Ecosystem ozone uptake can occur through stomatal and surface deposition and through gas phase chemical reactions. In a California pine forest, thinning dramatically enhanced both monoterpene emission and ozone uptake. These simultaneous enhancements provide strong evidence that ozone reactions with unmeasured biogenically emitted volatile organic compounds (BVOCs) dominate ozone uptake, and these unmeasured BVOC emissions are approximately 10 times the measured monoterpene flux. Branch enclosure measurements confirm more than 100 BVOCs are emitted but not typically observed above the forest. These BVOCs likely impact tropospheric composition as a previously unquantified source of secondary oxygenated VOCs, organic aerosols, and OH radicals.
Abstract. During the Biosphere Effects on AeRosols and Photochemistry EXperiment 2007 (BEARPEX-2007), we observed eddy covariance (EC) fluxes of speciated acyl peroxy nitrates (APNs), including peroxyacetyl nitrate (PAN), peroxypropionyl nitrate (PPN) and peroxymethacryloyl nitrate (MPAN), above a Ponderosa pine forest in the western Sierra Nevada. All APN fluxes are net downward during the day, with a median midday PAN exchange velocity of −0.3 cm s −1 ; nighttime storage-corrected APN EC fluxes are smaller than daytime fluxes but still downward. Analysis with a standard resistance model shows that loss of PAN to the canopy is not controlled by turbulent or molecular diffusion. Stomatal uptake can account for 25 to 50% of the observed downward PAN flux. Vertical gradients in the PAN thermal decomposition (TD) rate explain a similar fraction of the flux, suggesting that a significant portion of the PAN flux into the forest results from chemical processes in the canopy. The remaining "unidentified" portion of the net PAN flux (∼15%) is ascribed to deposition or reactive uptake on nonstomatal surfaces (e.g. leaf cuticles or soil). Shifts in temperature, moisture and ecosystem activity during the summerfall transition alter the relative contribution of stomatal uptake, non-stomatal uptake and thermochemical gradients to the net PAN flux. Daytime PAN and MPAN exchange velocities are a factor of 3 smaller than those of PPN during the first two weeks of the measurement period, consistent with strong intra-canopy chemical production of PAN and MPAN Correspondence to: J. A. Thornton (thornton@atmos.washington.edu) during this period. Depositional loss of APNs can be 3-21% of the gross gas-phase TD loss depending on temperature. As a source of nitrogen to the biosphere, PAN deposition represents approximately 4-19% of that due to dry deposition of nitric acid at this site.
We describe the construction of a continuous 38-year record of stratospheric aerosol optical properties. The Global Space-based Stratospheric Aerosol Climatology, or GloSSAC, provided the input data to the 15 construction of the Climate Model Intercomparison Project stratospheric aerosol forcing data set (1979 to 2014) and we have extended it through 2016 following an identical process. GloSSAC focuses on the Stratospheric Aerosol and Gas Experiment (SAGE) series of instruments through mid-2005 and on the Optical Spectrograph and InfraRed Imager System (OSIRIS) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) data thereafter. We also use data from other space 20 instruments and from ground-based, air and balloon borne instruments to fill in key gaps in the data set. The end result is a global and gap-free data set focused on aerosol extinction coefficient at 525 and 1020 nm and other parameters on an 'as available' basis. For the primary data sets, we developed a new method for filling the post-Pinatubo eruption data gap for 1991 to 1993 based on data from the Cryogenic Limb Array Etalon Spectrometer. In addition, we developed a new method for populating wintertime high 25 latitudes during the SAGE period employing a latitude-equivalent latitude conversion process that greatly improves the depiction of aerosol at high latitudes compared to earlier similar efforts. We report data in the troposphere only when and where it is available. This is primarily during the SAGE II period except the most enhanced part of the Pinatubo period. It is likely that the upper troposphere during Pinatubo was greatly enhanced over non-volcanic periods and that domain remains substantially under characterized. 30 We note that aerosol levels during the OSIRIS/CALIPSO period in the lower stratosphere at mid and high latitudes is routinely higher than what we observed during the SAGE II period. While this period had nearly continuous low-level volcanic activity, it is possible that the enhancement in part reflects deficiencies in the data set. We also expended substantial effort to quality assess the data set and the product is by far the best we have produced. GloSSAC version 1.0 is available in netCDF format at the NASA Atmospheric 35 Data Center at https://eosweb.larc.nasa.gov/. GloSSAC users should cite this paper and the data set DOI
Forests are complex ecosystems characterized by several distinctive vertical layers with different functional properties. Measurements of CO2 fluxes by the eddy-covariance method at different heights can be used to separate sources and sinks in these layers.We used meteorological and eddy-covariance flux data gathered at 10 sites in the FLUXNET network across a wide range of forest type, structure and climate. We showed that eddy-covariance flux measurements made in the understory are problematic at night in open forests because of the build up of a strong inversion layer, but are more reliable during the day. Denser forests have higher turbulence at night in the understory because the inversion is weaker. However, the flux footprint above and below canopy is less similar than in more open forests, partly because wind direction is more deflected while entering the canopy. We showed that gross primary productivity (GPP) of the understory can reach 39% of the total canopy GPP, with an average of 14% across the studied sites. Both understory leaf area index (LAI) and light penetration through the canopy are important for understory GPP. We found that understory respiration contributed an average of 55% to ecosystem respiration, with a range of 32–79%. Understory in deciduous forests (62%) had higher contributions to ecosystem respiration than in evergreen forests (49%). Boreal and temperate forests had a mean understory respiration contribution of 61%, while semi-arid forests showed lower values (44%). The normalized understory respiration fluxes at 20 8C were negatively related to soil temperature, when differences in soil moisture across sites are taken into account. We showed evidence that drought limited the efficiency of microbial metabolic activity. Understory respiration fluxes were positively correlated with gross ecosystem primary productivity
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