Single particle characterization of black carbon aerosols at a tropospheric alpine site in Switzerland

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Abstract

The refractory black carbon (rBC) mass, size distribution (190ĝ€"720 nm) and mixing state in sub-micron aerosols were characterized from late February to March 2007 using a single particle incandescence method at the high alpine research station Jungfraujoch (JFJ), Switzerland (46.33° N, 7.59° E, 3580 m a.s.l.). JFJ is a ground based location, which is at times exposed to continental free tropospheric air. A median mass absorption coefficient (MAC) of 10.2±3.2 m2 g-'1 at;lambda;=Combining double low line630 nm was derived by comparing single particle incandescence measurements of black carbon mass with continuous measurements of absorption coefficient. This value is comparable with other estimates at this location. The aerosols measured at the site were mostly well mixed and aged during transportation via the free troposphere. Pollutant sources were traced by air mass back trajectories, trace gases concentrations and the mass loading of rBC. In southeasterly wind directions, mixed or convective weather types provided the potential to vent polluted boundary layer air from the southern Alpine area and industrial northern Italy, delivering enhanced rBC mass loading and CN concentrations to the JFJ. The aerosol loadings at this site were also significantly influenced by precipitation, which led to the removal of rBC from the atmosphere. Precipitation events were shown to remove about 65% of the rBC mass from the free tropospheric background reducing the mean loading from 13±5 ng mg-'3 to 6±2 ng mg-'3(corrected to standard temperature and pressure). Overall, 40±15% of the observed rBC particles within the detectable size range were mixed with large amounts of non-refractory materials present as a thick coating. The growth of particle size into the accumulation mode was positively linked with the degree of rBC mixing, suggesting the important role of condensable materials in increasing particle size and leading to enhanced internal mixing of these materials with rBC. It is the first time that BC mass, size distribution and mixing state are reported in the free troposphere over Europe. These ground based measurements also provide the first temporal study of rBC in the European free troposphere quantitatively measured by single particle methods. At the present time there is only limited information of BC and its mixing state in the free troposphere, especially above Europe. The results reported in this paper provide an important constraint on modelled representation of BC. © 2010 Author(s).

Figures

  • Fig. 1. The experimental site was influenced by air mass history and local wind direction (A1–A5), back trajectory analysis calculated by NOAA Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT; Draxler, 2003). Time periods are classified according to the history of the air mass over the previous three days. Back trajectories are shown for arrival at 3400 m, 3600 m and 3800 m a.s.l. over the Jungfraujoch, labelled by the arriving date and are coloured by air pressure. (B) Wind rose plot for the whole experiment period, individual wind direction measurements are accumulated and the relative frequency is shown as a percentage. The plot is coloured according to the probability of wind speed.
  • Table 1. The 3 basic and 8 extended types of the Alpine weather statistics and their dominant synoptic scale motion.
  • Fig. 2. Time series of total rBC mass loading from the SP2 and absorption coefficient measured by the Multi-Angle Absorption Photometer (MAAP) for the entire experiment. The five synoptic periods classified by back trajectory analysis (Fig. 1, A1–A5) are separated by dotted lines. The top text line indicates the recognized weather types as detailed in Table 1, with arrows denoting respective periods. Particularly, the time periods when the dominant horizontal wind direction is southeast (SE) are coloured as yellow columns; the dark blue columns mark the periods of heavy precipitation (heavy snow, precipitation particle concentration over 200 L−1) as recorded by a present weather sensor.
  • Fig. 3 Fig. 3. (A) Correlation between absorption coefficient measured using the MAAP and total rBC mass loading measured using the SP2, plotted in logarithmic scale (left) and linear scale (right) respectively. The linear regression line and parameters are shown on the linear scale plot. (B) Probability distribution of derived mass absorption cross section (MAC).
  • Fig. 4. (A) Two examples of detected rBC in single particles, both having the same size of rBC core but the left one is less or relatively thinly coated compared to the thickly coated one on the right. (B) the refractory mass fraction related to the coating evaporation time, the upper and right lines show the histograms of x-axis and y-axis values respectively, units are particle counts. The definitions of thickly-coated and thinly-coated BC are illustrated.
  • Fig. 5. Fig. 5. The relationship between BC mixing efficiency over the entire size range of the SP2 and at the median diameter (190–210 nm).
  • Fig. 6. Fig. 6. (A) Time series of aerosol properties during the entire experiment with the classified periods separated by dotted lines, from bottom to top: numerical ratio of sub-micron/accumulation mode particles as measured by the SP2; BC mixing efficiency; CN concentration measured by the CPC; rBC number fraction within the population of sub-micron aerosols. (B) Time series of trace gases, from bottom to top: NOx volume mixing ratio (ppbv); CO volume mixing ratio (ppbv); BC/1CO (ng m−3 ppbv−1).
  • Table 2. A summary of meteorological conditions and aerosol properties categorized by five periods classified by back trajectory analysis (Fig. 1, A1–A5). The mean and standard deviations are shown for each parameter and the number in brackets is median value.

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CITATION STYLE

APA

Liu, D., Flynn, M., Gysel, M., Targino, A., Crawford, I., Bower, K., … Coe, H. (2010). Single particle characterization of black carbon aerosols at a tropospheric alpine site in Switzerland. Atmospheric Chemistry and Physics, 10(15), 7389–7407. https://doi.org/10.5194/acp-10-7389-2010

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