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We describe here the instrumental setup and first experiments with the mobile single particle analysis and sizing system (SPASS) for the on-line characterization of single atmospheric aerosol particles. Aerosols are introduced into the SPASS via a differentially pumped particle inlet system using an aerodynamic lens that forms a narrow particle beam. The particles are sized with a two-laser velocimeter and subsequently desorbed and ionized with a highpower pulsed Nd:YAG laser operating at 266 nm. Positive and negative ions formed are simultaneously detected in a bipolar time-offlight mass spectrometer. Thus, the size and chemical composition of single aerosol particles can be characterized simultaneously in real time. The SPASS system has been installed inside a truck, creating a mobile unit. The performance of the SPASS in terms of mass resolution and sizing capabilities of the laser velocimeter has been evaluated. Positive and negative mass spectra from different types of particles have been obtained to identify "typical" peak patterns. The relative detection sensitivity depending on particle size and chemical composition was studied. Significant differences in detection sensitivities for different compounds were observed, demonstrating that the results obtained from ambient single particle measurements are strongly biased and dominated by "easy-to-detect" particles. The instrument performance is illustrated with results from a 24 h measurement period during winter in Milan, Italy. The period encompasses two meteorologically different episodes, a period of stagnant conditions, where regional background pollutants contribute significantly and the aerosol is dominated by ammonium nitrate and sulfate, and a North-Foehn event, where accumulation mode particles are scavenged and the urban aerosol population is dominated by organic matter due to local emissions. INTRODUCTIONThe importance of aerosols in chemical and physical processes involved in, for example, air pollution (human health, acid deposition, and global warming), combustion (soot and soot precursors), materials synthesis and processing (nanoparticles and coatings), and clean-room technology has increased dramatically in the past years. Their physical and chemical characterization and the study of their composition and reaction mechanisms represent an area in which basic information is still needed (Andreae and Crutzen 1997). It has become important not only to perform bulk analysis of aerosol particles but also to be able to analyze single aerosol particles, on-line in real time (Peter 1996). This capability will allow us in particular to investigate the mixing state of the particles. In an internally mixed aerosol, all particles have roughly the same chemical composition, which can be a mixture of inorganic and organic components. Externally mixed particles show chemically different subpopulations, e.g., with a fraction of the particles dominated by organic compounds and another fraction dominated by inorganic compounds. The mixing state is of relevan...

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In order to prevent nuclear proliferation, the isotopic analysis of uranium and plutonium microparticles has strengthened the means in international safeguards for detecting undeclared nuclear activities. In order to ensure accuracy and precision in the analytical methodologies used, the instrumental techniques need to be calibrated. The objective of this study was to produce and characterize particles consisting of U, Pu, and mixed U-Pu, suitable for such reliability verifications. A TSI vibrating orifice aerosol generator in connection with a furnace system was used to produce micrometer sized, monodispersed particles from reference U and Pu materials in solution. The particle masses (in the range of 3-6 pg) and sizes (approximately 1.5 microm) were controlled by the experimental conditions and the parameters for the aerosol generator. Size distributions were obtained from scanning electron microscopy, and energy-dispersive X-ray analysis confirmed that the particle composition agreed with the starting material used. A secondary ion mass spectrometer (SIMS) was used to characterize the isotopic composition of the particles. Isobaric and polyatomic interference in the SIMS spectra was identified. In order to obtain accurate estimates of the interference, a batch of Pu particles were produced of mainly (242)Pu. These were used for SIMS analysis to characterize the relative ionization of Pu and U hydride ions and to determine the SIMS useful yields of U and Pu. It was found that U had a higher propensity to form the hydride than Pu. Useful yields were determined at a mass resolution of 450 for U-Pu particles: (1.71 +/- 0.15) % for Pu and (0.72 +/- 0.06) % for U. For Pu particles: (1.65 +/- 0.14) % for Pu. This gave a relative sensitivity factor between U and Pu (RSF(U:Pu)) of 2.4 +/- 0.2. However, the RSF(U:Pu) showed large fluctuations during the sputtering time for each analyses of the mixed U-Pu particles, in the range of 1.9-3.4.