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Title: Long-term observations of cloud condensation nuclei over the Amazon rain forest - Part 2: Variability and characteristics of biomass burning, long-range transport, and pristine rain forest aerosols

Journal Article · · Atmospheric Chemistry and Physics (Online)
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  1. Max Planck Inst. for Chemistry, Mainz (Germany). Multiphase Chemistry and Biogeochemistry Dept.
  2. Max Planck Inst. for Chemistry, Mainz (Germany). Multiphase Chemistry and Biogeochemistry Dept.; Braunschweig Univ. of Technology (Germany)
  3. Brazilian Agricultural Research Corp. (EMBRAPA), Belem (Brazil)
  4. Univ. of Sao Paulo (Brazil). Inst. of Physics; Univ. of Clermont Auvergne, Aubière (France). Physical Meterorology Lab.
  5. Univ. of Sao Paulo (Brazil). Inst. of Physics; Federal Univ. of Uberlandia (Brazil). Inst. of Agrarian Sciences
  6. Max Planck Inst. for Chemistry, Mainz (Germany). Multiphase Chemistry and Biogeochemistry Dept.; Nanjing Univ. (China). Inst. for Climate and Global Change Research and School of Atmospheric Sciences
  7. Indian Inst. of Technology (IIT), Madras (India). Environmental and Water Resources Engineering (EWRE) Division and Dept. of Civil Engineering
  8. Technical Univ. of Darmstadt (Germany). Inst. of Applied Geosciences
  9. Max Planck Inst. for Biogeochemistry, Jena (Germany). Dept. of Biogeochemical Systems
  10. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences and Dept. of Earth and Planetary Sciences
  11. St. Petersburg State Univ. (Russian Federation)
  12. Federal Univ. of Sao Paulo (UNIFESP) (Brazil). Inst. of Environmental, Chemical and Pharmaceutical Sciences
  13. Goethe Univ., Frankfurt (Germany). Inst. of Atmospheric and Environmental Sciences; Hessian Agency for Nature Conservation, Environment and Geology (HLNUG), Wiesbaden (Germany)
  14. Brookhaven National Lab. (BNL), Upton, NY (United States). Biological, Environmental & Climate Sciences Dept.; Snow College, Richfield, UT (United States). Dept. of Chemistry
  15. Brookhaven National Lab. (BNL), Upton, NY (United States). Biological, Environmental & Climate Sciences Dept.
  16. Univ. of Sao Paulo (Brazil). Inst. of Physics
  17. Max Planck Inst. for Chemistry, Mainz (Germany). Multiphase Chemistry and Biogeochemistry Dept.; Univ. of California, San Diego, CA (United States). Scripps Inst. of Oceanography
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For this study, size-resolved measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted over a full seasonal cycle at the remote Amazon Tall Tower Observatory (ATTO, March 2014–February 2015). In a preceding companion paper, we presented annually and seasonally averaged data and parametrizations (Part 1; Pöhlker et al., 2016a). In the present study (Part 2), we analyze key features and implications of aerosol and CCN properties for the following characteristic atmospheric conditions: Empirically pristine rain forest (PR) conditions, where no influence of pollution was detectable, as observed during parts of the wet season from March to May. The PR episodes are characterized by a bimodal aerosol size distribution (strong Aitken mode with DAit ≈ 70nm and NAit ≈ 160cm-3, weak accumulation mode with Dacc ≈ 160nm and Nacc ≈ 90cm-3), a chemical composition dominated by organic compounds, and relatively low particle hygroscopicity (κAit ≈ 0.12, κacc ≈ 0.18). Long-range-transport (LRT) events, which frequently bring Saharan dust, African biomass smoke, and sea spray aerosols into the Amazon Basin, mostly during February to April. The LRT episodes are characterized by a dominant accumulation mode (DAit ≈ 80nm, NAit ≈ 120cm-3 vs. Dacc ≈ 180nm, Nacc ≈ 310cm-3), an increased abundance of dust and salt, and relatively high hygroscopicity (κAit ≈ 0.18, κacc ≈ 0.35). The coarse mode is also significantly enhanced during these events. Biomass burning (BB) conditions characteristic for the Amazonian dry season from August to November. The BB episodes show a very strong accumulation mode (DAit ≈ 70nm, NAit ≈ 140cm-3 vs. Dacc ≈ 170nm, Nacc ≈ 3400cm-3), very high organic mass fractions (~90%), and correspondingly low hygroscopicity (κAit ≈ 0.14, κacc ≈ 0.17). Mixed-pollution (MPOL) conditions with a superposition of African and Amazonian aerosol emissions during the dry season. During the MPOL episode presented here as a case study, we observed African aerosols with a broad monomodal distribution (D ≈ 130nm, NCN, 10 ≈ 1300cm-3), with high sulfate mass fractions (~20%) from volcanic sources and correspondingly high hygroscopicity (κ < 100 nm ≈ 0.14, κ > 10 nm ≈ 0.22), which were periodically mixed with fresh smoke from nearby fires (D ≈ 110nm, NCN, 10 ≈ 2800cm-3) with an organic-dominated composition and sharply decreased hygroscopicity (κ < 150 nm ≈ 0.10, κ > 150 nm ≈ 0.20). Insights into the aerosol mixing state are provided by particle hygroscopicity (κ) distribution plots, which indicate largely internal mixing for the PR aerosols (narrow κ distribution) and more external mixing for the BB, LRT, and MPOL aerosols (broad κ distributions). The CCN spectra (CCN concentration plotted against water vapor supersaturation) obtained for the different case studies indicate distinctly different regimes of cloud formation and microphysics depending on aerosol properties and meteorological conditions. The measurement results suggest that CCN activation and droplet formation in convective clouds are mostly aerosol-limited under PR and LRT conditions and updraft-limited under BB and MPOL conditions. Normalized CCN efficiency spectra (CCN divided by aerosol number concentration plotted against water vapor supersaturation) and corresponding parameterizations (Gaussian error function fits) provide a basis for further analysis and model studies of aerosol–cloud interactions in the Amazon.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER); Max Planck Society; German Federal Ministry of Education and Research (BMBF); Ministry of Science, Technology, Innovation and Communication (MCTIC) (Brazil); Amazon State Univ. (UEA), Manaus (Brazil); Amazonas State Research Support Foundation (FAPEAM) (Brazil); National Inst. of Amazonian Research (INPA). Large Scale Biosphere-Atmosphere Program in Amazonia (LBA); German Research Foundation (DFG); European Union (EU); Sao Paulo Research Foundation (FAPESP); Russian Science Federation (RSF); National Aeronautics and Space Administration (NASA)
Grant/Contract Number:
SC0012704; 01LB1001A; 01.11.01248.00; KA 2280/2; 11.37.220.2016; 603445; 13/05014-0; 13/50510-5; 18-17- 00076
OSTI ID:
1466979
Report Number(s):
BNL-208012-2018-JAAM
Journal Information:
Atmospheric Chemistry and Physics (Online), Vol. 18, Issue 14; ISSN 1680-7324
Publisher:
European Geosciences UnionCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 47 works
Citation information provided by
Web of Science

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Cited By (7)

African volcanic emissions influencing atmospheric aerosols over the Amazon rain forest journal January 2018
Single-particle characterization of aerosols collected at a remote site in the Amazonian rainforest and an urban site in Manaus, Brazil journal January 2019
Land cover and its transformation in the backward trajectory footprint region of the Amazon Tall Tower Observatory journal January 2019
The challenge of simulating the sensitivity of the Amazonian cloud microstructure to cloud condensation nuclei number concentrations journal January 2020
Long-term observations of cloud condensation nuclei in the Amazon rain forest – Part 1: Aerosol size distribution, hygroscopicity, and new model parametrizations for CCN prediction journal January 2016
Urban influence on the concentration and composition of submicron particulate matter in central Amazonia journal January 2018
Aitken mode particles as CCN in aerosol- and updraft-sensitive regimes of cloud droplet formation journal August 2021

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