The resonance enhanced Raman spectra in the 1B2u mode of the forbidden benzene electronic transition band, ~230-270 nm, has been investigated. Resonance enhanced Raman scattering in both liquid benzene and liquid toluene exhibit the greatest enhancement when the wavelength of excitation is tuned to the vapor-phase absorption peaks; even though the sample volume is in a liquid state. Raman signals for the symmetric breathing mode of the carbon ring are found to be resonantly enhanced by several orders of magnitude (>500X) with deep UV excitation compared to non-resonant visible excitation. Since the benzene absorbs near this resonant wavelength, its effect on the sampled volume cannot be neglected in determining the resonance gain, as we discuss in detail. Large resonant gains correspond with excitation at the 247, 253, and 259 nm absorption peaks in the benzene vapor spectrum. The narrow region of resonance gain is investigated in detail around the absorption peak located at 259 nm using 0.25 nm steps in the excitation wavelength. We observe the resonance gain tracking the vapor phase absorption peaks and valleys within this narrow range. Results are interpreted in terms of the coherence forced by the use of a forbidden transition for resonance excitation.

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The magnitude of resonance Raman intensity, in terms of the real signal level measured on-resonance compared to the signal level measured off-resonance for the same sample, is investigated using a tunable laser source. Resonance Raman enhancements, occurring as the excitation energy is tuned through ultraviolet absorption lines, are used to examine the 1332 cm−1 vibrational mode of diamond and the 992 cm−1 ring-breathing mode of benzene. Competition between the wavelength dependent optical absorption and the magnitude of the resonance enhancement is studied using measured signal levels as a function of wavelength. Two system applications are identified where the resonance Raman significantly increases the real signal levels despite the presence of strong absorption: characterization of trace species in laser remote sensing and spectroscopy of the few molecules in the tiny working volumes of near-field optical microscopy.

This paper presents the first, to our knowledge, direct measurement of aerosol produced by an aluminized solid rocket propellant (SRP) fire on the ground. Such fires produce aluminum oxide particles small enough to loft high into the atmosphere and disperse over a wide area. These results can be applied to spacecraft launchpad accidents that expose spacecraft to such fires; during these fires, there is concern that some of the plutonium from the spacecraft power system will be carried with the aerosols. Accident-related lofting of this material would be the net result of many contributing processes that are currently being evaluated. To resolve the complexity of fire processes, a self-consistent model of the ground-level and upper-level parts of the plume was determined by merging ground-level optical measurements of the fire with lidar measurements of the aerosol plume at height during a series of SRP fire tests that simulated propellant fire accident scenarios. On the basis of the measurements and model results, the Johns Hopkins University Applied Physics Laboratory (JHU/APL) team was able to estimate the amount of aluminum oxide (alumina) lofted into the atmosphere above the fire. The quantification of this ratio is critical for a complete understanding of accident scenarios, because contaminants are transported through the plume. This paper provides an estimate for the mass of alumina lofted into the air.

Measurements obtained by the PSU Lidar Atmospheric Profile Sensor (LAPS) Raman lidar, during different periods, provide a comprehensive dataset to characterize cloud properties and aerosol distributions. The PSU Raman lidar measures the profiles of molecular nitrogen, molecular oxygen and the rotational Raman scatter (the mixture of all molecular species) at both visible and ultraviolet wavelengths, which are then used to generate vertical aerosol extinction profiles from the incremental extinction. Since the optical extinction at different wavelengths is strongly dependent on the size distribution of aerosols, variations in the profile of the size distribution can be inferred over an interesting range corresponding to accumulation mode particles, 50 nm to 1µm. The variation in the extinction profiles at different wavelengths is also used along with the water vapor profiles to observe the formation, growth and dissipation of cloud structures. The water vapor concentrations have been seen to decrease in regions surrounding a growing cloud as the particles increase in size by absorbing the water. Also, the water vapor concentration is found to increase as clouds begin to dissipate. The change in the size of the cloud particles during the different stages can also be observed in the multi-wavelength aerosol extinction. Results obtained from different locations, and for a wide range of atmospheric conditions, are used to compare and contrast the aerosol distributions and also to study the physical properties of clouds.