19 research outputs found
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Evaluating the effect of alternative carbon allocation schemes in a land surface model (CLM4.5) on carbon fluxes, pools, and turnover in temperate forests
How carbon (C) is allocated to different plant tissues (leaves, stem, and roots) determines how long C remains in plant biomass and thus remains a central challenge for understanding the global C cycle. We used a diverse set of observations (AmeriFlux eddy covariance tower observations, biomass estimates from tree-ring data, and leaf area index (LAI) measurements) to compare C fluxes, pools, and LAI data with those predicted by a land surface model (LSM), the Community Land Model (CLM4.5). We ran CLM4.5 for nine temperate (including evergreen and deciduous) forests in North America between 1980 and 2013 using four different C allocation schemes: i. dynamic C allocation scheme (named "D-CLM4.5") with one dynamic allometric parameter, which allocates C to the stem and leaves to vary in time as a function of annual net primary production (NPP); ii. an alternative dynamic C allocation scheme (named "D-Litton"), where, similar to (i), C allocation is a dynamic function of annual NPP, but unlike (i) includes two dynamic allometric parameters involving allocation to leaves, stem, and coarse roots; iii.-iv. a fixed C allocation scheme with two variants, one representative of observations in evergreen (named "F-Evergreen") and the other of observations in deciduous forests (named "F-Deciduous"). D-CLM4.5 generally overestimated gross primary production (GPP) and ecosystem respiration, and underestimated net ecosystem exchange (NEE). In D-CLM4.5, initial aboveground biomass in 1980 was largely overestimated (between 10 527 and 12 897 g Cm-2) for deciduous forests, whereas aboveground biomass accumulation through time (between 1980 and 2011) was highly underestimated (between 1222 and 7557 gCm(-2)) for both evergreen and deciduous sites due to a lower stem turnover rate in the sites than the one used in the model. D-CLM4.5 overestimated LAI in both evergreen and deciduous sites because the leaf C-LAI relationship in the model did not match the observed leaf C-LAI relationship at our sites. Although the four C allocation schemes gave similar results for aggregated C fluxes, they translated to important differences in long-term aboveground biomass accumulation and aboveground NPP. For deciduous forests, D-Litton gave more realistic C-stem/C-leaf ratios and strongly reduced the overestimation of initial aboveground biomass and aboveground NPP for deciduous forests by D-CLM4.5. We identified key structural and parameterization deficits that need refinement to improve the accuracy of LSMs in the near future. These include changing how C is allocated in fixed and dynamic schemes based on data from current forest syntheses and different parameterization of allocation schemes for different forest types. Our results highlight the utility of using measurements of aboveground biomass to evaluate and constrain the C allocation scheme in LSMs, and suggest that stem turnover is overestimated by CLM4.5 for these AmeriFlux sites. Understanding the controls of turnover will be critical to improving long-term C processes in LSMs
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An update on ozone profile trends for the period 2000 to 2016
Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48km altitude (5 and 1hPa). Near 2hPa (42km), ozone has been increasing by about 1.5% per decade in the tropics (20°S to 20°N), and by 2 to 2.5% per decade in the 35 to 60° latitude bands of both hemispheres. At levels below 35km (5hPa), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2hPa in the 35 to 60° latitude bands from about ±5% (2σ) in Harris et al. (2015) to less than ±2% (2σ). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected
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Anthropogenic influences on the physical state of submicron particulate matter over a tropical forest
The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Measurements were conducted during two intensive operating periods (IOP1 and IOP2) that took place during the wet and dry seasons of the GoAmazon2014/5 campaign. Air masses representing variable influences of background conditions, urban pollution, and regional- and continental-scale biomass burning passed over the research site. As the air masses varied, particle rebound fraction, an indicator of physical state, was measured in real time at ground level using an impactor apparatus. Micrographs collected by transmission electron microscopy confirmed that liquid particles adhered, while nonliquid particles rebounded. Relative humidity (RH) was scanned to collect rebound curves. When the apparatus RH matched ambient RH, 95 % of the particles adhered as a campaign average. Secondary organic material, produced for the most part by the oxidation of volatile organic compounds emitted from the forest, produces liquid PM over this tropical forest. During periods of anthropogenic influence, by comparison, the rebound fraction dropped to as low as 60 % at 95 % RH. Analyses of the mass spectra of the atmospheric PM by positive-matrix factorization (PMF) and of concentrations of carbon monoxide, total particle number, and oxides of nitrogen were used to identify time periods affected by anthropogenic influences, including both urban pollution and biomass burning. The occurrence of nonliquid PM at high RH correlated with these indicators of anthropogenic influence. A linear model having as output the rebound fraction and as input the PMF factor loadings explained up to 70 % of the variance in the observed rebound fractions. Anthropogenic influences can contribute to the presence of nonliquid PM in the atmospheric particle population through the combined effects of molecular species that increase viscosity when internally mixed with background PM and increased concentrations of nonliquid anthropogenic particles in external mixtures of anthropogenic and biogenic PM
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Introduction to the SPARC Reanalysis Intercomparison Project (S-RIP) and overview of the reanalysis systems
The climate research community uses atmospheric reanalysis data sets to understand a wide range of processes and variability in the atmosphere, yet different reanalyses may give very different results for the same diagnostics. The Stratosphere-troposphere Processes And their Role in Climate (SPARC) Reanalysis Intercomparison Project (S-RIP) is a coordinated activity to compare reanalysis data sets using a variety of key diagnostics. The objectives of this project are to identify differences among reanalyses and understand their underlying causes, to provide guidance on appropriate usage of various reanalysis products in scientific studies, particularly those of relevance to SPARC, and to contribute to future improvements in the reanalysis products by establishing collaborative links between reanalysis centres and data users. The project focuses predominantly on differences among reanalyses, although studies that include operational analyses and studies comparing reanalyses with observations are also included when appropriate. The emphasis is on diagnostics of the upper troposphere, stratosphere, and lower mesosphere. This paper summarizes the motivation and goals of the S-RIP activity and extensively reviews key technical aspects of the reanalysis data sets that are the focus of this activity. The special issue The SPARC Reanalysis Intercomparison Project (S-RIP) in this journal serves to collect research with relevance to the S-RIP in preparation for the publication of the planned two (interim and full) S-RIP reports
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Perspectives on the Future of Ice Nucleation Research: Research Needs and Unanswered Questions Identified from Two International Workshops
There has been increasing interest in ice nucleation research in the last decade. To identify important gaps in our knowledge of ice nucleation processes and their impacts, two international workshops on ice nucleation were held in Vienna, Austria in 2015 and 2016. Experts from these workshops identified the following research needs: (1) uncovering the molecular identity of active sites for ice nucleation; (2) the importance of modeling for the understanding of heterogeneous ice nucleation; (3) identifying and quantifying contributions of biological ice nuclei from natural and managed environments; (4) examining the role of aging in ice nuclei; (5) conducting targeted sampling campaigns in clouds; and (6) designing lab and field experiments to increase our understanding of the role of ice-nucleating particles in the atmosphere. Interdisciplinary teams of scientists should work together to establish and maintain a common, unified language for ice nucleation research. A number of commercial applications benefit from ice nucleation research, including the production of artificial snow, the freezing and preservation of water-containing food products, and the potential modulation of weather. Additional work is needed to increase our understanding of ice nucleation processes and potential impacts on precipitation, water availability, climate change, crop health, and feedback cycles
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BrO and inferred Br-y profiles over the western Pacific: relevance of inorganic bromine sources and a Br-y minimum in the aged tropical tropopause layer
We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box model to infer total gas-phase inorganic bromine (Bry) over the tropical western Pacific Ocean (tWPO) during the CONTRAST field campaign (January–February 2014). The observed BrO and inferred Bry profiles peak in the marine boundary layer (MBL), suggesting the need for a bromine source from sea-salt aerosol (SSA), in addition to organic bromine (CBry). Both profiles are found to be C-shaped with local maxima in the upper free troposphere (FT). The median tropospheric BrO vertical column density (VCD) was measured as 1.6×1013 molec cm−2, compared to model predictions of 0.9×1013 molec cm−2 in GEOS-Chem (CBry but no SSA source), 0.4×1013 molec cm−2 in CAM-Chem (CBry and SSA), and 2.1×1013 molec cm−2 in GEOS-Chem (CBry and SSA). Neither global model fully captures the C-shape of the Bry profile. A local Bry maximum of 3.6 ppt (2.9–4.4 ppt; 95 % confidence interval, CI) is inferred between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective tropical tropopause layer (TTL) to the aged TTL, gas-phase Bry decreases from the convective TTL to the aged TTL. Analysis of gas-phase Bry against multiple tracers (CFC-11, H2O ∕ O3 ratio, and potential temperature) reveals a Bry minimum of 2.7 ppt (2.3–3.1 ppt; 95 % CI) in the aged TTL, which agrees closely with a stratospheric injection of 2.6 ± 0.6 ppt of inorganic Bry (estimated from CFC-11 correlations), and is remarkably insensitive to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.6–7.0 ppt; 95 % CI) in the stratospheric "middleworld" and 6.9 ppt (6.5–7.3 ppt; 95 % CI) in the stratospheric "overworld". The local Bry minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-Chem, and suggests a more complex partitioning of gas-phase and aerosol Bry species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA-derived gas-phase Bry) are needed to explain the gas-phase Bry budget in the upper free troposphere and TTL. They are also consistent with observations of significant bromide in Upper Troposphere–Lower Stratosphere aerosols. The total Bry budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas-phase Bry species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. Such simultaneous measurements are needed to (1) quantify SSA-derived Bry in the upper FT, (2) test Bry partitioning, and possibly explain the gas-phase Bry minimum in the aged TTL, (3) constrain heterogeneous reaction rates of bromine, and (4) account for all of the sources of Bry to the lower stratosphere
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CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions
During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ∼ 0. 15 is consistent with the largely uniform and high O : C value (∼ 0. 8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through multivariable linear regression. For the SOA factors, the variation of the κ value with O : C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O : C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O : C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O : C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase in κorg with O : C, as observed during this and earlier field studies. This finding helps better understand and reconcile the differences in the relationships between κorg and O : C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context
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Global impacts of tropospheric halogens (Cl, Br, I) on oxidants and composition in GEOS-Chem
We present a simulation of the global present-day composition of the troposphere which includes the chemistry of halogens (Cl, Br, I). Building on previous work within the GEOS-Chem model we include emissions of inorganic iodine from the oceans, anthropogenic and biogenic sources of halogenated gases, gas phase chemistry, and a parameterised approach to heterogeneous halogen chemistry. Consistent with Schmidt et al. (2016) we do not include sea-salt debromination. Observations of halogen radicals (BrO, IO) are sparse but the model has some skill in reproducing these. Modelled IO shows both high and low biases when compared to different datasets, but BrO concentrations appear to be modelled low. Comparisons to the very sparse observations dataset of reactive Cl species suggest the model represents a lower limit of the impacts of these species, likely due to underestimates in emissions and therefore burdens. Inclusion of Cl, Br, and I results in a general improvement in simulation of ozone (O3) concentrations, except in polar regions where the model now underestimates O3 concentrations. Halogen chemistry reduces the global tropospheric O3 burden by 18.6%, with the O3 lifetime reducing from 26 to 22 days. Global mean OH concentrations of 1.28 × 106moleculescm-3 are 8.2% lower than in a simulation without halogens, leading to an increase in the CH4 lifetime (10.8%) due to OH oxidation from 7.47 to 8.28 years. Oxidation of CH4 by Cl is small (∼ 2%) but Cl oxidation of other VOCs (ethane, acetone, and propane) can be significant (∼ 15-27%). Oxidation of VOCs by Br is smaller, representing 3.9% of the loss of acetaldehyde and 0.9% of the loss of formaldehyde
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Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning
Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustion sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds–water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively. Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, and seasons and years. The model with representation of semivolatile POA improves predictions of hourly OA observations over the traditional nonvolatile model at sites during field campaigns in southern California (CalNex, May–June 2010), northern California (CARES, June 2010), the southeast US (SOAS, June 2013; SEARCH, January and July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from −5.62 to −2.42 µg m−3). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73 µg m−3, but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these more-complicated approaches as they currently rely on numerous uncertain parameters. The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in real pcSOA in different regions or time periods, too-high concentrations of other OA sources in the model that are important over the larger domain, or other model issues such as loss processes. This discrepancy is likely regionally and temporally dependent and driven by interferences from factors like varying emissions and chemical regimes
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Source attribution of Arctic black carbon constrained by aircraft and surface measurements
Black carbon (BC) contributes to Arctic warming, yet sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne (NETCARE 2015; PAMARCMiP 2009 and 2011 campaigns) and ground-based measurements (at Alert, Barrow and Ny-Ålesund) from multiple methods (thermal, laser incandescence and light absorption) with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. This is the first comparison with a chemical transport model of refractory BC (rBC) measurements at Alert. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to above 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Our simulations with the addition of seasonally varying domestic heating and of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE  < 13 %) and with airborne measurements of the BC vertical profile across the Arctic (rRMSE  = 17 %) except for an underestimation in the middle troposphere (500–700 hPa)