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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  ≈  70 nm and NAit  ≈  160 cm−3, weak accumulation mode with Dacc  ≈  160 nm and Nacc ≈  90 cm−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  ≈  80 nm, NAit  ≈  120 cm−3 vs. Dacc  ≈  180 nm, Nacc  ≈  310 cm−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  ≈  70 nm, NAit  ≈  140 cm−3 vs. Dacc  ≈  170 nm, Nacc  ≈  3400 cm−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  ≈  130 nm, NCN, 10  ≈  1300 cm−3), with high sulfate mass fractions (∼  20 %) from volcanic sources and correspondingly high hygroscopicity (κ ≈  0.14, κ > 100 nm ≈  0.22), which were periodically mixed with fresh smoke from nearby fires (D  ≈  110 nm, NCN, 10  ≈  2800 cm−3) with an organic-dominated composition and sharply decreased hygroscopicity (κ ≈  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.

Nocturnal turbulent kinetic energy (TKE) and fluxes of energy, CO2 and O3 between the Amazon forest and the atmosphere are evaluated for a 20-day campaign at the Amazon Tall Tower Observatory (ATTO) site. The distinction of these quantities between fully turbulent (weakly stable) and intermittent (very stable) nights is discussed. Spectral analysis indicates that low-frequency, nonturbulent fluctuations are responsible for a large portion of the variability observed on intermittent nights. In these conditions, the low-frequency exchange may dominate over the turbulent transfer. In particular, we show that within the canopy most of the exchange of CO2 and H2O happens on temporal scales longer than 100 s. At 80 m, on the other hand, the turbulent fluxes are almost absent in such very stable conditions, suggesting a boundary layer shallower than 80 m. The relationship between TKE and mean winds shows that the stable boundary layer switches from the very stable to the weakly stable regime during intermittent bursts of turbulence. In general, fluxes estimated with long temporal windows that account for low-frequency effects are more dependent on the stability over a deeper layer above the forest than they are on the stability between the top of the canopy and its interior, suggesting that low-frequency processes are controlled over a deeper layer above the forest.

We estimated the isoprene and monoterpene source strengths of a pristine tropical forest north of Manaus in the central Amazon Basin using three different micrometeorological flux measurement approaches. During the early dry season campaign of the Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001), a tower-based surface layer gradient (SLG) technique was applied simultaneously with a relaxed eddy accumulation (REA) system. Airborne measurements of vertical profiles within and above the convective boundary layer (CBL) were used to estimate fluxes on a landscape scale by application of the mixed layer gradient (MLG) technique. The mean daytime fluxes of organic carbon measured by REA were 2.1 mg C m−2 h−1 for isoprene, 0.20 mg C m−2 h−1 for α-pinene, and 0.39 mg C m−2 h−1 for the sum of monoterpenes. These values are in reasonable agreement with fluxes determined with the SLG approach, which exhibited a higher scatter, as expected for the complex terrain investigated. The observed VOC fluxes are in good agreement with simulations using a single-column chemistry and climate model (SCM). In contrast, the model-derived mixing ratios of VOCs were by far higher than observed, indicating that chemical processes may not be adequately represented in the model. The observed vertical gradients of isoprene and its primary degradation products methyl vinyl ketone (MVK) and methacrolein (MACR) suggest that the oxidation capacity in the tropical CBL is much higher than previously assumed. A simple chemical kinetics model was used to infer OH radical concentrations from the vertical gradients of (MVK+MACR)/isoprene. The estimated range of OH concentrations during the daytime was 3–8×106 molecules cm−3, i.e., an order of magnitude higher than is estimated for the tropical CBL by current state-of-the-art atmospheric chemistry and transport models. The remarkably high OH concentrations were also supported by results of a simple budget analysis, based on the flux-to-lifetime relationship of isoprene within the CBL. Furthermore, VOC fluxes determined with the airborne MLG approach were only in reasonable agreement with those of the tower-based REA and SLG approaches after correction for chemical decay by OH radicals, applying a best estimate OH concentration of 5.5×106 molecules cm−3. The SCM model calculations support relatively high OH concentration estimates after specifically being constrained by the mixing ratios of chemical constituents observed during the campaign. The relevance of the VOC fluxes for the local carbon budget of the tropical rainforest site during the measurements campaign was assessed by comparison with the concurrent CO2 fluxes, estimated by three different methods (eddy correlation, Lagrangian dispersion, and mass budget approach). Depending on the CO2 flux estimate, 1–6% or more of the carbon gained by net ecosystem productivity appeared to be re-emitted through VOC emissions.