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Investigating growth to detonation in vapor-deposited hexanitrostilbene and pentaerythritol tetranitrate films using high-throughput methods

Journal of Applied Physics

Knepper, Robert; Rupper, Stephen G.; DeJong, Stephanie D.; Marquez, Michael P.; Kittell, David E.; Schmitt, Randal L.; Tappan, Alexander S.

In this work, a high-throughput experimental setup was used to characterize initiation threshold and growth to detonation in the explosives hexanitrostilbene (HNS) and pentaerythritol tetranitrate (PETN). The experiment sequentially launched an array of laser-driven flyers to shock samples arranged in a 96-well microplate geometry, with photonic Doppler velocimetry diagnostics to characterize flyer velocity and particle velocity at the explosive–substrate interface. Vapor-deposited films of HNS and PETN were used to provide numerous samples with various thicknesses, enabling characterization of the evolution of growth to detonation. One-dimensional hydrocode simulations were performed with reactions disabled to illustrate where the experimental data deviate from the predicted inert response. Prompt initiation was observed in 144 μm thick HNS films at flyer velocities near 3000 m/s and in 125 μm thick PETN films at flyer velocities near 2400 m/s. This experimental setup enables rapid quantification of the growth of reactions in explosive materials that can reach detonation at sub-millimeter length scales. These data can subsequently be used for parameterizing reactive burn models in hydrocode simulations, as discussed in Paper II [D. E. Kittell, R. Knepper, and A. S. Tappan, J. Appl. Phys. 131, 154902 (2022)].

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Concept for maritime near-surface surveillance using water Raman scattering

Applied Optics

Shokair, Isaac R.; Johnson, Mark S.; Schmitt, Randal L.; Sickafoose, Shane S.

We discuss a maritime surveillance and detection concept based on Raman scattering of water molecules. Using a range-gated scanning lidar that detects Raman scattered photons from water, the absence or change of signal indicates the presence of a non-water object. With sufficient spatial resolution, a two-dimensional outline of the object can be generated by the scanning lidar. Because Raman scattering is an inelastic process with a relatively large wavelength shift for water, this concept avoids the often problematic elastic scattering for objects at or very close to the water surface or from the bottom surface for shallow waters. The maximum detection depth for this concept is limited by the attenuation of the excitation and return Raman light in water. If excitation in the UV is used, fluorescence can be used for discrimination between organic and non-organic objects. In this paper, we present a lidar model for this concept and discuss results of proof-of-concept measurements. Using published cross section values, the model and measurements are in reasonable agreement and show that a sufficient number of Raman photons can be generated for modest lidar parameters to make this concept useful for near-surface detection.

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Concept for Maritime Near-Surface Surveillance Using Water Raman Scattering

Shokair, Isaac R.; Johnson, Mark S.; Schmitt, Randal L.; Sickafoose, Shane S.

In this report we discuss a new maritime surveillance and detection concept based on Raman scattering of water molecules. Using a scanning lidar that detects Raman scattered photons from water, the absence or change of signal indicates the p resence of a non - water object. With sufficient spatial resolution a negative two dimensional imag e of the object can be generate d by the scanning lidar . Because Raman scatt er ing is an inelastic process with a relatively large wavelength shift for water , this concept completely avoids the problematic elastic sc attering for objects at or very close to the water surface . Elastic scattering makes it difficult to disc riminate between water and dark objects at or near the water surface especially when automated detection is required . It is also difficult to deal wit h elastic scattering from the bottom surface for shallow waters. The maximum detection depth for this concept is limited by the attenuation of the excitation and return Raman light in water. If excitation in the UV is used, fluorescence can be used for dis crimination between organic and non - organic objects. Range gating can be used for this concept for detection of objects below a specified depth. In this report we develop a lidar model for this concept to estimate the number of detected Raman photons fo r variable lidar parameters and depths in the presence of the solar background . We also report on the results of proof - of - concept measurements using the Sandia Ares lidar with excitation at 355 nm. The measurements show good agreement with the lidar mode l predictions. The detected number of photons for typical lidar parameter shows the concept is viable and applicable to a variety of day and nighttime detection scenarios. This concept has many potential applications including ne ar - surface mine detection, swimmer detection for security purposes, wide area search, as well as other civilian applications.

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Aerosol characterization study using multi-spectrum remote sensing measurement techniques

Schmitt, Randal L.; Sobczak, Alice M.; Sanchez, A.L.; Johnson, Mark S.; Servantes, B.L.

A unique aerosol flow chamber coupled with a bistatic LIDAR system was implemented to measure the optical scattering cross sections and depolarization ratio of common atmospheric particulates. Each of seven particle types (ammonium sulfate, ammonium nitrate, sodium chloride, potassium chloride, black carbon and Arizona road dust) was aged by three anthropogenically relevant mechanisms: 1. Sulfuric acid deposition, 2. Toluene ozonolysis reactions, and 3. m-Xylene ozonolysis reactions. The results of pure particle scattering properties were compared with their aged equivalents. Results show that as most particles age under industrial plume conditions, their scattering cross sections are similar to pure black carbon, which has significant impacts to our understanding of aerosol impacts on climate. In addition, evidence emerges that suggest chloride-containing aerosols are chemically altered during the organic aging process. Here we present the direct measured scattering cross section and depolarization ratios for pure and aged atmospheric particulates.

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The damage mechanism in borosilicate glass generated by nanosecond pulsed laser at 1.064 μm

Proceedings of SPIE - The International Society for Optical Engineering

Do, Binh T.; Kimmel, Mark W.; Pack, Michael P.; Schmitt, Randal L.; Smith, Arlee V.

We studied theoretically the laser-plasma interaction, and performed experiments to investigate the mechanisms giving rise to optical damage in Borosilicate glass using nanosecond laser pulses at wavelength 1064 nm. Our experimental result shows that the optical damage process generated by nanosecond laser pulses is the result of an optically induced plasma. The plasma is initiated when the laser irradiance frees electrons from the glass. Although it may be debated, the electrons are likely freed by multi-photon absorption and the number density grows via impact ionization. Later when the electron gas density reaches the critical density, the electron gas resonantly absorbs the laser beam through collective excitation since the laser frequency is equal to the plasma frequency. The laser energy absorbed through the collective excitation is much larger than the energy absorbed by multi-photon ionization and impact ionization. Our experimental result also shows the plasma survives until the end of the laser pulse and the optical damage occurs after the laser pulse ceases. The plasma decay releases heat to the lattice. This heat causes the glass to be molten and soft. It is only as the glass cools and solidifies that stresses induced by this process cause the glass to fracture and damage. We also show the experimental evidence of the change of the refractive index of the focusing region as the density of the electron gas changes from sub-critical to overcritical, and the reflection of the over-critical plasma. This reflection limits the electron gas density to be not much larger than the critical density. © 2012 SPIE.

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A short-standoff bistatic lidar system for aerosol cloud backscatter cross section measurement

CLEO: Applications and Technology, CLEO_AT 2012

Schmitt, Randal L.; Glen, Crystal C.; Sickafoose, Shane S.; Shagam, Richard N.; Santarpia, Joshua S.; Brockmann, John E.; Reichardt, Thomas A.; Pack, Michael P.; Chavez, Victor; Boney, Craig M.; Servantes, B.L.

A short-standoff bistatic lidar system coupled with an aerosol chamber has been built to measure aerosol optical backscatter and laser induced fluorescence cross-sections. Preliminary results show good sensitivity across all channels with high signal-to-noise ratio. © OSA 2012.

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Fluorescence measurements for evaluating the application of multivariate analysis techniques to optically thick environments

Reichardt, Thomas A.; Schmitt, Randal L.; Sickafoose, Shane S.; Jones, Howland D.; Timlin, Jerilyn A.

Laser-induced fluorescence measurements of cuvette-contained laser dye mixtures are made for evaluation of multivariate analysis techniques to optically thick environments. Nine mixtures of Coumarin 500 and Rhodamine 610 are analyzed, as well as the pure dyes. For each sample, the cuvette is positioned on a two-axis translation stage to allow the interrogation at different spatial locations, allowing the examination of both primary (absorption of the laser light) and secondary (absorption of the fluorescence) inner filter effects. In addition to these expected inner filter effects, we find evidence that a portion of the absorbed fluorescence is re-emitted. A total of 688 spectra are acquired for the evaluation of multivariate analysis approaches to account for nonlinear effects.

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Vibrational spectroscopy of HNS degradation

Martin, Laura E.; Schmitt, Randal L.; Ten Eyck, Gregory A.; Welle, Eric W.

Hexanitrostilbene (HNS) is a widely used explosive, due in part to its high thermal stability. Degradation of HNS is known to occur through UV, chemical exposure, and heat exposure, which can lead to reduced performance of the material. Common methods of testing for HNS degradation include wet chemical and surface area testing of the material itself, and performance testing of devices that use HNS. The commonly used chemical tests, such as volatility, conductivity and contaminant trapping provide information on contaminants rather than the chemical stability of the HNS itself. Additionally, these tests are destructive in nature. As an alternative to these methods, we have been exploring the use of vibrational spectroscopy as a means of monitoring HNS degradation non-destructively. In particular, infrared (IR) spectroscopy lends itself well to non-destructive analysis. Molecular variations in the material can be identified and compared to pure samples. The utility of IR spectroscopy was evaluated using pressed pellets of HNS exposed to DETA (diethylaminetriamine). Amines are known to degrade HNS, with the proposed product being a {sigma}-adduct. We have followed these changes as a function of time using various IR sampling techniques including photoacoustic and attenuated total reflectance (ATR).

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Compact, narrow-linewidth, tunable ultraviolet laser source for detecting Hg emissions

Proceedings of SPIE - The International Society for Optical Engineering

Hoops, Alexandra A.; Farrow, Roger L.; Schulz, Paul; Reichardt, Thomas A.; Bambha, Ray B.; Schmitt, Randal L.; Kliner, Dahv A.V.

Recent EPA regulations targeting mercury (Hg) emissions from utility coal boilers have prompted increased activity in the development of reliable chemical sensors for monitoring Hg emissions with high sensitivity, high specificity, and fast time response. We are developing a portable, laser-based instrument for real-time, stand-off detection of Hg emissions that involves exciting the Hg (6 3P1 ← 6 1S0) transition at 253.7 nm and detecting the resulting resonant emission from Hg (6 3P1). The laser for this approach must be tunable over the Hg absorption line at 253.7 nm, while system performance modeling has indicated a desired output pulse energy ≥0.1 μJ and linewidth ≤5 GHz (full width at half-maximum, FWHM). In addition, the laser must have the requisite physical characteristics for use in coal-fired power plants. To meet these criteria, we are pursing a multistage frequency-conversion scheme involving an optical parametric amplifier (OPA). The OPA is pumped by the frequency-doubled output of a passively Q-switched, monolithic Nd:YAG micro-laser operating at 10-Hz repetition rate and is seeded by a 761-nm, cw distributed-feedback diode laser. The resultant pulse-amplified seed beam is frequency tripled in two nonlinear frequency-conversion steps to generate 253.7-nm light. The laser system is mounted on a 45.7 cm × 30.5 cm breadboard and can be further condensed using custom optical mounts. Based on simulations of the nonlinear frequency-conversion processes and current results, we expect this laser architecture to exceed the desired pulse energy. Moreover, this approach provides a compact, all-solid-state source of tunable, narrow-linewidth visible and ultraviolet radiation, which is required for many chemical sensing applications.

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Design and performance of a high-repetition-rate single-frequency Yb:YAG microlaser

Proceedings of SPIE - The International Society for Optical Engineering

Schmitt, Randal L.; Do, Binh T.

We describe the design and performance of a high-repetition-rate single-frequency passively Q-switched Yb:YAG microlaser operating near 1030 nm. By using short cavity length, an intracavity Brewster polarizer, and an etalon output coupler, we are able to produce ∼1-ns-long single-frequency pulses at repetition rates up to 19 kHz without shot-to-shot mode hopping. The laser's output spatial mode is TEM00 and its pulse energy varies between 31 μJ and 47 μJ depending on repetition rate. Its peak optical-to-optical efficiency is 22%.

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Power scaling of fiber-based amplifiers seeded with microchip lasers

Proceedings of SPIE - The International Society for Optical Engineering

Schrader, Paul E.; Fève, Jean P.; Farrow, Roger L.; Kliner, Dahv A.V.; Schmitt, Randal L.; Do, Binh T.

We summarize the performance of mode-filtered, Yb-doped fiber amplifiers seeded by microchip lasers with nanosecond-duration pulses. These systems offer the advantages of compactness, efficiency, high peak power, diffraction-limited beam quality, and widely variable pulse energy and repetition rate. We review the fundamental limits on pulsed fiber amplifiers imposed by nonlinear processes, with a focus on the specific regime of nanosecond pulses. Different design options for the fiber and the seed laser are discussed, including the effects of pulse duration, wavelength, and linewidth. We show an example of a microchip-seeded, single-stage, single-pass fiber amplifier that produced pulses with 1.1 MW peak power, 0.76 mJ pulse energy, smooth temporal and spectral profiles, diffractionlimited beam quality, and linear polarization.

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Development of a compact, narrow-linewidth, tunable ultraviolet laser source for detection of Hg0

Optics InfoBase Conference Papers

Hoops, Alexandra A.; Reichardt, Thomas A.; Schulz, P.; Farrow, Roger L.; Bambha, Ray B.; Schmitt, Randal L.; Kliner, Dahv A.V.

A portable laser for real-time, stand-off detection of Hg0 emissions from coal-fired power plants is developed and characterized. The pulse energy of the 254-nm laser is 1.8 μJ, which will enable sub-ppb detection of Hg0. © 2007 Optical Society of America.

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Design and performance of a high-repetition-rate single-frequency Yb:YAG microlaser

Schmitt, Randal L.

We describe the design and performance of a high-repetition-rate single-frequency passively Q-switched Yb:YAG microlaser operating near 1030 nm. By using short cavity length, an intracavity Brewster polarizer, and an etalon output coupler, we are able to produce {approx}1-ns-long single-frequency pulses at repetition rates up to 19 kHz without shot-to-shot mode hopping. The laser's output spatial mode is TEM{sub 00} and its pulse energy varies between 31 {micro}J and 47 {micro}J depending on repetition rate. Its peak optical-to-optical efficiency is 22%.

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Final LDRD report : development of advanced UV light emitters and biological agent detection strategies

Crawford, Mary H.; Armstrong, Andrew A.; Allerman, A.A.; Figiel, J.J.; Schmitt, Randal L.; Serkland, Darwin K.

We present the results of a three year LDRD project which has focused on the development of novel, compact, ultraviolet solid-state sources and fluorescence-based sensing platforms that apply such devices to the sensing of biological and nuclear materials. We describe our development of 270-280 nm AlGaN-based semiconductor UV LEDs with performance suitable for evaluation in biosensor platforms as well as our development efforts towards the realization of a 340 nm AlGaN-based laser diode technology. We further review our sensor development efforts, including evaluation of the efficacy of using modulated LED excitation and phase sensitive detection techniques for fluorescence detection of bio molecules and uranyl-containing compounds.

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Next generation gas imaging: Active differential absorption measurement to enhance sensitivity and quantify concentration

Proceedings of the Air and Waste Management Association's Annual Conference and Exhibition, AWMA

Bambha, Ray B.; Reichardt, Thomas A.; Sommers, Ricky; Birtola, Sal; Hubbard, Gary; Kulp, Thomas J.; Schmitt, Randal L.; Tamura, Masayuki; Kothari, Kiran

A discussion on an active gas imager that can potentially improve system performance and reliability in Smart Leak Detection and Repair covers conventional single-wavelength imaging; differential imaging; methane detection; modification for detecting fugitive emissions relevant to refineries and chemical plants; and system description. This is an abstract of a paper presented at the AWMA's 99th Annual Conference and Exhibition (New Orleans, LA 6/20-23/2006).

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MEMS-activated mirrors for arming and safing in optical firing sets

Proceedings of SPIE - The International Society for Optical Engineering

Schmitt, Randal L.; Do, Binh T.; Davis, Coby L.; Reicher, David; Peplinski, Stanley Z.

In optical firing sets, laser light is used to supply power to electronics (to charge capacitors, for example), to trigger electronics (such as vacuum switches), or in some cases, initiate explosives directly. Since MEMS devices combine electronics with electro-mechanical actuators, one can integrate safe and arm logic alongside the actuators to provide all functions in a single miniature package. We propose using MEMS-activated mirrors to make or break optical paths as part of the safe and arm architecture in an optical firing set. In the safe mode, a miniature (∼1 mm diameter) mirror is oriented to prevent completion of the optical path. To arm the firing set, the MEMS mirrors are deflected into the proper orientation thereby completing the optical path required for system functionality (e.g., light from a miniature laser completes the path to an optically triggered switch). The optical properties (i.e. damage threshold, reflectivity, transmission, absorption and scatter) of the miniature mirrors are critical to this application. Since Si is a strong absorber at the wavelengths under consideration (800 to 1064 nm), high-reflectivity, high-damage-threshold, dielectric coatings must be applied to the MEMS devices. In this paper we present conceptual MEMS-activated mirror architectures for performing arming and safing functions in an optical firing set and report test data which shows that dielectric coatings applied to MEMS-mirrors can withstand the prerequisite laser pulse irradiance. The measured optical damage threshold of polysilicon membranes with high-reflectivity multilayer dielectric coatings is ∼ 4 GW/cm 2, clearly demonstrating the feasibility of using coated MEMS mirrors in firing sets.

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Studies of the laser-induced fluorescence of explosives and explosive compositions

Schmitt, Randal L.; Thorne, Lawrence R.; Hargis, Philip J.; Parmeter, John E.

Continuing use of explosives by terrorists throughout the world has led to great interest in explosives detection technology, especially in technologies that have potential for standoff detection. This LDRD was undertaken in order to investigate the possible detection of explosive particulates at safe standoff distances in an attempt to identify vehicles that might contain large vehicle bombs (LVBs). The explosives investigated have included the common homogeneous or molecular explosives, 2,4,6-trinitrotoluene (TNT), pentaerythritol tetranitrate (PETN), cyclonite or hexogen (RDX), octogen (HMX), and the heterogeneous explosive, ammonium nitrate/fuel oil (ANFO), and its components. We have investigated standard excited/dispersed fluorescence, laser-excited prompt and delayed dispersed fluorescence using excitation wavelengths of 266 and 355 nm, the effects of polarization of the laser excitation light, and fluorescence imaging microscopy using 365- and 470-nm excitation. The four nitro-based, homogeneous explosives (TNT, PETN, RDX, and HMX) exhibit virtually no native fluorescence, but do exhibit quenching effects of varying magnitude when adsorbed on fluorescing surfaces. Ammonium nitrate and fuel oil mixtures fluoresce primarily due to the fuel oil, and, in some cases, due to the presence of hydrophobic coatings on ammonium nitrate prill or impurities in the ammonium nitrate itself. Pure ammonium nitrate shows no detectable fluorescence. These results are of scientific interest, but they provide little hope for the use of UV-excited fluorescence as a technique to perform safe standoff detection of adsorbed explosive particulates under real-world conditions with a useful degree of reliability.

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High-peak-power (>1.2 MW) pulsed fiber amplifier

Proceedings of SPIE - The International Society for Optical Engineering

Farrow, Roger L.; Kliner, Dahv A.V.; Schrader, Paul E.; Hoops, Alexandra A.; Moore, Scan W.; Hadley, G.R.; Schmitt, Randal L.

We report results from Yb-doped fiber amplifiers seeded with two microchip lasers having 0.38-ns and 2.3-ns pulse durations. The shorter duration seed resulted in output pulses with a peak power of > 1.2 MW and pulse energy of 0.67 mJ. Peak power was limited by nonlinear processes that caused breakup and broadening of the pulse envelope as the pump power increased. The 2.3-ns duration seed laser resulted in output pulses with a peak power of >300 kW and pulse energy of > 1.1 mJ. Pulse energies were limited by the onset of stimulated Brillouin scattering and ultimately by internal optical damage (fluences in excess of 400 J/cm 2 were generated). In both experiments, nearly diffraction-limited beam profiles were obtained, with M 2 values of < 1.2. Preliminary results of a pulse-amplification model are in excellent agreement with the experimental results of the amplifiers operating in the low-to-moderate gain-depletion regime.

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Monolithic passively Q-switched Cr:Nd:GSGG microlaser

Proceedings of SPIE - The International Society for Optical Engineering

Schmitt, Randal L.

Optical firing sets need miniature, robust, reliable pulsed laser sources for a variety of triggering functions. In many cases, these lasers must withstand high transient radiation environments. In this paper we describe a monolithic passively Q-switched microlaser constructed using Cr:Nd:GSGG as the gain material and Cr4+:YAG as the saturable absorber, both of which are radiation hard crystals. This laser consists of a 1-mm-long piece of undoped YAG, a 7-mm-long piece of Cr:Nd:GSGG, and a 1.5-mm-long piece of Cr 4+:YAG diffusion bonded together. The ends of the assembly are polished flat and parallel and dielectric mirrors are coated directly on the ends to form a compact, rugged, monolithic laser. When end pumped with a diode laser emitting at ∼807.6 nm, this passively Q-switched laser produces ∼1.5-ns-wide pulses. While the unpumped flat-flat cavity is geometrically unstable, thermal lensing and gain guiding produce a stable cavity with a TEM00 gaussian output beam over a wide range of operating parameters. The output energy of the laser is scalable and dependent on the cross sectional area of the pump beam. This laser has produced Q-switched output energies from several μJ per pulse to several 100 μJ per pulse with excellent beam quality. Its short pulse length and good beam quality result in high peak power density required for many applications such as optically triggering sprytrons. In this paper we discuss the design, construction, and characterization of this monolithic laser as well as energy scaling of the laser up to several 100 μJ per pulse.

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Tracking Honey Bees Using LIDAR (Light Detection and Ranging) Technology

Bender, Susan F.; Bender, Susan F.; Rodacy, Philip J.; Schmitt, Randal L.; Hargis, Philip J.; Johnson, Mark S.; Klarkowski, James R.; Magee, Glen I.; Bender, Gary L.

The Defense Advanced Research Projects Agency (DARPA) has recognized that biological and chemical toxins are a real and growing threat to troops, civilians, and the ecosystem. The Explosives Components Facility at Sandia National Laboratories (SNL) has been working with the University of Montana, the Southwest Research Institute, and other agencies to evaluate the feasibility of directing honeybees to specific targets, and for environmental sampling of biological and chemical ''agents of harm''. Recent work has focused on finding and locating buried landmines and unexploded ordnance (UXO). Tests have demonstrated that honeybees can be trained to efficiently and accurately locate explosive signatures in the environment. However, it is difficult to visually track the bees and determine precisely where the targets are located. Video equipment is not practical due to its limited resolution and range. In addition, it is often unsafe to install such equipment in a field. A technology is needed to provide investigators with the standoff capability to track bees and accurately map the location of the suspected targets. This report documents Light Detection and Ranging (LIDAR) tests that were performed by SNL. These tests have shown that a LIDAR system can be used to track honeybees. The LIDAR system can provide both the range and coordinates of the target so that the location of buried munitions can be accurately mapped for subsequent removal.

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Distributed Sensor Particles for Remote Fluorescence Detection of Trace Analytes: UXO/CW

Singh, Anup K.; Schmitt, Randal L.; Johnson, Mark S.; Hargis, Philip J.; Simonson, Robert J.; Simonson, Robert J.; Schoeniger, Joseph S.; Ashley, Carol S.; Brinker, C.J.; Hance, Bradley G.

This report summarizes the development of sensor particles for remote detection of trace chemical analytes over broad areas, e.g residual trinitrotoluene from buried landmines or other unexploded ordnance (UXO). We also describe the potential of the sensor particle approach for the detection of chemical warfare (CW) agents. The primary goal of this work has been the development of sensor particles that incorporate sample preconcentration, analyte molecular recognition, chemical signal amplification, and fluorescence signal transduction within a ''grain of sand''. Two approaches for particle-based chemical-to-fluorescence signal transduction are described: (1) enzyme-amplified immunoassays using biocompatible inorganic encapsulants, and (2) oxidative quenching of a unique fluorescent polymer by TNT.

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37 Results
37 Results