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We have recently made advancements in a linear electrodynamic quadrupole (LEQ) device for capturing and levitating either single or multiple micro-particles that provides significant improvements in capture efficiency, reliability, and optical measurement access. We have used our LEQ to trap particles ranging from 30 to less than 0.5 μm in size and provide a controlled environment to study particle physical/chemical dependencies on temperature, relative humidity, and gas constituents. To demonstrate this approach, we present data and analysis of liquid-droplet evaporation rates for two materials: glycerol and dibutyl sebacate. Droplet size was monitored as a function of time by two independent optical methods: direct imaging and fixed-angle light scattering. This new approach provides a means to rapidly characterize a wide range of aerosol particle properties and a platform for development of new aerosol optical-diagnostic measurements.

Fluorescence spectra from individual aerosol particles that were either coated or embedded with metallic nanoparticles (MNPs) was acquired on-the-fly using 266 nm and 355 nm excitation. Using aqueous suspensions of MNPs with either polystyrene latex (PSL) spheres or dissolved proteins (tryptophan or ovalbumin), we generated PSL spheres coated with MNPs, or protein clusters embedded with MNPs as aerosols. Both enhanced and quenched fluorescence intensities were observed as a function of MNP concentration. Optimizing MNP material, size and spacing should yield enhanced sensitivity for specific aerosol materials that could be exploited to improve detection limits of single-particle, on-the-fly fluorescence or Raman based spectroscopic sensors.

A novel liquid injection vapor generator (LIVG) is demonstrated that is amenable to low vapor pressure explosives, 2,4,6-trinitrotoluene and hexahydro-1,3,5-trinitro-1,3,5-triazine. The LIVG operates in a continuous manner, providing a constant and stable vapor output over a period of days and whose concentration can be extended over as much as three orders of magnitude. In addition, a large test atmosphere chamber attached to the LIVG is described, which enables the generation of a stable test atmosphere with controllable humidity and temperature. The size of the chamber allows for the complete insertion of testing instruments or arrays of materials into a uniform test atmosphere, and various electrical feedthroughs, insertion ports, and sealed doors permit simple and effective access to the sample chamber and its vapor.

A method for controlled generation of composite aerosol particles is achieved by coating a core particle material, such as glass or polymer beads, with a second (analyte) material on the core surface. The mass fraction of the analyte can be varied over a wide range to generate resultant composite aerosol particles, which for the low end of analyte mass fractions has little influence on the particle size, but can be varied up to mass fractions nearly equivalent to the core material, as demonstrated in this paper. Analysis of this method was carried out using fluorescent analyte and core particle materials in separable spectral bands to measure both particle size distributions and fluorescent emission distributions on individual particle basis.

A two-wavelength laser-induced fluorescence (LIF) instrument has been developed and used to characterize individual biological aerosol particles, including biological warfare (BW) agent surrogates. Fluorescence in discrete spectral bands from widely different species, and also from similar species under different growth conditions were measured and compared. The two-wavelength excitation approach was found to increase discrimination among several biological materials, and especially with respect to diesel exhaust particles, a common interferent for LIF BW detection systems. The spectral characteristics of a variety of biological materials and ambient air components have been studied as a function of aerosol particle size and incident fluence.

We use a compact chirped-pulse amplified system to harmonically generate ultrashort pulses for aerosol fluorescence measurements. The seed laser is a compact, all-normal dispersion, mode-locked Yb-doped fiber laser with a 1050 nm center wavelength operating at 41 MHz. Average powers of more than 1.2 W at 525 nm and 350 mW at 262 nm are generated with <500 fs pulse durations. The pulses are time-stretched with high-dispersion fiber, amplified by a high-power, large-mode-area fiber amplifier, and recompressed using a chirped volume holographic Bragg grating. The resulting high-peak-power pulses allow for highly efficient harmonic generation. We also demonstrate for the first time to our knowledge, the use of a mode-locked ultraviolet source to excite individual biological particles and other calibration particles in an inlet air flow as they pass through an optical chamber. The repetition rate is ideal for biofluorescence measurements as it allows faster sampling rates as well as the higher peak powers as compared to previously demonstrated Q-switched systems while maintaining a pulse period that is longer than the typical fluorescence lifetimes. Thus, the fluorescence excitation can be considered to be quasicontinuous and requires no external synchronization and triggering.

We report results of scattering measurements using femtosecond pulses to collect a wealth of information in a single experiment. Potential issues with particle scattering, such as variation in particle size, were avoided by using 9 and 50 microm diameter glass fibers. We first establish an angular scattering intensity baseline, and we show that the spectral width of very short pulses leads to smoothing of the angular scattering pattern, consistent with continuous broadband illumination. We then measure the angular scattering pattern from short pulses with a spectrometer and reveal an underlying spectral periodicity of broadband scattered light that is consistent with narrowband cw scattering. Our experimental results compare well with existing theory. We show that such two-dimensional experimental data and derived analytic solution can provide robust characterization of scattering objects even in the presence of noise.

We describe the development and performance evaluation of a system for optical interrogation, subsequent selection, and collection of individual aerosol particles entrained in an inlet air stream. Elastic scatter and laser-induced fluorescence obtained from single particles on-the-fly provide compositional information for classification criteria. Individual particles could then be selectively electrically charged and captured to a conductive substrate with an electric potential. The optical subsystem also includes a novel two-beam velocimeter to provide accurate downstream timing. Good overall quantitative performance values are reported for particles in the size range of 1-8 microm at mean rates up to 4 kHz.

The elastic-scattering intensity pattern from a single particle as a function of spherical coordinate angles theta and phi provides detailed information on the pattern's morphology. By use of an ellipsoidal reflector and a CCD camera, a single-laser-shot intensity pattern from a large angular range (theta from 90 degrees to 168 degrees and phi from 0 degrees to 360 degrees) was detected from a single aerosol (e.g., a Bacillus subtilisspore, a 1-microm-diameter polystyrene latex sphere, or a cluster of either of these) flowing through the reflectors focal volume at 5 m/s. Noticeable difference in the large-angle-range two-dimensional angular optical scattering (LATAOS) suggest that the LATAOS pattern could be useful in differentiating and classifying life-threatening aerosols from normal background aerosols.

Van de Hulst's localization principle relates the principal mode number to the external beam position that maximizes energy coupling to a spherical cavity mode. Our experiments in lasing microdroplets verify localization but only for low- Q modes, when the cavity may be considered to be a nearly perfect homogeneous sphere. The principle fails in the perturbation-dominated high- Q limit. Surprisingly, near-surface resonances are still efficiently excited in these cases but require impact parameters slightly smaller than the sphere radius. Numerical modeling suggests that this new input channel depends on surface scattering.

Spectrally resolved emission (270-560 nm) from dilute suspensions of washed Bacillus subtilis and Escherichia coli were measured by use of tunable laser excitation between 270 and 300 nm. Integrated absolute emission cross sections increase with decreasing excitation wavelength and range from 1.8 x 10(-12) to 6.0 x 10(-11) cm(2)/(particle sr). An emission band near 340 nm dominates all observed spectra. At each excitation wavelength spectrally resolved emissions from the E. coli and B. subtilis suspensions are indistinguishable.

Continuous-wave stimulated Raman scattering was observed in 11-13-microm-diameter benzene and toluene microdroplets at pump intensities as low as 8 and 24 kW/cm(2), respectively. Low thresholds were achieved by exploiting simultaneous pump and Stokes wave resonance in the droplets and Raman gains that were cavity QED enhanced ~50 times with respect to bulk liquid values. Based on a photon-state conservation argument, the cavity gain enhancement factor may be approximated by the ratio of the spectral spacing between resonant modes of the same order to that of the homogeneous Raman linewidth. This relation appears to be consistent with the relative experimental behavior of benzene, ethanol, and toluene.

The effect of absorption on microdroplet resonance emission line intensities was studied in 15-microm-diameter Rhodamine 6G/ethanol solution droplets. Absorption was controlled by varying the concentration of the additive nigrosin. Spectrally integrated intensities of resonant features are found to be proportional to a droplet cavity mode efficiency Q(a)/(Q(a)+Q(o)) expressed in terms of cavity output coupling and absorption factors Q(o) and Q(a), respectively. These Q's are determined from linewidths calculated from Lorenz-Mie theory by using combinations of the real and complex indices of refraction. An experimental upper limit of Q for first-order modes was determined to be 10(8) from the data.

Nonlinear Mie scattering at 532 nm was observed from 23-microm-diameter ethanol droplets excited by picosecond light pulses. Low-order optical modes (l = 2-4), normally hidden at low intensity, became visible as new peaks in elastic scattering spectra at 2 GW/cm(2). When higher-Q resonances were selectively excited, the scattered light showed an amplitude-modulated time dependence. The data are explained by electrostrictive generation of acoustic modes of the droplet by the incident radiation and subsequent coupling of the acoustic disturbance back onto the light field.

Spectral features observed in stimulated Raman scattering from 20-microm methanol droplets at 1-GW/cm(2) pumping levels appeared locked in wavelength at the center of their respective gain profiles. Typically, a feature's wavelength remained constant while the droplet size varied by as much as 0.3%. This is attributed to frequency-pulling effects caused by the presence of Raman gain. Wavelength shifts of up to +/-0.5 nm in the positions of morphologydependent resonances would explain the observations and are consistent with calculations.

Experimental elastic-scattering characteristics of layered microspheres are reported. Single particles consisting of glass cores coated with glycerine are suspended in an evacuated quadrupole trap, and scattered light intensity is measured at a fixed angle as the glycerine evaporates. The results are compared with those calculated for concentric spheres using the Mie theory. Excellent agreement is obtained for glycerine layers of thickness less than 700 nm. For thicker layers, differences occur that are attributed to the effect of gravity on particle structure.