| 1. |
- Barkley, Michael P., et al.
(författare)
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Assessing sources of uncertainty in formaldehyde air mass factors over tropical South America: Implications for top-down isoprene emission estimates
- 2012
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 117, s. 13304-13304
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Tidskriftsartikel (refereegranskat)abstract
- We use a nested-grid version of the GEOS-Chem chemistry transport model, constrained by isoprene emissions from the Model of Emissions of Gases and Aerosols from Nature (MEGAN), and the Lund-Potsdam-Jena General Ecosystem Simulator (LPJ-GUESS) bottom-up inventories, to evaluate the impact that surface isoprene emissions have on formaldehyde (HCHO) air-mass factors (AMFs) and vertical column densities (VCDs) over tropical South America during 2006, as observed by the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) and Ozone Monitoring Instrument (OMI). Although the large-scale seasonal variability of monthly mean HCHO VCDs is typically unaffected by the choice of bottom-up inventory, large relative differences of up to +/- 45% in the HCHO VCD can occur for individual regions and months, but typically most VCD differences are of order +/- 20%. These relative changes are comparable to those produced by other sources of uncertainty in the AMF including aerosols and surface albedo, but less than those from clouds. In a sensitivity test, we find that top-down annual isoprene emissions inferred from SCIAMACHY and OMI HCHO vertical columns can vary by as much as +/- 30-50% for each instrument respectively, depending on the region studied and the a priori isoprene emissions used. Our analysis suggests that the influence of the a priori isoprene emissions on HCHO AMFs and VCDs is therefore non-negligible and must be carefully considered when inferring top-down isoprene emissions estimates over this, or potentially any other, region.
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| 2. |
- Barkley, Michael P., et al.
(författare)
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Can a "state of the art" chemistry transport model simulate Amazonian tropospheric chemistry?
- 2011
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 116, s. 16302-16302
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Tidskriftsartikel (refereegranskat)abstract
- We present an evaluation of a nested high-resolution Goddard Earth Observing System (GEOS)-Chem chemistry transport model simulation of tropospheric chemistry over tropical South America. The model has been constrained with two isoprene emission inventories: (1) the canopy-scale Model of Emissions of Gases and Aerosols from Nature (MEGAN) and (2) a leaf-scale algorithm coupled to the Lund-Potsdam-Jena General Ecosystem Simulator (LPJ-GUESS) dynamic vegetation model, and the model has been run using two different chemical mechanisms that contain alternative treatments of isoprene photo-oxidation. Large differences of up to 100 Tg C yr (1) exist between the isoprene emissions predicted by each inventory, with MEGAN emissions generally higher. Based on our simulations we estimate that tropical South America (30-85 degrees W, 14 degrees N-25 degrees S) contributes about 15-35% of total global isoprene emissions. We have quantified the model sensitivity to changes in isoprene emissions, chemistry, boundary layer mixing, and soil NOx emissions using ground-based and airborne observations. We find GEOS-Chem has difficulty reproducing several observed chemical species; typically hydroxyl concentrations are underestimated, whilst mixing ratios of isoprene and its oxidation products are overestimated. The magnitude of model formaldehyde (HCHO) columns are most sensitive to the choice of chemical mechanism and isoprene emission inventory. We find GEOS-Chem exhibits a significant positive bias (10-100%) when compared with HCHO columns from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) and Ozone Monitoring Instrument (OMI) for the study year 2006. Simulations that use the more detailed chemical mechanism and/or lowest isoprene emissions provide the best agreement to the satellite data, since they result in lower-HCHO columns.
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| 3. |
- Friedman, Beth, et al.
(författare)
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Subarctic atmospheric aerosol composition: 1. Ambient aerosol characterization
- 2009
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 114
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Tidskriftsartikel (refereegranskat)abstract
- Subarctic aerosol was sampled during July 2007 at the Abisko Research Station Stordalen field site operated by the Royal Swedish Academy of Sciences. Located in northern Sweden at 68 degrees latitude and 385 m above sea level (m asl), this site is classified as a semicontinuous permafrost mire. Number density, size distribution, cloud condensation nucleus properties, and chemical composition of the ambient aerosol were determined. Back trajectories showed that three distinct air masses were present over Stordalen during the sampling period. Aerosol properties changed and correlated with air mass origin to the south, northeast, or west, suggesting that particle source and transport were important factors. We observe that Arctic aerosol is not compositionally unlike that found in the free troposphere at midlatitudes. Internal mixtures of sulfates and organics, many on insoluble biomass burning and/or elemental carbon cores, dominate the number density of particles from similar to 200-to 2000-nm aerodynamic diameter. Mineral dust that had interacted with gas-phase species was observed in all air masses. Sea salt, due to the uptake of nitrate species and loss of chlorine, was the aerosol type that most varied chemically with air mass.
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| 4. |
- Groenendijk, M., et al.
(författare)
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Seasonal variation of photosynthetic model parameters and leaf area index from global Fluxnet eddy covariance data
- 2011
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 116, s. 04027-04027
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Tidskriftsartikel (refereegranskat)abstract
- Global vegetation models require the photosynthetic parameters, maximum carboxylation capacity (V(cm)), and quantum yield (alpha) to parameterize their plant functional types (PFTs). The purpose of this work is to determine how much the scaling of the parameters from leaf to ecosystem level through a seasonally varying leaf area index (LAI) explains the parameter variation within and between PFTs. Using Fluxnet data, we simulate a seasonally variable LAI(F) for a large range of sites, comparable to the LAI(M) derived from MODIS. There are discrepancies when LAI(F) reach zero levels and LAI(M) still provides a small positive value. We find that temperature is the most common constraint for LAI(F) in 55% of the simulations, while global radiation and vapor pressure deficit are the key constraints for 18% and 27% of the simulations, respectively, while large differences in this forcing still exist when looking at specific PFTs. Despite these differences, the annual photosynthesis simulations are comparable when using LAI(F) or LAIM (r(2) = 0.89). We investigated further the seasonal variation of ecosystem-scale parameters derived with LAI(F). V(cm) has the largest seasonal variation. This holds for all vegetation types and climates. The parameter alpha is less variable. By including ecosystem-scale parameter seasonality we can explain a considerable part of the ecosystem-scale parameter variation between PFTs. The remaining unexplained leaf-scale PFT variation still needs further work, including elucidating the precise role of leaf and soil level nitrogen.
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| 5. |
- Jardine, K., et al.
(författare)
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Within-canopy sesquiterpene ozonolysis in Amazonia
- 2011
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 116
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Tidskriftsartikel (refereegranskat)abstract
- Through rapid reactions with ozone, which can initiate the formation of secondary organic aerosols, the emission of sesquiterpenes from vegetation in Amazonia may have significant impacts on tropospheric chemistry and climate. Little is known, however, about sesquiterpene emissions, transport, and chemistry within plant canopies owing to analytical difficulties stemming from very low ambient concentrations, high reactivities, and sampling losses. Here, we present ambient sesquiterpene concentration measurements obtained during the 2010 dry season within and above a primary tropical forest canopy in Amazonia. We show that by peaking at night instead of during the day, and near the ground instead of within the canopy, sesquiterpene concentrations followed a pattern different from that of monoterpenes, suggesting that unlike monoterpene emissions, which are mainly light dependent, sesquiterpene emissions are mainly temperature dependent. In addition, we observed that sesquiterpene concentrations were inversely related with ozone (with respect to time of day and vertical concentration), suggesting that ambient concentrations are highly sensitive to ozone. These conclusions are supported by experiments in a tropical rain forest mesocosm, where little atmospheric oxidation occurs and sesquiterpene and monoterpene concentrations followed similar diurnal patterns. We estimate that the daytime dry season ozone flux of -0.6 to -1.5 nmol m(-2) s(-1) due to in-canopy sesquiterpene reactivity could account for 7%-28% of the net ozone flux. Our study provides experimental evidence that a large fraction of total plant sesquiterpene emissions (46%-61% by mass) undergo within-canopy ozonolysis, which may benefit plants by reducing ozone uptake and its associated oxidative damage.
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| 6. |
- Jung, Martin, et al.
(författare)
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Global patterns of land-atmosphere fluxes of carbon dioxide, latent heat, and sensible heat derived from eddy covariance, satellite, and meteorological observations
- 2011
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 116, s. 00-07
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Tidskriftsartikel (refereegranskat)abstract
- We upscaled FLUXNET observations of carbon dioxide, water, and energy fluxes to the global scale using the machine learning technique, model tree ensembles (MTE). We trained MTE to predict site-level gross primary productivity (GPP), terrestrial ecosystem respiration (TER), net ecosystem exchange (NEE), latent energy (LE), and sensible heat (H) based on remote sensing indices, climate and meteorological data, and information on land use. We applied the trained MTEs to generate global flux fields at a 0.5 degrees x 0.5 degrees spatial resolution and a monthly temporal resolution from 1982 to 2008. Cross-validation analyses revealed good performance of MTE in predicting among-site flux variability with modeling efficiencies (MEf) between 0.64 and 0.84, except for NEE (MEf = 0.32). Performance was also good for predicting seasonal patterns (MEf between 0.84 and 0.89, except for NEE (0.64)). By comparison, predictions of monthly anomalies were not as strong (MEf between 0.29 and 0.52). Improved accounting of disturbance and lagged environmental effects, along with improved characterization of errors in the training data set, would contribute most to further reducing uncertainties. Our global estimates of LE (158 +/- 7 J x 10(18) yr(-1)), H (164 +/- 15 J x 10(18) yr(-1)), and GPP (119 +/- 6 Pg C yr(-1)) were similar to independent estimates. Our global TER estimate (96 +/- 6 Pg C yr(-1)) was likely underestimated by 5-10%. Hot spot regions of interannual variability in carbon fluxes occurred in semiarid to semihumid regions and were controlled by moisture supply. Overall, GPP was more important to interannual variability in NEE than TER. Our empirically derived fluxes may be used for calibration and evaluation of land surface process models and for exploratory and diagnostic assessments of the biosphere.
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| 7. |
- Kammermann, Lukas, et al.
(författare)
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Subarctic atmospheric aerosol composition: 3. Measured and modeled properties of cloud condensation nuclei
- 2010
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 115
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol particles can modify cloud properties by acting as cloud condensation nuclei (CCN). Predicting CCN properties is still a challenge and not properly incorporated in current climate models. Atmospheric particle number size distributions, hygroscopic growth factors, and polydisperse CCN number concentrations were measured at the remote subarctic Stordalen mire, 200 km north of the Arctic Circle in northern Sweden. The CCN number concentration was highly variable, largely driven by variations in the total number of sufficiently large particles, though the variability of chemical composition was increasingly important for decreasing supersaturation. The hygroscopicity of particles measured by a hygroscopicity tandem differential mobility analyzer (HTDMA) was in agreement with large critical diameters observed for CCN activation (kappa approximate to 0.07-0.21 for D = 50-200 nm). Size distribution and time- and size-resolved HTDMA data were used to predict CCN number concentrations. Agreement of predictions with measured CCN within +/- 11% was achieved using parameterized Kohler theory and assuming a surface tension of pure water. The sensitivity of CCN predictions to various simplifying assumptions was further explored: We found that (1) ignoring particle mixing state did not affect CCN predictions, (2) averaging the HTDMA data in time with retaining the size dependence did not introduce a substantial bias, while individual predictions became more uncertain, and (3) predictions involving the hygroscopicity parameter recommended in literature for continental sites (kappa approximate to 0.3 +/- 0.1) resulted in a significant prediction bias. Future modeling studies should therefore at least aim at using averaged, size-resolved, site-specific hygroscopicity or chemical composition data for predictions of CCN number concentrations.
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| 8. |
- Kergoat, Laurent, et al.
(författare)
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Nitrogen controls plant canopy light-use efficiency in temperate and boreal ecosystems
- 2008
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 113:G4, s. 04017-04017
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Forskningsöversikt (refereegranskat)abstract
- Optimum daily light-use efficiency (LUE) and normalized canopy photosynthesis (GEE*) rate, a proxy for LUE, have been derived from eddy covariance CO2 flux measurements obtained at a range of sites located in the mid to high latitudes. These two variables were analyzed with respect to environmental conditions, plant functional types (PFT) and leaf nitrogen concentration, in an attempt to characterize their variability and their potential drivers. LUE averaged 0.0182 mol/mol with a coefficient of variation of 37% (42% for GEE*). Foliar nitrogen N of the dominant plant species was found to explain 71% of LUE (n = 26) and 62% of GEE* (n = 44) variance, across all PFTs and sites. Mean Annual Temperature, MAT, explained 27% of LUE variance, and the two factors (MAT and N) combined in a simple linear model explain 80% of LUE and 76% GEE* variance. These results showed that plant canopies in the temperate, boreal and arctic zones fit into a general scheme closely related to the one, which had been established for plant leaves worldwide. The N-MAT- LUE relationships offer perspectives for LUE-based models of terrestrial photosynthesis based on remote sensing. On a continental scale, the decrease of LUE from the temperate to the arctic zone found in the data derived from flux measurements is not in line with LUE resulting from inversion of atmospheric CO2.
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| 9. |
- Schurgers, Guy, et al.
(författare)
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Effect of climate-driven changes in species composition on regional emission capacities of biogenic compounds
- 2011
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 116, s. 22304-22304
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Tidskriftsartikel (refereegranskat)abstract
- Regional or global modeling studies of dynamic vegetation often represent vegetation by large functional units (plant functional types (PFTs)). For simulation of biogenic volatile organic compounds (BVOC) in these models, emission capacities, which give the emission under standardized conditions, are provided as an average value for a PFT. These emission capacities thus hide the known heterogeneity in emission characteristics that are not straightforwardly related to functional characteristics of plants. Here we study the effects of the aggregation of species-level information on emission characteristics at PFT level. The roles of temporal and spatial variability are assessed for Europe by comparing simulations that represent vegetation by dominant tree species on the one hand and by plant functional types on the other. We compare a number of time slices between the Last Glacial Maximum (21,000 years ago) and the present day to quantify the effects of dynamically changing vegetation on BVOC emissions. Spatial heterogeneity of emission factors is studied with present-day simulations. We show that isoprene and monoterpene emissions are of similar magnitude in Europe when the simulation represents dominant European tree species, which indicates that simulations applying typical global-scale emission capacities for PFTs tend to overestimate isoprene and underestimate monoterpene emissions. Moreover, both spatial and temporal variability affect emission capacities considerably, and by aggregating these to PFT level averages, one loses the information on local heterogeneity. Given the reactive nature of these compounds, accounting for spatial and temporal heterogeneity can be important for studies of their fate in the atmosphere.
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