Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity
1Max Planck Institute for Chemistry, Biogeochemistry Department, Mainz, Germany
2Harvard University, School of Engineering and Applied Sciences & Department of Earth and Planetary Sciences, Cambridge, MA, USA
3Lund University, Nuclear Physics, Faculty of Technology, Lund, Sweden
4University of Colorado, Dept. of Chemistry & Biochemistry and CIRES, Boulder, CO, USA
5Instituto de Fisica, Universidade de Sao Paulo, Sao Paulo, Brazil
Abstract. Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10–0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ=0.05–0.45. The overall median value of κ≈0.15 was only half of the value typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≈0.1 at D≈50 nm; κ≈0.2 at D≈200 nm).
The CCN measurement results were fully consistent with aerosol mass spectrometry (AMS) data, which showed that the organic mass fraction (Xm,org) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≈200 nm). The κ values exhibited a close linear correlation with Xm,org and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≈0.1 which is consistent with laboratory measurements of secondary organic aerosols and κinorg≈0.6 which is characteristic for ammonium sulfate and related salts. Both the size-dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=0.1 Xm,org+0.6 Xm,inorg), and the CCN number concentrations predicted with κp were in fair agreement with the measurement results. The median CCN number concentrations at S=0.1–0.82% ranged from NCCN,0.10≈30 cm−3 to NCCN,0.82≈150 cm−3, the median concentration of aerosol particles larger than 30 nm was NCN,30≈180 cm−3, and the corresponding integral CCN efficiencies were in the range of NCCN,0.10/NCN,30≈0.1 to NCCN,0.82/NCN,30≈0.8.
Although the number concentrations and hygroscopicity parameters were much lower, the integral CCN efficiencies observed in pristine rainforest air were similar to those in highly polluted mega-city air. Moreover, model calculations of NCCN,S with a global average value of κ=0.3 led to systematic overpredictions, but the relative deviations exceeded ~50% only at low water vapor supersaturation (0.1%) and low particle number concentrations (≤100 cm−3). These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators.
Depending on the required and applicable level of detail, the information and parameterizations presented in this paper should enable efficient description of the CCN properties of pristine tropical rainforest aerosols in detailed process models as well as in large-scale atmospheric and climate models.