, long radiative lifetimes, and high efficiency. A family of barium substituted S-FAP crystals were grown in an effort to modify the pump and emission bandwidths for application to broadband diode pumping and short pulse generation. Crystals of Yb{sup 3+}:Sr{sub 5-x}Ba{sub x}(PO{sub 4}){sub 3}F where x < 1 showed homogeneous lines offering 8.4 nm (1.8 times enhancement) of absorption bandwidth and 6.9 nm (1.4 times enhancement) of emission bandwidth. The gain saturation fluence of Yb:S-FAP …

Benchmark calculations for radiation transport coupled to a material temperature equation in a 1-D slab and 1-D spherical geometry binary random media are presented. The mixing statistics are taken to be homogeneous Markov statistics in the 1-D slab but only approximately Markov statistics in the 1-D sphere. The material chunk sizes are described by Poisson distribution functions. The material opacities are first taken to be constant and then allowed to vary as a strong function of material temperature. Benchmark values and variances for time evolution of the ensemble average of material temperature energy density and radiation transmission are computed via a Monte Carlo type method. These benchmarks are used as a basis for comparison with three other approximate methods of solution. One of these approximate methods is simple atomic mix. The second approximate model is an adaptation of what is commonly called the Levermore-Pomraning model and which is referred to here as the standard model. It is shown that recasting the temperature coupling as a type of effective scattering can be useful in formulating the third approximate model, an adaptation of a model due to Su and Pomraning which attempts to account for the effects of scattering in a stochastic …

This work describes several research projects aimed towards developing new instruments and novel methods for high throughput chemical and biological analysis. Approaches are taken in two directions. The first direction takes advantage of well-established semiconductor fabrication techniques and applies them to miniaturize instruments that are workhorses in analytical laboratories. Specifically, the first part of this work focused on the development of micropumps and microvalves for controlled fluid delivery. The mechanism of these micropumps and microvalves relies on the electrochemically-induced surface tension change at a mercury/electrolyte interface. A miniaturized flow injection analysis device was integrated and flow injection analyses were demonstrated. In the second part of this work, microfluidic chips were also designed, fabricated, and tested. Separations of two fluorescent dyes were demonstrated in microfabricated channels, based on an open-tubular liquid chromatography (OT LC) or an electrochemically-modulated liquid chromatography (EMLC) format. A reduction in instrument size can potentially increase analysis speed, and allow exceedingly small amounts of sample to be analyzed under diverse separation conditions. The second direction explores the surface enhanced Raman spectroscopy (SERS) as a signal transduction method for immunoassay analysis. It takes advantage of the improved detection sensitivity as a result of surface enhancement on colloidal gold, the …

Surface vibrational spectroscopy via infrared-visible sum-frequency generation (SFG) has been established as a useful tool to study the structures of different kinds of surfaces and interfaces. This technique was used to study the (0001) face of hexagonal ice (Ih). SFG spectra in the O-H stretch frequency range were obtained at various sample temperatures. For the vapor(air)/ice interface, the degree of orientational order of the dangling OH bonds at the surface was measured as a function of temperature. Disordering sets in around 200 K and increases dramatically with temperature, which is strong evidence of surface melting of ice. For the other ice interfaces (silica/OTS/ice and silica/ice), a similar temperature dependence of the hydrogen bonded OH stretch peak was observed; the free OH stretch mode, however, appears to be different from that of the vapor (air)/ice interface due to interactions at the interfaces. The technique was also used to measure the orientational distributions of the polymer chains on a rubbed polyvinyl alcohol surface. Results show that the polymer chains at the surface appear to be well aligned by rubbing, and the adsorbed liquid crystal molecules are aligned, in turn, by the surface polymer chains. A strong correlation exists between the orientational distributions …

The UV photolysis of hexanes solutions containing the complexes M(CO){sub 6} (M=Cr, Mo, W) or CpMn(CO){sub 3} (Cp={eta}{sup 5}-C{sub 5}H{sub 5}) and excess thiophene (T{sup *}) (T{sup *}=2,5-dimethylthiophene (2,5-Me{sub 2}T), benzothiophene (BT), and dibenzothiophene (DBT)) produces the {eta}{sup 1}(S)-T{sup *} complexes (CO){sub 5}M({eta}{sup 1}(S)-T{sup *}) 1-8 or Cp(CO){sub 2}Mn({eta}{sup 1}(S)-T{sup *})9-11, respectively. However, when T{sup *}=DBT, and M=Mo, a mixture of two products result which includes the {eta}{sup 1}(S)-DBT complex (CO){sub 5}Mo({eta}{sup 1}(S)-DBT) 4a and the unexpected {pi}-complex (CO){sub 3}Mo({eta}{sup 6}-DBT) 4b as detected by {sup 1}H NMR. The liability of the {eta}{sup 1}(S)-T{sup *} ligands is illustrated by the rapid displacement of DBT in the complex (CO){sub 5}W({eta}{sup 1}(S)-DBT) (1) by THF, and also in the complexes (CO){sub 5}Cr({eta}{sup 1}(S)-DBT) (5) and CpMn(CO){sub 2}({eta}{sup 1}(S)-DBT) (9) by CO (1 atm) at room temperature. Complexes 1-11 have been characterized spectroscopically ({sup 1}H NMR, IR) and when possible isolated as analytically pure solids (elemental analysis, EIMS). Single crystal, X-ray structural determinations are reported for (CO){sub 5}W({eta}{sup 1}(S)-DBT) and Cp(CO){sub 2}Mn({eta}{sup 1}(S)-DBT).

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