Publications

The ability to detect Weapons of Mass Destruction biological agents rapidly and sensitively is vital to homeland security, spurring development of compact detection systems at Sandia and elsewhere. One such system is Sandia's microseparations-based pChemLab. Many bio-agents are serious health threats even at extremely low concentrations. Therefore, a universal challenge for detection systems is the efficient collection and selective transport of highly diffuse bio-agents against the enormous background of benign particles and species ever present in the ambient environment. We have investigated development of a ''front end'' system for the collection, preconcentration, and selective transport of aerosolized biological agents from dilute (1-10 active particles per liter of air) atmospheric samples, to ultimate concentrations of {approx}20 active particles per microliter of liquid, for interface with microfluidic-based analyses and detection systems. Our approach employs a Sandia-developed aerosol particle-focusing microseparator array to focus size-selected particles into a mating microimpinger array of open microfluidic transport channels. Upon collection (i.e., impingement, submergence, and liquid suspension), microfluidic dielectrophoretic particle concentrators and sorters can be employed to further concentrate and selectively transport bio-agent particles to the sample preparation stages of microfluidic analyses and detection systems. This report documents results in experimental testing, modeling and analysis, component design, and materials fabrication critical to establishing proof-of-principle for this collection ''front end''. Outstanding results have been achieved for the aerodynamic microseparator, and for the post-collection dielectrophoretic concentrator and sorter. Results have been obtained for the microimpinger, too, but issues of particle-trapping by surface tension in liquid surfaces have proven difficult. Subsequent particle submergence into liquid suspension for microfluidic transport has been demonstrated only inefficiently despite significant and varied effort. Importantly, the separate technologies whose development is described, (inertial microseparator, dielectrophoretic corduroy concentrator/sorter) should each, independently, prove greatly useful in a variety of additional applications.

A combined experimental/modeling study was conducted to better understand the critical role of gas-surface interactions in rarefied gas flows. An experimental chamber and supporting diagnostics were designed and assembled to allow simultaneous measurements of gas heat flux and inter-plate gas density profiles in an axisymmetric, parallel-plate geometry. Measurements of gas density profiles and heat flux are made under identical conditions, eliminating an important limitation of earlier studies. The use of in situ, electron-beam fluorescence is demonstrated as a means to measure gas density profiles although additional work is required to improve the accuracy of this technique. Heat flux is inferred from temperature-drop measurements using precision thermistors. The system can be operated with a variety of gases (monatomic, diatomic, polyatomic, mixtures) and carefully controlled, well-characterized surfaces of different types (metals, ceramics) and conditions (smooth, rough). The measurements reported here are for 304 stainless steel plates with a standard machined surface coupled with argon, helium, and nitrogen. The resulting heat-flux and gas-density-profile data are analyzed using analytic and computational models to show that a simple Maxwell gas-surface interaction model is adequate to represent all of the observations. Based on this analysis, thermal accommodation coefficients for 304 stainless steel coupled with argon, nitrogen, and helium are determined to be 0.88, 0.80, and 0.38, respectively, with an estimated uncertainty of {+-}0.02.

A general, approximate expression is described that can be used to predict the thermophoretic force on a free-molecular, motionless, spherical particle suspended in a quiescent gas with a temperature gradient. The thermophoretic force is equal to the product of an order-unity coefficient, the gas-phase translational heat flux, the particle cross-sectional area, and the inverse of the mean molecular speed. Numerical simulations are used to test the accuracy of this expression for monatomic gases, polyatomic gases, and mixtures thereof. Both continuum and noncontinuum conditions are examined; in particular, the effects of low pressure, wall proximity, and high heat flux are investigated. The direct simulation Monte Carlo (DSMC) method is used to calculate the local molecular velocity distribution, and the force-Green's-function method is used to calculate the thermophoretic force. The approximate expression is found to predict the calculated thermophoretic force to within 10% for all cases examined.

Abstract not provided.

The molecular velocity distribution of a gas with heat flow was analyzed using Bird's direct simulation Monte Carlo (DSMC) method. Large numbers of computational molecules represented the gas in DSMC. Chapman-Enskog behavior was obtained for inverse-power-law molecules at continuum nonequilibrium conditions. It was shown that the Sonine-polynomial coefficients differ systematically from their continuum values as the local Knudsen number is increased, at noncontinuum nonequilibrium conditions.

An approach is presented to compute the force on a spherical particle in a rarefied flow of a monatomic gas. This approach relies on the development of a Green's function that describes the force on a spherical particle in a delta-function molecular velocity distribution function. The gas-surface interaction model in this development allows incomplete accommodation of energy and tangential momentum. The force from an arbitrary molecular velocity distribution is calculated by computing the moment of the force Green's function in the same way that other macroscopic variables are determined. Since the molecular velocity distribution function is directly determined in the DSMC method, the force Green's function approach can be implemented straightforwardly in DSMC codes. A similar approach yields the heat transfer to a spherical particle in a rarefied gas flow. The force Green's function is demonstrated by application to two problems. First, the drag force on a spherical particle at arbitrary temperature and moving at arbitrary velocity through an equilibrium motionless gas is found analytically and numerically. Second, the thermophoretic force on a motionless particle in a motionless gas with a heat flux is found analytically and numerically. Good agreement is observed in both situations.

A major cause of semiconductor yield degradation is contaminant particles that deposit on wafers while they reside in processing tools during integrated circuit manufacturing. This report presents numerical models for assessing particle transport and deposition in a parallel-plate geometry characteristic of a wide range of single-wafer processing tools: uniform downward flow exiting a perforated-plate showerhead separated by a gap from a circular wafer resting on a parallel susceptor. Particles are assumed to originate either upstream of the showerhead or from a specified position between the plates. The physical mechanisms controlling particle deposition and transport (inertia, diffusion, fluid drag, and external forces) are reviewed, with an emphasis on conditions encountered in semiconductor process tools (i.e., sub-atmospheric pressures and submicron particles). Isothermal flow is assumed, although small temperature differences are allowed to drive particle thermophoresis. Numerical solutions of the flow field are presented which agree with an analytic, creeping-flow expression for Re < 4. Deposition is quantified by use of a particle collection efficiency, which is defined as the fraction of particles in the reactor that deposit on the wafer. Analytic expressions for collection efficiency are presented for the limiting case where external forces control deposition (i.e., neglecting particle diffusion and inertia). Deposition from simultaneous particle diffusion and external forces is analyzed by an Eulerian formulation; for creeping flow and particles released from a planar trap, the analysis yields an analytic, integral expression for particle deposition based on process and particle properties. Deposition from simultaneous particle inertia and external forces is analyzed by a Lagrangian formulation, which can describe inertia-enhanced deposition resulting from particle acceleration in the showerhead. An approximate analytic expression is derived for particle velocity at the showerhead exit as a function of showerhead geometry, flow rate, and gas and particle properties. The particle showerhead-exit velocity is next used as an initial condition for particle transport between the plates to determine whether the particle deposits on the wafer, as a function of shower-head-exit particle velocity, the plate separation, flow rate, and gas and particle properties. Based on the numerical analysis, recommendations of best practices are presented that should help tool operators and designers reduce particle deposition in real tools. These guidelines are not intended to replace detailed calculations, but to provide the user with a general feel for inherently-clean practices.

This report presents the results of an experimental study of the aerosol produced by the combustion of high-velocity molten-uranium droplets produced by the simultaneous heating and electromagnetic launch of uranium wires. These tests are intended to simulate the reduction of high-velocity fragments into aerosol in high-explosive detonations or reactor accidents involving nuclear materials. As reported earlier, the resulting aerosol consists mainly of web-like chain agglomerates. A condensation nucleus counter was used to investigate the decay of the total particle concentration due to coagulation and losses. Number size distributions based on mobility equivalent diameter obtained soon after launch with a Differential Mobility Particle Sizer showed lognormal distributions with an initial count median diameter (CMD) of 0.3 {mu}m and a geometric standard deviation, {sigma}{sub g} of about 2; the CMD was found to increase and {sigma}{sub g} decrease with time due to coagulation. Mass size distributions based on aerodynamic diameter were obtained for the first time with a Microorifice Uniform Deposit Impactor, which showed lognormal distributions with mass median aerodynamic diameters of about 0.5 {mu}m and an aerodynamic geometric standard deviation of about 2. Approximate methods for converting between number and mass distributions and between mobility and aerodynamic equivalent diameters are presented.

SEMATECH and the Department of Energy have established a Contamination Free Manufacturing Research Center (CFMRC) located at Sandia National Laboratories. One of the programs underway at the CFMRC is directed towards defect reduction in semiconductor process reactors by the application of computational modeling. The goal is to use fluid, thermal, plasma, and particle transport models to identify process conditions and tool designs that reduce the deposition rate of particles on wafers. The program is directed toward defect reduction in specific manufacturing tools, although some model development is undertaken when needed. The need to produce quantifiable improvements in tool defect performance requires the close cooperation among Sandia, universities, SEMATECH, SEMATECH member companies, and equipment manufacturers. Currently, both plasma (e.g., etch, PECVD) and nonplasma tools (e.g., LPCVD, rinse tanks) are being worked on under this program. In this paper the authors summarize their recent efforts to reduce particle deposition on wafers during plasma-based semiconductor manufacturing.

In past five years, Department 1510 has developed a state-of-the-art Aerosol Dynamics Laboratory (ADL). This report documents the current instrumentation and capabilities that exist in this laboratory. The ADL was developed from a variety of sources, with a primary contribution from Department 1510's Independent Research and Development program in aerosol dynamics. Current capabilities of the ADL include: (1) generation of calibration-quality monodisperse particles with diameters between 0.005 to 100 {mu}m, (2) real-time measurement of particle size distributions for particle diameters between 0.01 and 100 {mu}m, (3) in situ, real-time measurement of particle size distributions for particle diameters between 0.3 and 100 {mu}m, and (4) real-time measurement of particle charge distributions for particle diameters between 0.01 and 1.0 {mu}m. 14 refs., 5 figs.

Gravitational forces have been found to be an important factor in defining the particle collection efficiency curve of inertial impactors for large particles. In general it was found that if the parameter {cflx G} = gW/V{sub 0}{sup 2} (g is the gravitational acceleration, W is the nozzle diameter and V{sub 0} is the average fluid velocity at the nozzle throat) in greater than 10{sup {minus}3}, the efficiency curve would shift to lower particle sizes. No effect could be seen for lower values of {cflx G}. 1 ref., 1 fig., 1 tab.