Jerold R. Bottiger

Measurement of polarized light interactions via the Mueller matrix.

A new instrument for rapid and accurate measurement of the Mueller matrix is described. Distinct measurements of all sixteen elements are made simultaneously and with an absolute accuracy of 1-5%. The instrument employs electrooptic modulators. Results are presented for several simple optical devices and systems.

Fluorescence from airborne microparticles: dependence on size, concentration of fluorophores, and illumination intensity.

We measured fluorescence from spherical water droplets containing tryptophan and from aggregates of bacterial cells and compared these measurements with calculations of fluorescence of dielectric spheres. The measured dependence of fluorescence on size, from both droplets and dry-particle aggregates of bacteria, is proportional to the absorption cross section calculated for homogeneous spheres containing the appropriate percentage of tryptophan. However, as the tryptophan concentration of the water droplets is increased, the measured fluorescence from droplets increases less than predicted, probably because of concentration quenching. We model the dependence of the fluorescence on input intensity by assuming that the average time between fluorescence emission events is the sum of the fluorescence lifetime and the excitation lifetime (the average time it takes for an illuminated molecule to be excited), which we calculated assuming that the intensity inside the particle is uniform. Even though the intensity inside the particles spatially varies, this assumption of uniform intensity still leads to results consistent with the measured intensity dependence.

Fluorescence spectra of atmospheric aerosol particles measured using one or two excitation wavelengths: comparison of classification schemes employing different emission and scattering results.

An improved Dual-wavelength-excitation Particle Fluorescence Spectrometer (DPFS) has been reported. It measures two fluorescence spectra excited sequentially by lasers at 263 nm and 351 nm, from single atmospheric aerosol particles in the 1-10 mum diameter size range. Here we investigate the different levels of discrimination capability obtained when different numbers of excitation and fluorescence-emission wavelengths are used for analysis. We a) use the DPFS to measure fluorescence spectra of Bacillus subtilis and other aerosol particles, and a 25-hour sample of atmospheric aerosol at an urban site in Maryland, USA; b) analyze the data using six different algorithms that employ different levels of detail of the measured data; and c) show that when more of the data measured by the DPFS is used, the ability to discriminate among particle types is significantly increased.

Observations and calculations of light scattering from clusters of spheres.

Two-dimensional angular optical scattering (TAOS) patterns from clusters of polystyrene latex spheres are measured in the near-forward and near-backward directions. In both cases, the scattering pattern contains a rich and complicated structure that is the result of the interaction and interference of light among the primary particles. Calculations are made for aggregates that are similar to those generated experimentally and also demonstrate the rich structure in the scattering pattern. A comparison of the experimental and theoretical TAOS patterns gives good qualitative agreement.

Backward-enhanced fluorescence from clusters of microspheres and particles of tryptophan

Measured fluorescence from single-particle clusters of dye-doped polystyrene microspheres, dried nonspherical particles of tryptophan, and single polystyrene microspheres is enhanced in the backward direction (180 degrees from the incident laser). This enhancement (a factor of 2-3 compared to 90 degrees), which can be interpreted as a consequence of the reciprocity principle, increases with the particle refractive index.

Differential absorption Mueller matrix spectroscopy and the infrared detection of crystalline organics

The complete 16-element Mueller matrices for backscattering from amino acids, sugars, and other enantiomorphic compounds pressed into wafer form were measured at infrared wavelengths. For each compound a pair of CO(2) laser lines was selected from the 9.1-11.6-mum region such that one line excited an absorption band in the compound, whereas the other did not. It was observed that at least some of the matrix elements differed significantly depending on which of the two wavelengths was used in the measurement. We propose that a neural network pattern recognition system can be trained to detect the presence of specific compounds based on multiwavelength backscatter Mueller matrix measurements.

Phase Matrix Measurements for Electromagnetic Scattering by Sphere Aggregates

An instrument which permits accurate measurement of all elements of the phase matrix simultaneously has been constructed. Aggregates consisting of attached polystyrene spheres are suspended in an electric field and the phase matrix is measured.

Photopolarimetric lidar dual-beam switching device and Mueller matrix standoff detection method

We present an optomechanical switching device (OSD) for a photopolarimetric lidar system with differential-absorption Mueller matrix spectroscopy standoff detection method. An output train of alternate continuous-wave CO2 laser beams [...L1:L2...] is directed onto suspect chemical-biological (CB) aerosol plume or the land mass it contaminates (S) vis-à-vis the OSD, where L1 [L2] is tuned on [detuned off] a resonant molecular absorption moiety of CB analyte. Moreover, both incident beams and their backscattered radiances, from S, are polarization-modulated synchronously so as to produce gated temporal voltage waveforms called scattergrams recorded on focus at the receiver end of polarization lidar sensor system. All 16 elements of the Mueller matrix (Mij) of S are measured via digital or analog filtration of constituent frequency components in these running scattergram data streams (phase-sensitive detection). A collective set of normalized differential elements {ΔMi,j} (ratioed to element M11) that are susceptible to the analyte, probed on-then-off its molecular absorption band, form a unique detection domain that is scrutinized. Any mapping onto this domain in Mueller-space, from incoming sensor scattergram data sets preprocessed by algorithm and forwarded through a trained neural network pattern recognition system, cues a standoff detection event.

Concentration, size, and excitation power effects on fluorescence from microdroplets and microparticles containing tryptophan and bacteria

Our group has been developing a system for single-particle fluorescence detection of aerosolized agents. This paper describes the most recent steps in the evolution of this system. The effects of fluorophore concentrations, droplet size, and excitation power have also been investigated with microdroplets containing tryptophan in water to determine the effects of these parameters on our previous results. The vibrating orifice droplet generator was chosen for this study base don its ability to generate particles of well- known and reproducible size. The power levels required to reach saturation and photodegradation were determined. In addition, the collection of fluorescence emission was optimized through the use of a UV achromatic photographic lens. This arrangement permitted collection of images of the droplet stream. Finally, the use of a dual-beam, conditional firing scheme facilitated the collection of improved signal- to-noise single-shot spectra from individual biological particles.

Scattering Matrix Measurements Of Oceanic Hydrosols

Measurements have been made of the light scattering properties, including all polarization effects, ofoseveralocultured samples of phytoplankton. The range of scattering angles is from 8° to 168°. The measurements indicate the extent to which these phytoplankton may be regarded as spherical particles with respect to their light scattering properties.