An air ion spectrometer (AIS) was deployed for the first time at the Concordia station at Dome C (75 degrees 06'S, 123 degrees 23'E; 3220 ma.s.l.), Antarctica during the period 22 December 2010-16 November 2011 for measuring the number size distribution of air ions. In this work, we present results obtained from this air ion data set together with aerosol particle and meteorological data. The main processes that modify the number size distribution of air ions during the measurement period at this high-altitude site included new particle formation (NPF, observed on 85 days), wind-induced ion formation (observed on 36 days), and ion production and loss associated with cloud/fog formation (observed on 2 days). For the subset of days when none of these processes seemed to operate, the concentrations of cluster ions (0.9-1.9 nm) exhibited a clear seasonality, with high concentrations in the warm months and low concentrations in the cold. Compared to event-free days, days with NPF were observed with higher cluster ion concentrations. A number of NPF events were observed with restricted growth below 10 nm, which were termed as suppressed NPF. There was another distinct feature, namely a simultaneous presence of two or three separate NPF and subsequent growth events, which were named as multi-mode NPF events. Growth rates (GRs) were determined using two methods: the appearance time method and the mode fitting method. The former method seemed to have advantages in characterizing NPF events with a fast GR, whereas the latter method is more suitable when the GR was slow. The formation rate of 2 nm positive ions (J(2)(+)) was calculated for all the NPF events for which a GR in the 2-3 nm size range could be determined. On average, J(2)(+) was about 0.014 cm(-3) s(-1). The ion production in relation to cloud/fog formation in the size range of 8-42 nm seemed to be a unique feature at Dome C, which has not been reported elsewhere. These ions may, however, either be multiply charged particles but detected as singly charged in the AIS, or be produced inside the instrument, due to the breakage of cloud condensation nuclei (CCN), possibly related to the instrumental behaviour under the extremely cold condition. For the wind-induced ion formation, our observations suggest that the ions originated more likely from atmospheric nucleation of vapours released from the snow than from mechanical charging of shattered snow flakes and ice crystals.

Measuring aerosol size distributions accurately down to similar to 1 nm is a key to nucleation studies, and it requires developments and improvements in instruments such as electrical mobility spectrometers in use today. The key factors characterizing the performance of an electrical mobility spectrometer for sub-3 nm particles are discussed in this study. A parameter named as Pi is proposed as a figure of merit for the performance of an electrical mobility spectrometer in the sub-3 nm size range instead of the overall detection efficiency. Pi includes the overall detection efficiency, the measurement time in each size bin, the aerosol flow rate passing through the detector, and the aerosol-to-sheath flow ratio of the differential mobility analyzer. The particle raw count number recorded by the detector can be estimated using Pi at a given aerosol size distribution function, dN/dlogd(p)( ). The limit of detection for the spectrometer and the statistical uncertainty of the measured aerosol size distribution can also be readily estimated using Pi. In addition to Pi, the size resolution of an electrical mobility analyzer is another factor characterizing the systematic errors originated from particle sizing. Four existing electrical mobility spectrometers designed for measuring sub-3 nm aerosol size distributions, including three scanning/differential mobility particle spectrometers and one differential mobility analyzer train, are examined. Their optimal performance is evaluated using Pi and the size resolution. For example, the Pi value and the size resolution of a diethylene-glycol differential mobility particle spectrometer for 1.5 nm particles are 8.0 x 10(-4) cm(3) and 5.7, respectively. The corresponding relative uncertainty of the measured size distribution is approximately 9.6% during an atmospheric new particle formation event with a dN/dlogd(p) of 5 x 10(5) cm(-3) . Assuming an adjustable sheath flow rate of the differential mobility analyzer, the optimal size resolution is approximately 5-9 when measuring atmospheric new particle formation events.

Intense and frequent new particle formation (NPF) events have been observed in polluted urban environments, yet the dominant mechanisms are still under debate. To understand the key species and governing processes of NPF in polluted urban environments, we conducted comprehensive measurements in downtown Beijing during January-March, 2018. We performed detailed analyses on sulfuric acid cluster composition and budget, as well as the chemical and physical properties of oxidized organic molecules (OOMs). Our results demonstrate that the fast clustering of sulfuric acid (H2SO4) and base molecules triggered the NPF events, and OOMs further helped grow the newly formed particles toward climate- and health-relevant sizes. This synergistic role of H2SO4, base species, and OOMs in NPF is likely representative of polluted urban environments where abundant H2SO4 and base species usually co-exist, and OOMs are with moderately low volatility when produced under high NOx concentrations.

The vertical profile of new particle formation (NPF) events was studied by comparing the aerosol size number distributions measured aloft and at surface level in a suburban environment in Madrid, Spain, using airborne instruments. The horizontal distribution and regional impact of the NPF events was investigated with data from three urban, urban background, and suburban stations in the Madrid metropolitan area. Intensive regional NPF episodes followed by particle growth were simultaneously recorded at three stations in and around Madrid during a field campaign in July 2016. The urban stations presented larger formation rates compared to the suburban station. Condensation and coagulation sinks followed a similar evolution at all stations, with higher values at urban stations. However, the total number concentration of particles larger than 2.5 nm was lower at the urban station and peaked around noon, when black carbon (BC) levels are at a minimum. The vertical soundings demonstrated that ultrafine particles (UFPs) are formed exclusively inside the mixed layer. As convection becomes more effective and the mixed layer grows, UFPs are detected at higher levels. The morning soundings revealed the presence of a residual layer in the upper levels in which aged particles (nucleated and grown on previous days) prevail. The particles in this layer also grow in size, with growth rates significantly smaller than those inside the mixed layer. Under conditions with strong enough convection, the soundings revealed homogeneous number size distributions and growth rates at all altitudes, which follow the same evolution at the other stations considered in this study. This indicates that UFPs are detected quasi-homogenously in an area spanning at least 17 km horizontally. The NPF events extend over the full vertical extension of the mixed layer, which can reach as high as 3000 m in the area, according to previous studies. On some days a marked decline in particle size (shrinkage) was observed in the afternoon, associated with a change in air masses. Additionally, a few nocturnal nucleation-mode bursts were observed at the urban stations, for which further research is needed to elucidate their origin.