American Cancer Society; Centers for Disease Control and Prevention; Swiss Re; Swiss Cancer Research foundation; Swiss Cancer League; Institut National du Cancer; La Ligue Contre le Cancer; Rossy Family Foundation; US National Cancer Institute; and the Susan G Komen Foundation.

Amazonia as a carbon source linked to deforestation and climate change

Wetlands are the largest global source of atmospheric methane (CH), a potent greenhouse gas. However, methane emission inventories from the Amazon floodplain, the largest natural geographic source of CH in the tropics, consistently underestimate the atmospheric burden of CH determined via remote sensing and inversion modelling, pointing to a major gap in our understanding of the contribution of these ecosystems to CH emissions. Here we report CH fluxes from the stems of 2,357 individual Amazonian floodplain trees from 13 locations across the central Amazon basin. We find that escape of soil gas through wetland trees is the dominant source of regional CH emissions. Methane fluxes from Amazon tree stems were up to 200 times larger than emissions reported for temperate wet forests and tropical peat swamp forests, representing the largest non-ebullitive wetland fluxes observed. Emissions from trees had an average stable carbon isotope value (δC) of -66.2 ± 6.4 per mil, consistent with a soil biogenic origin. We estimate that floodplain trees emit 15.1 ± 1.8 to 21.2 ± 2.5 teragrams of CH a year, in addition to the 20.5 ± 5.3 teragrams a year emitted regionally from other sources. Furthermore, we provide a 'top-down' regional estimate of CH emissions of 42.7 ± 5.6 teragrams of CH a year for the Amazon basin, based on regular vertical lower-troposphere CH profiles covering the period 2010-2013. We find close agreement between our 'top-down' and combined 'bottom-up' estimates, indicating that large CH emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH budget. Our findings demonstrate the importance of tree stem surfaces in mediating approximately half of all wetland CH emissions in the Amazon floodplain, a region that represents up to one-third of the global wetland CH source when trees are combined with other emission sources.

Abstract. Spectral aerosol light absorption is an important parameter for the assessment of the radiation budget of the atmosphere. Although on-line measurement techniques for aerosol light absorption, such as the Aethalometer and the Particle Soot Absorption Photometer (PSAP), have been available for two decades, they are limited in accuracy and spectral resolution because of the need to deposit the aerosol on a filter substrate before measurement. Recently, a 7-wavelength (λ) Aethalometer became commercially available, which covers the visible (VIS) to near-infrared (NIR) spectral range (λ=450-950 nm), and laboratory calibration studies improved the degree of confidence in these measurement techniques. However, the applicability of the laboratory calibration factors to ambient conditions has not been investigated thoroughly yet.As part of the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia -SMOke aerosols, Clouds, rainfall and Climate) campaign from September to November 2002 in the Amazon basin we performed an extensive field calibration of a 1-λ PSAP and a 7-λ Aethalometer utilizing a photoacoustic spectrometer (PAS, 532 nm) as reference device. Especially during the dry period of the campaign, the aerosol population was dominated by pyrogenic emissions. The most pronounced artifact of integrating-plate type attenuation techniques (e.g. Aethalometer, PSAP) is due to multiple scattering effects within the filter matrix. ForCorrespondence to: O. Schmid (oschmid@mpch-mainz.mpg.de) the PSAP, we essentially confirmed the laboratory calibration factor by Bond et al. (1999). On the other hand, for the Aethalometer we found a multiple scattering enhancement of 5.23 (or 4.55, if corrected for aerosol scattering), which is significantly larger than the factors previously reported (∼2) for laboratory calibrations. While the exact reason for this discrepancy is unknown, the available data from the present and previous studies suggest aerosol mixing (internal versus external) as a likely cause. For Amazonian aerosol, we found no absorption enhancement due to hygroscopic particle growth in the relative humidity (RH) range between 40% and 80%. However, a substantial bias in PSAP sensitivity that correlated with both RH and temperature (T) was observed for 20%

Abstract. 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 towerbased 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 VOCsCorrespondence to: U. Kuhn (kuhn@mpch-mainz.mpg.de)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 3-8×10 6 molecules cm −3 , i.e., an order of magnitude higher than is estimated for the tropical CBL by current state-of-theart 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 5.5×10 6 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.Published by Copernicus Publications on behalf of the European Geosciences Union. 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 CO 2 fluxes, estimated by three different methods (eddy correlation, Lagrangian dispersion, and mass budget approach). Depending on the CO 2 flux estimate, 1-6% or more of the carbon gained by net ecosystem productivity appeared to be re-...

Abstract. Spectral aerosol light absorption is an important parameter for the assessment of the radiation budget of the atmosphere. Although on-line measurement techniques for aerosol light absorption, such as the Aethalometer and the Particle Soot Absorption Photometer (PSAP), have been available for two decades, they are limited in accuracy and spectral resolution because of the need to deposit the aerosol on a filter substrate before measurement. Recently, a 7-wavelength (λ) Aethalometer became commercially available, which covers the visible (VIS) to near-infrared (NIR) spectral range (λ=450–950 nm), and laboratory calibration studies improved the degree of confidence in these measurement techniques. However, the applicability of the laboratory calibration factors to ambient conditions has not been investigated thoroughly yet. As part of the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia – SMOke aerosols, Clouds, rainfall and Climate) campaign from September to November 2002 in the Amazon basin we performed an extensive field calibration of a 1-λ PSAP and a 7-λ Aethalometer utilizing a photoacoustic spectrometer (PAS, 532 nm) as reference device. Especially during the dry period of the campaign, the aerosol population was dominated by pyrogenic emissions. The most pronounced artifact of integrating-plate type attenuation techniques is due to multiple scattering effects within the filter matrix. For the PSAP, we essentially confirmed the laboratory calibration factor by Bond (1999). On the other hand, for the Aethalometer we found a multiple scattering enhancement of 5.23 (or 4.55, if corrected for aerosol scattering), which is significantly larger than the factors previously reported (~2). While the exact reason for this discrepancy is unknown, the available data from the present and previous studies suggest aerosol mixing (internal versus external) as a likely cause. While it is well-known that RH may (moderately) affect aerosol absorption, we found no dependence of either PSAP or Aethalometer on relative humidity (RH) for 30%<RH<55% and 40%<RH<80%, respectively. However, a substantial decrease in PSAP sensitivity was observed for low RH (20%<RH<30%). In addition, while the PSAP demonstrated no sensitivity to gaseous adsorption, the Aethalometer response was clearly positively correlated with the gradient in pollution level. Hence, although very similar in measurement principle, the PSAP and Aethalometer require markedly different correction factors, which is probably due to the different filter media used. Although on-site calibration of the PSAP and Aethalometer is suggested for best data quality, we recommend a set of PSAP and Aethalometer correction factors for ambient sampling based on the data from the present and previous studies. For this study, the estimated accuracies of the absorption coefficients determined by the PAS, PSAP and Aethalometer were 10, 15 and 20%, respectively.

Abstract. 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 regional 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.

[1] Measurements of NO-NO 2 -O 3 trace gas exchange were performed for two transition season periods during the La Niña year 1999 (30 April to 17 May, ''wet-dry,'' and 24 September to 27 October, ''dry-wet'') over a cattle pasture in Rondônia. A dynamic chamber system (applied during the dry-wet season) was used to directly measure emission fluxes of nitric oxide (NO) and surface resistances for nitrogen dioxide (NO 2 ) and ozone (O 3 ) deposition. A companion study was simultaneously performed in an oldgrowth forest. In order to determine ecosystem-representative NO 2 and O 3 deposition fluxes for both measurement periods, an inferential method (multiresistance model) was applied to measure ambient NO 2 and O 3 concentrations using observed quantities of turbulent transport. Supplementary measurements included soil NO diffusivity and soil nutrient analysis. The observed NO soil emission fluxes were nine times lower than oldgrowth rain forest emissions under similar soil moisture and temperature conditions and were attributed to the combination of a reduced soil N cycle and lower effective soil NO diffusion at the pasture. Canopy resistances (R c ) of both gases controlled the deposition processes during the day for both measurement periods. Day and night NO 2 canopy resistances were significantly similar (a = 0.05) during the dry-wet period. Ozone canopy resistances revealed significantly higher daytime resistances of 106 s m À1 versus 65 s m À1at night because of plant, soil, and wet skin uptake processes, enhanced by stomatal activity at night and aqueous phase chemistry on vegetative and soil surfaces. The surface of the pasture was a net NO x sink during 1999, removing seven times more NO 2 from the atmosphere than was emitted as NO.