Abstract. Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5-20 µm were separated from larger ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR) were analyzed for size and composition by the two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT) and a commercial Aerosol Time-of-Flight Mass Spectrometer (ATOFMS, TSI Model 3800). During CLACE 6 the SPLAT instrument characterized 355 individual IR that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 IR. The mass spectra were binned Correspondence to: J. Curtius (curtius@iau.uni-frankfurt.de) in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS) and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094). The measurements showed that mineral dust was strongly enhanced in the ice particle residues. Close to all of the SPLAT spectra from ice residues did contain signatures from mineral compounds, albeit connected with varying amounts of soluble compounds. Similarly, close to all of the ATOFMS IR spectra show a mineral or metallic component. Pure sulfate and nitrate containing particles were depleted in the ice residues. Sulfate and nitrate was found to dominate the droplet residues (∼90% of the particles). The results from the two different single particle mass spectrometers were generally in agreement. Differences in the results originate from several causes, such as the different wavelength of the desorption and ionisation lasers and different size-dependent particle detection efficiencies.
Abstract. Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5 μm up to 20 μm were separated from large ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR) were analyzed for size and composition by two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT) and a commercial Aerosol Time of Flight Mass Spectrometer (ATOFMS, TSI Model 3800). During CLACE 6 the SPLAT instrument characterized 355 individual ice residues that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 particles. The mass spectra were binned in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS) and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094). The measurements showed that mineral dust particles were strongly enhanced in the ice particle residues. 57% of the SPLAT spectra from ice residues were dominated by signatures from mineral compounds, and 78% of the ATOFMS spectra. Sulfate and nitrate containing particles were strongly depleted in the ice residues. Sulfate was found to dominate the droplet residues (~90% of the particles). The results from the two different single particle mass spectrometers were generally in agreement. Differences in the results originate from several causes, such as the different wavelength of the desorption and ionisation lasers and different size-dependent particle detection efficiencies.
By means of a newly designed portable aerosol mass spectrometer SPLAT (Single Particle Laser Ablation Time-of-flight mass spectrometer) for the analysis of single atmospheric aerosol particles we investigated the system performance in dependency on two different aerodynamic lenses (Liu and Schreiner type) capable of focusing particles with diameters ranging from 80 nm to 800 nm and 300 nm to 3000 nm, respectively. By using the pressure regulated Schreiner lens, the instrument is independent of variations in atmospheric pressure which would lead to changing dynamical properties of the aerosol particles. Active pressure control inside the inlet system facilitates airborne measurements without complicated corrections. With the Liu setup no pressure regulation was used. Here the overall efficiency of our instrument was 7% while with the Schreiner setup 2% was achieved. The Liu lens setup is optimal for measuring submicron particles at low particle concentrations. To detect supermicron particles the Schreiner lens setup is favored. Together with these experiments we present key details of the SPLAT setup and its characterization. Our instrument is able to measure simultaneously the size and the chemical composition of individual aerosol particles larger than 300 nm in diameter. It uses forward scattered light of single aerosol particles at two positions to determine their vacuum aerodynamic diameter from the flight time between the two lasers. Chemical analysis of the particles is done by laser ablation mass spectrometry utilizing a bipolar time-of-flight mass spectrometer.
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