Hygroscopic growth of atmospheric aerosol particles based on active remote sensing and radiosounding measurements: selected cases in southeastern Spain

A new methodology based on combining active and passive remote sensing and simultaneous and collocated radiosounding data to study the aerosol hygroscopic growth effects on the particle optical and microphysical properties is presented. The identification of hygroscopic growth situations combines the analysis of multispectral aerosol particle backscatter coefficient and particle linear depolarization ratio with thermodynamic profiling of the atmospheric column. We analyzed the hygroscopic growth effects on aerosol properties, namely the aerosol particle backscatter coefficient and the volume concentration profiles, using data gathered at Granada EARLINET station. Two study cases, corresponding to different aerosol loads and different aerosol types, are used for illustrating the potential of this methodology. Values of the aerosol particle backscatter coefficient enhancement factors range from 2.1 ± 0.8 to 3.9 ± 1.5, in the ranges of relative humidity 60–90 and 40–83%, being similar to those previously reported in the literature. Differences in the enhancement factor are directly linked to the composition of the atmospheric aerosol. The largest value of the aerosol particle backscatter coefficient enhancement factor corresponds to the presence of sulphate and marine particles that are more affected by hygroscopic growth. On the contrary, the lowest value of the enhancement factor corresponds to an aerosol mixture containing sulphates and slight traces of mineral dust. The Hänel parameterization is applied to these case studies, obtaining results within the range of values reported in previous studies, with values of the γ exponent of 0.56 ± 0.01 (for anthropogenic particles slightly influenced by mineral dust) and 1.07 ± 0.01 (for the situation dominated by anthropogenic particles), showing the convenience of this remote sensing approach for the study of hygroscopic effects of the atmospheric aerosol under ambient unperturbed conditions. For the first time, the retrieval of the volume concentration profiles for these cases using the Lidar Radiometer Inversion Code (LIRIC) allows us to analyze the aerosol hygroscopic growth effects on aerosol volume concentration, observing a stronger increase of the fine mode volume concentration with increasing relative humidity.

Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2:5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 μm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60–91 %) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved longterm data sets.

Isotope signature of the Younger Dryas and two minor oscillations at Gerzensee (Switzerland): palaeoclimatic and palaeolimnologic interpretation based on bulk and biogenic carbonates

Oxygen- and carbon-isotope ratios in the carbonate of benthic ostracodes (Pseudocandona marchica) and molluscs (Pisidium ssp.) were measured across the transitions bordering the Younger Dryas chronozone in littoral lacustrine cores from Gerzensee (Switzerland). The specific biogenic carbonate records confirm the major shifts already visible in the continuous bulk-carbonate oxygen-isotope record (δ18OCc). If corrected for their vital offsets, oxygen-isotope ratios of Pisidium and juvenile P. marchica, both formed in summer, are almost identical to δ18OCc. This bulk carbonate is mainly composed of encrustations of benthic macrophythes (Chara ssp.), also mainly produced during summer. Adult P. marchica, which calcify in winter, show consistently higher δ18O, larger shifts across both transitions, and short positive excursions compared with the summer forms, especially during early Preboreal. Despite such complexity, the δ18O of adult P. marchica probably reflects more accurately the variations of the δ18O of former lake water because, during winter, calcification temperatures are less variable and the water column isotopically uniform. The difference between normalised δ18O of calcite precipitated in winter to that formed in summer can be used to estimate the minimum difference between summer and winter water temperatures. In general, the results indicate warmer summers during the late Allerød and early Preboreal compared with the Younger Dryas. Altogether, the isotopic composition of lake water (δ18OL) and of the dissolved inorganic carbonate (δ13CDIC) reconstructed from adult Pseudocandona marchica, as well as the seasonal water temperature contrasts, indicate that the major shifts in the δ18O of local precipitation at Gerzensee were augmented by changes of the lake's water balance, with relatively higher evaporative loss occurring during the Allerød compared with the Younger Dryas. It is possible that during the early Preboreal the lake might even have been hydrologically closed for a short period. We speculate that such hydrologic changes reflect a combination of varying evapotranspiration and a rearrangement of groundwater recharge during those climatic shifts.