Continuous condensation particle (CP) observations were conducted from 1984 through 2009 at Neumayer Station under stringent contamination control. During this period, the CP concentration (median 258 cm−3) showed no significant long term trend but exhibited a pronounced seasonality characterized by a stepwise increase starting in September and reaching its annual maximum of around 103 cm−3 in March. Minimum values below 102 cm–3 were observed during June/July. Dedicated time series analyses in the time and frequency domain revealed no significant correlations between inter-annual CP concentration variations and atmospheric circulation indices like Southern Annular Mode (SAM) or Southern Ocean Index (SOI). The impact of the Pinatubo volcanic eruption and strong El Niño events did not affect CP concentrations. From thermodenuder experiments we deduced that the portion of volatile (at 125 °C) and semi-volatile (at 250 °C) particles which could be both associated with biogenic sulfur aerosol, was maximum during austral summer, while during winter non-volatile sea salt particles dominated. During September through April we could frequently observe enhanced concentrations of ultrafine particles within the nucleation mode (between 3 nm and 7 nm particle diameter), preferentially in the afternoon.
Number concentrations of total and non-volatile aerosol particles with size diameters >0.01 μm as well as particle size distributions (0.4–23 μm diameter) were measured in situ in the Arctic lower stratosphere (10–20.5 km altitude). The measurements were obtained during the campaigns European Polar Stratospheric Cloud and Lee Wave Experiment (EUPLEX) and Envisat-Arctic-Validation (EAV). The campaigns were based in Kiruna, Sweden, and took place from January to March 2003. Measurements were conducted onboard the Russian high-altitude research aircraft Geophysica using the low-pressure Condensation Nucleus Counter COPAS (COndensation PArticle Counter System) and a modified FSSP 300 (Forward Scattering Spectrometer Probe). Around 18–20 km altitude typical total particle number concentrations nt range at 10–20 cm−3 (ambient conditions). Correlations with the trace gases nitrous oxide (N2O) and trichlorofluoromethane (CFC-11) are discussed. Inside the polar vortex the total number of particles >0.01 μm increases with potential temperature while N2O is decreasing which indicates a source of particles in the above polar stratosphere or mesosphere. A separate channel of the COPAS instrument measures the fraction of aerosol particles non-volatile at 250°C. Inside the polar vortex a much higher fraction of particles contained non-volatile residues than outside the vortex (~67% inside vortex, ~24% outside vortex). This is most likely due to a strongly increased fraction of meteoric material in the particles which is transported downward from the mesosphere inside the polar vortex. The high fraction of non-volatile residual particles gives therefore experimental evidence for downward transport of mesospheric air inside the polar vortex. It is also shown that the fraction of non-volatile residual particles serves directly as a suitable experimental vortex tracer. Nanometer-sized meteoric smoke particles may also serve as nuclei for the condensation of gaseous sulfuric acid and water in the polar vortex and these additional particles may be responsible for the increase in the observed particle concentration at low N2O. The number concentrations of particles >0.4 μm measured with the FSSP decrease markedly inside the polar vortex with increasing potential temperature, also a consequence of subsidence of air from higher altitudes inside the vortex. Another focus of the analysis was put on the particle measurements in the lowermost stratosphere. For the total particle density relatively high number concentrations of several hundred particles per cm3 at altitudes below ~14 km were observed in several flights. To investigate the origin of these high number concentrations we conducted air mass trajectory calculations and compared the particle measurements with other trace gas observations. The high number concentrations of total particles in the lowermost stratosphere are probably caused by transport of originally tropospheric air from lower latitudes and are potentially influenced by recent particle nucleation.
Aircraft inlets connect airborne instruments for particle microphysical and chemical measurements with the ambient atmosphere. These inlets may bias the measurements due to their potential to enhance or remove certain particle size fractions in the sample. The aircraft body itself may disturb the ambient air streamlines and, hence, the particle sampling. Also, anisokinetic sampling and transmission losses within the sampling lines may cause the sampled aerosol to differ from the ambient aerosol. In addition, inlets may change the particle composition and size through the evaporation of water and other volatile materials due to compressibility effects or heat transfer. These problems have been discussed at an international workshop that was held at the Leibniz-Institute for Tropospheric Research (IfT) in Leipzig, Germany, on 12–13 April 2002. The discussions, conclusions, and recommendations from this workshop are summarized here.
Rapid particle growth by the condensation of water vapour resulting from expansion in the inlet of particle sizing instruments such as optical particle counters and impactors was modelled. The corrected Mason diffusion growth equation extended to the application for particles beyond the continuum region has been found suitable. The influence of particle acceleration in the nozzle air flow, modelled with the CFX-FLOW3D program, on the condensation process was considered. The study was focused on a typical inlet nozzle of an optical particle counter with an inner diameter of 0.5 mm and a length of 20 mm, connected by an additional 20 mm long conical nozzle at a flow rate of 28.5mls−1. The results show that particles smaller than 1.0μm can grow quickly during the very short-time passage through the nozzle as the saturation in the nozzle flow can increase several times. For particles with an initial radius of 0.15μm, i.e. the typical minimum detectable size of many commercial optical particle sizing instruments, condensational growth will cause a size increase up to 7% in the viewing volume. The whole particle size distribution will shift to larger radii, which results in an overestimate of both particle size and number in measurements. This condensational over-numbering and sizing effect should be given concern in evaluating measurement results as well as in aerosol instrument design.
During the 1997 POLSTAR‐1 winter campaign in northern Sweden a flight was performed across a cold trough of air (≃ 196 K) in the tropopause region. Measurements of total water vapour, nitric acid, particles and reactive nitrogen (NOy) were taken. The particle measurements indicate that about 3% of the particles in the moist tropospheric air were ice particles. Forward and backward facing NOy inlets were used simultaneously to determine condensed phase HNO3. The combined NOy and particle measurements reveal that less than 1% of a monolayer of NOy could have resided on the ice particles. This casts doubt on the hypothesis that sedimenting cirrus particles generally lead to a strong downward flux of NOy. In addition to the NOy measurements, independent HNO3 measurements were used to determine total HNO3. Although quantitative uncertainties do not allow to completely rule out that the NOy uptake on ice was limited by total HNO3, the combined NOy and HNO3 data suggest that there was low uptake of NOy on ice despite abundant HNO3 in the gas phase. Model studies indicate, that the most likely explanation of the measured nitric acid partitioning is given by HNO3 in ternary solution droplets coexisting with almost HNO3 free ice in the same air mass.