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Dust is one of the dominant aerosol types over Asia and the North Pacific Ocean, but quantitative estimation of dust distribution and its contribution to the total regional aerosol load from observations is challenging due to the presence of significant anthropogenic and natural aerosols and the frequent influence of clouds over the region. This study presents the dust aerosol distributions over Asia and the North Pacific using simulations from five global models that participated in the AeroCom phase II model experiments, and from multiple satellite remote-sensing and ground-based measurements of total aerosol optical depth (AOD) and dust optical depth (DOD). We examine various aspects of aerosol and dust presence in our study domain: (1) the horizontal distribution, (2) the longitudinal gradient during trans-Pacific transport, (3) seasonal variations, (4) vertical profiles, and (5) model-simulated dust life cycles. This study reveals that the diversity of DOD is mostly driven by the diversity of the dust source followed by residence time and mass extinction efficiency.

International audience; Ammonia (NH3) and nitrogen oxides (NOx: nitrogen dioxide [NO2] + nitric oxide [NO]) play important roles in atmospheric chemistry. Throughout most of Africa, emissions of these gases are predominantly from soils and biomass burning. Here we use observations of tropospheric NO2 vertical column densities (VCDs) from the Ozone Monitoring Instrument from 2005 through 2017 and atmospheric NH3 VCDs from the Infrared Atmospheric Sounding Interferometer from 2008 through 2017 to evaluate seasonal variation of NO2 and NH3 VCDs across Africa and in seven African ecoregions. In regions where mean annual precipitation (MAP) is under 500 mm yr−1, we find that NO2 and NH3 VCDs are positively related to monthly precipitation, and where MAP is between 500 and 1,750 mm yr−1 or higher, NO2 VCDs are negatively related to monthly precipitation. In dry ecoregions, temperature and precipitation were important predictors of NH3 and NO2 VCDs, likely related to variation in soil emissions. In mesic ecoregions, monthly NO2 VCDs were strongly related to burned area, suggesting that biomass burning drives seasonality. NH3 VCDs in mesic ecoregions were positively related to both monthly temperature and monthly carbon monoxide (CO) VCDs, suggesting that a mixture of soil and biomass burning emissions influenced NH3 seasonality. In northern mesic ecoregions, monthly temperature explained most of the variance in monthly NH3 VCDs, suggesting that soil sources, including animal excreta, determined NH3 seasonality. In southern mesic ecoregions, monthly CO VCDs explained more variation in NH3 VCDs than temperature, suggesting that biomass burning may have greater influence over NH3 seasonality.

Simulations of the CMIP6 historical period 1850–2014, characterized by the emergence of anthropogenic climate drivers like greenhouse gases, are presented for different configurations of the NASA Goddard Institute for Space Studies (GISS) Earth System ModelE2.1. The GISS‐E2.1 ensembles are more sensitive to greenhouse gas forcing than their CMIP5 predecessors (GISS‐E2) but warm less during recent decades due to a forcing reduction that is attributed to greater longwave opacity in the GISS‐E2.1 pre‐industrial simulations. This results in an atmosphere less sensitive to increases in opacity from rising greenhouse gas concentrations, demonstrating the importance of the base climatology to forcing and forced climate trends. Most model versions match observed temperature trends since 1979 from the ocean to the stratosphere. The choice of ocean model is important to the transient climate response, as found previously in CMIP5 GISS‐E2: the model that more efficiently exports heat to the deep ocean shows a smaller rise in tropospheric temperature. Model sea level rise over the historical period is traced to excessive drawdown of aquifers to meet irrigation demand with a smaller contribution from thermal expansion. This shows how fully coupled models can provide indirect observational constraints upon forcing, in this case, constraining irrigation rates with observed sea level changes. The overall agreement of GISS‐E2.1 with observed trends is familiar from evaluation of its predecessors, as is the conclusion that these trends are almost entirely anthropogenic in origin. We thank two anonymous reviewers for their comments that substantially improved this article. Development of GISS‐E2.1 was supported by the NASA Modeling, Analysis, and Prediction (MAP) Program. CMIP6 simulations with GISS‐E2.1 were made possible by the NASA High‐End Computing (HEC) Program through the NASA Center for Climate Simulation (NCCS) at Goddard Space Flight Center. We thank Ellen Salmon and the NCCS staff for hosting and providing convenient access to the model output. Peer Reviewed "Article signat per 47 autors/es: Ron L. Miller, Gavin A. Schmidt, Larissa S. Nazarenko, Susanne E. Bauer, Maxwell Kelley, Reto Ruedy, Gary L. Russell , Andrew S. Ackerman, Igor Aleinov, Michael Bauer, Rainer Bleck, Vittorio Canuto, Grégory Cesana, Ye Cheng, Thomas L. Clune, Ben I. Cook, Carlos A. Cruz, Anthony D. Del Genio, Gregory S. Elsaesser, Greg Faluvegi, Nancy Y. Kiang, Daehyun Kim, Andrew A. Lacis , Anthony Leboissetie,r Allegra N. LeGrande, Ken K. Lo, John Marshall, Elaine E. Matthews, Sonali McDermid, Keren Mezuman, Lee T. Murray, Valdar Oinas, Clara Orbe, Carlos Pérez García‐Pando, Jan P. Perlwitz, Michael J. Puma, David Rind, Anastasia Romanou, Drew T. Shindell, Shan Sun, Nick Tausnev, Kostas Tsigaridis, George Tselioudis, Ensheng Weng, Jingbo Wu, Mao‐Sung Yao"

The Earth's climate is rapidly changing. Over the past centuries, aerosols, via their ability to absorb or scatter solar radiation and alter clouds, played an important role in counterbalancing some of the greenhouse gas (GHG) caused global warming. The multicentury anthropogenic aerosol cooling effect prevented present‐day climate from reaching even higher surface air temperatures and subsequent more dramatic climate impacts. Trends in aerosol concentrations and optical depth show that in many polluted regions such as Europe and the United States, aerosol precursor emissions decreased back to levels of the 1950s. More recent polluting countries such as China may have reached a turning point in recent years as well, while India still follows an upward trend. Here we study aerosol trends in the Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations of the GISS ModelE2.1 climate model using a fully coupled atmosphere composition configuration, including interactive gas‐phase chemistry and either an aerosol microphysical (MATRIX) or a mass‐based (One‐Moment Aerosol, OMA) aerosol module. Results show that whether global aerosol radiative forcing is already declining depends on the aerosol scheme used. Using the aerosol microphysical scheme, where the aerosol system reacts more strongly to the trend in sulfur dioxide (SO2) emissions, global peak direct aerosol forcing was reached in the 1980s, whereas the mass‐based scheme simulates peak direct aerosol forcing around 2010.

The ability of 11 models in simulating the aerosol vertical distribution from regional to global scales, as part of the second phase of the AeroCom model intercomparison initiative (AeroCom II), is assessed and compared to results of the first phase. The evaluation is performed using a global monthly gridded data set of aerosol extinction profiles built for this purpose from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Layer Product 3.01. Results over 12 subcontinental regions show that five models improved, whereas three degraded in reproducing the interregional variability in Zα0–6 km, the mean extinction height diagnostic, as computed from the CALIOP aerosol profiles over the 0–6 km altitude range for each studied region and season. While the models' performance remains highly variable, the simulation of the timing of the Zα0–6 km peak season has also improved for all but two models from AeroCom Phase I to Phase II. The biases in Zα0–6 km are smaller in all regions except Central Atlantic, East Asia, and North and South Africa. Most of the models now underestimate Zα0–6 km over land, notably in the dust and biomass burning regions in Asia and Africa. At global scale, the AeroCom II models better reproduce the Zα0–6 km latitudinal variability over ocean than over land. Hypotheses for the performance and evolution of the individual models and for the intermodel diversity are discussed. We also provide an analysis of the CALIOP limitations and uncertainties contributing to the differences between the simulations and observations.

Particulate matter is a major concern for public health, causing cancer and cardiopulmonary mortality. Therefore, governments in most industrialized countries monitor and set limits for particulate matter. To assist policy makers, it is important to connect the chemical composition and severity of particulate pollution to its sources. Here we show how agricultural practices, livestock production, and the use of nitrogen fertilizers impact near-surface air quality. In many densely populated areas, aerosols formed from gases that are released by fertilizer application and animal husbandry dominate over the combined contributions from all other anthropogenic pollution. Here we test reduction scenarios of combustion-based and agricultural emissions that could lower air pollution. For a future scenario, we find opposite trends, decreasing nitrate aerosol formation near the surface while total tropospheric loads increase. This suggests that food production could be increased to match the growing global population without sacrificing air quality if combustion emission is decreased.

We examine the anthropogenically forced climate response for the 21st century representative concentration pathway (RCP) emission scenarios and their extensions for the period 2101–2500. The experiments were performed with ModelE2, a new version of the NASA Goddard Institute for Space Sciences (GISS) coupled general circulation model that includes three different versions for the atmospheric composition components: a noninteractive version (NINT) with prescribed composition and a tuned aerosol indirect effect (AIE), the TCAD version with fully interactive aerosols, whole-atmosphere chemistry, and the tuned AIE, and the TCADI version which further includes a parameterized first indirect aerosol effect on clouds. Each atmospheric version is coupled to two different ocean general circulation models: the Russell ocean model (GISS-E2-R) and HYCOM (GISS-E2-H). By 2100, global mean warming in the RCP scenarios ranges from 1.0 to 4.5°C relative to 1850–1860 mean temperature in the historical simulations. In the RCP2.6 scenario, the surface warming in all simulations stays below a 2°C threshold at the end of the 21st century. For RCP8.5, the range is 3.5–4.5°C at 2100. Decadally averaged sea ice area changes are highly correlated to global mean surface air temperature anomalies and show steep declines in both hemispheres, with a larger sensitivity during winter months. By the year 2500, there are complete recoveries of the globally averaged surface air temperature for all versions of the GISS climate model in the low-forcing scenario RCP2.6. TCADI simulations show enhanced warming due to greater sensitivity to CO2, aerosol effects, and greater methane feedbacks, and recovery is much slower in RCP2.6 than with the NINT and TCAD versions. All coupled models have decreases in the Atlantic overturning stream function by 2100. In RCP2.6, there is a complete recovery of the Atlantic overturning stream function by the year 2500 while with scenario RCP8.5, the E2-R climate model produces a complete shutdown of deep water formation in the North Atlantic.

Observations of climate change during the CMIP5 extended historical period (1850-2012) are compared to trends simulated by six versions of the NASA Goddard Institute for Space Studies ModelE2 Earth System Model. The six models are constructed from three versions of the ModelE2 atmospheric general circulation model, distinguished by their treatment of atmospheric composition and the aerosol indirect effect, combined with two ocean general circulation models, HYCOM and Russell. Forcings that perturb the model climate during the historical period are described. Five-member ensemble averages from each of the six versions of ModelE2 simulate trends of surface air temperature, atmospheric temperature, sea ice and ocean heat content that are in general agreement with observed trends, although simulated warming is slightly excessive within the past decade. Only simulations that include increasing concentrations of long-lived greenhouse gases match the warming observed during the twentieth century. Differences in twentieth-century warming among the six model versions can be attributed to differences in climate sensitivity, aerosol and ozone forcing, and heat uptake by the deep ocean. Coupled models with HYCOM export less heat to the deep ocean, associated with reduced surface warming in regions of deepwater formation, but greater warming elsewhere at high latitudes along with reduced sea ice. All ensembles show twentieth-century annular trends toward reduced surface pressure at southern high latitudes and a poleward shift of the midlatitude westerlies, consistent with observations.

We present a description of the ModelE2 version of the Goddard Institute for Space Studies (GISS) General Circulation Model (GCM) and the configurations used in the simulations performed for the Coupled Model Intercomparison Project Phase 5 (CMIP5). We use six variations related to the treatment of the atmospheric composition, the calculation of aerosol indirect effects, and ocean model component. Specifically, we test the difference between atmospheric models that have noninteractive composition, where radiatively important aerosols and ozone are prescribed from precomputed decadal averages, and interactive versions where atmospheric chemistry and aerosols are calculated given decadally varying emissions. The impact of the first aerosol indirect effect on clouds is either specified using a simple tuning, or parameterized using a cloud microphysics scheme. We also use two dynamic ocean components: the Russell and HYbrid Coordinate Ocean Model (HYCOM) which differ significantly in their basic formulations and grid. Results are presented for the climatological means over the satellite era (1980-2004) taken from transient simulations starting from the preindustrial (1850) driven by estimates of appropriate forcings over the 20th Century. Differences in base climate and variability related to the choice of ocean model are large, indicating an important structural uncertainty. The impact of interactive atmospheric composition on the climatology is relatively small except in regions such as the lower stratosphere, where ozone plays an important role, and the tropics, where aerosol changes affect the hydrological cycle and cloud cover. While key improvements over previous versions of the model are evident, these are not uniform across all metrics.

Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

Ice core measurements in conjunction with climate model simulations are of tremendous value when examining anthropogenic and natural aerosol loads and their role in past and future climates. Refractory black carbon (BC) records from the Arctic, the Antarctic, and the Himalayas are analyzed using three transient climate simulations performed with the Goddard Institute for Space Studies ModelE. Simulations differ in aerosol schemes (bulk aerosols vs. aerosol microphysics) and ocean couplings (fully coupled vs. prescribed ocean). Regional analyses for past (1850-2005) and future (2005-2100) carbonaceous aerosol simulations focus on the Antarctic, Greenland, and the Himalayas. Measurements from locations in the Antarctic show clean conditions with no detectable trend over the past 150 years. Historical atmospheric deposition of BC and sulfur in Greenland shows strong trends and is primarily influenced by emissions from early twentieth century agricultural and domestic practices. Models fail to reproduce observations of a sharp eightfold BC increase in Greenland at the beginning of the twentieth century that could be due to the only threefold increase in the North American emission inventory. BC deposition in Greenland is about 10 times greater than in Antarctica and 10 times less than in Tibet. The Himalayas show the most complicated transport patterns, due to the complex terrain and dynamical regimes of this region. Projections of future climate based on the four CMIP5 Representative Concentration Pathways indicate further dramatic advances of pollution to the Tibetan Plateau along with decreasing BC deposition fluxes in Greenland and the Antarctic.

Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth's energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically based model expresses the aerosol indirect effect (AIE) using analytic representations of cloud and aerosol distributions and processes. Although the simple model is able to produce estimates of AIEs that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates by the simple model are sensitive to preindustrial cloud condensation nuclei concentration, preindustrial accumulation mode radius, width of the accumulation mode, size of primary particles, cloud thickness, primary and secondary anthropogenic emissions, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Estimates of present-day AIEs as low as 5 W/sq m and as high as 0.3 W/sq m are obtained for plausible sets of parameter values. Estimates are surprisingly linear in emissions. The estimates depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models, which adds to understanding of the dependence on AIE uncertainty on uncertainty in parameter values.

Observations from the US Department of Energy's Atmospheric Radiation Measurement (ARM) program are used to evaluate the ability of the NASA GISS ModelE global climate model in reproducing observed interactions between aerosols and clouds. Included in the evaluation are comparisons of basic meteorology and aerosol properties, droplet activation, effective radius parameterizations, and surface-based evaluations of aerosol-cloud interactions (ACI). Differences between the simulated and observed ACI are generally large, but these differences may result partially from vertical distribution of aerosol in the model, rather than the representation of physical processes governing the interactions between aerosols and clouds. Compared to the current observations, the ModelE often features elevated droplet concentrations for a given aerosol concentration, indicating that the activation parameterizations used may be too aggressive. Additionally, parameterizations for effective radius commonly used in models were tested using ARM observations, and there was no clear superior parameterization for the cases reviewed here. This lack of consensus is demonstrated to result in potentially large, statistically significant differences to surface radiative budgets, should one parameterization be chosen over another.

[1] Rivers transport carbon (C) from terrestrial ecosystems to the coastal ocean, providing significant heterotrophic support within both rivers and receiving coastal waters. The amounts and ages of these terrestrial-river-coastal ocean C fluxes, however, are still poorly constrained. To address this uncertainty, a study of eight rivers discharging to the Middle Atlantic Bight (MAB) was undertaken. The rivers were sampled periodically over 2 years for concentrations and δ13C and Δ14C signatures of particulate organic C (POC), dissolved organic C (DOC), and dissolved inorganic C (DIC). For the watersheds draining to the MAB, it was estimated that ∼3800 Gg of terrestrial organic C (OC) and 700 Gg of terrestrial inorganic C was removed annually by fluvial transport. Of the terrestrial OC loss, ∼64% was contemporary C representing approximately 1% of the annual terrestrial net primary productivity. Net fluvial C inputs to the MAB shelf were estimated to be ∼70 Gg·yr − 1 of POC, 280 Gg·yr − 1 of DOC, and 800 Gg·yr − 1 of DIC. Terrestrial C, as opposed to in situ produced river C, comprised the majority of the riverine POC and DOC flux and around half of the total C flux. A smaller but significant fraction (

[1] Photochemical and microbial transformations of DOM were evaluated in headwater streams draining forested and human-modified lands (pasture, cropland, and urban development) by laboratory incubations. Changes in DOC concentrations, DOC isotopic signatures, and DOM fluorescence properties were measured to assess the amounts, sources, ages, and properties of reactive and refractory DOM under the influence of photochemistry and/or bacteria. DOC in streams draining forest-dominated watersheds was more photoreactive than in streams draining mostly human-modified watersheds, possibly due to greater contributions of terrestrial plant-derived DOC and lower amounts of prior light exposure in forested streams. Overall, the percentage of photoreactive DOC in stream waters was best predicted by the relative content of terrestrial fluorophores. The bioreactivity of DOC was similar in forested and human-modified streams, but variations were correlated with temperature and may be further controlled by the diagenetic status of organic matter. Alterations to DOC isotopes and DOM fluorescence properties during photochemical and microbial incubations were similar between forested and human-modified streams and included (1) negligible effects of microbial alteration on DOC isotopes and DOM fluorescence properties, (2) selective removal of 13C-depleted and 14C-enriched DOC under the combined influence of photochemical and microbial processes, and (3) photochemical alteration of DOM resulting in a preferential loss of terrestrial humic fluorescence components relative to microbial fluorescence components. This study provides a unique comparison of DOC reactivity in a regional group of streams draining forested and human-modified watersheds and indicates the importance of land use on the photoreactivity of DOC exported from upstream watersheds.

[1] Riverine exports of carbon (C) and organic matter (OM) are regulated by a variety of natural and anthropogenic factors. Understanding the relationships between these various factors and C and OM exports can help to constrain global C budgets and allow assessment of current and future anthropogenic impacts on both riverine and global C cycles. We quantified the effects of multiple natural and anthropogenic controls on riverine export fluxes and compositions of particulate organic C, dissolved organic C, and dissolved inorganic C for a regional group of eight rivers in the northeastern U.S. Potential controls related to hydrogeomorphology and regional climate, soil order, soil texture, bedrock lithology, land use, and anthropogenic factors were analyzed individually, collectively, and at scales of both local and regional influence. Factors related to hydrogeomorphology and climate, followed in importance by land use and anthropogenic factors, exhibited the strongest impacts on riverine C exports and compositions, particularly at smaller localized scales. The effects of hydrogeomorphology and climate were primarily related to volumetric flow, which resulted in greater exports of terrestrial and total C. Principal anthropogenic factors included impacts of wastewater treatment plants (WWTPs) and river impoundments. The presence of WWTPs as well as anthropogenic use of carbonate-based materials (e.g., limestone) may have substantially increased riverine C exports, particularly fossil C exports, in the study region. The presence of nuclear power plants in the associated watersheds is also discussed because of the potential for anthropogenic 14C inputs and subsequent biasing of aquatic C studies utilizing natural abundance 14C.

Continental shelves and slopes are productive and dynamic ocean margin systems that also regulate the fluxes of terrestrial, riverine, and estuarine materials between the continents and oceans. In order to evaluate the ages, potential sources, and transformations of organic matter in an ocean margin system, we measured the radiocarbon (A14C) and 613C distributions of total dissolved organic carbon (DOC), suspended particulate organic carbon (POC), and dissolved inorganic carbon (DIC) in waters of the Middle Atlantic Bight (MAB) continental shelf and slope in April-May 1994. The A•4C of DOC was greatest (as high as -39%0) in surface waters of the shelf, decreasing rapidly offshore and with depth, even in relatively shallow (25-50 m depth) shelf waters. The lowest A14C-DOC values were observed in deep slope waters, where they were significantly lower than values measured previously for the deep Sargasso Sea. There was a strong inverse relationship between A14C-DOC and 613C-DOC in all shelf and surface slope waters of the MAB, which is likely attributable to varying contributions of young, 14C-enriched organic matter of terrestrial and/or riverine origin. The more highly •4C-depleted DOC in deep slope waters (as low as -442%0) generally had a correspondingly lower bl3C (as low as -22.3%0) component. However, this must originate from relic terrestrial material either in the MAB itself or be discharged to the MAB from rivers and estuaries. The isotopic signatures of POC were clearly differentiable from DOC and indicate that this pool also contained a broad range of both old and young material of terrestrial (•3C as low as -24.9%0) and marine (•3C as high as -19.9%o) origin throughout the MAB shelf and slope. The highest A14C-POC values (up to 78%0) were observed in shallow shelf waters of the southern MAB. Conversely, the lowest A14C-POC values as low as -394%0) were found in MAB deep slope waters and were also significantly more depleted in 14C than POC from the central north Atlantic (Sargasso Sea). A multiple-source isotopic mass balance model employing both 14C and 13C was used to evaluate the relative contributions of both young and old terrigenous versus marine organic matter to DOC and POC in the MAB. The results indicate that shelf and slope DOC is comprised of an old marine fraction (represented by offshore Sargasso Sea material) and either a young terrestrial/riverine/ estuarine (TRE) component (in shelf and shallow slope waters) or a relic TRE component (in deep and some shallow slope waters). In contrast, suspended POC from the MAB appears to originate predominantly from a mixture of recent MAB primary production and an old, TRE component, similar to that observed in one of the major subestuaries of the Chesapeake Bay. These results suggest that both young and old sources of terrestrial and rivefine organic matter can comprise a significant fraction of the DOC and POC in ocean margins. Preliminary calculations indicate that the export of this compositionally unique DOC and suspended POC may be significant terms in the organic carbon budgets of the MAB and other margin systems

Dissolved organic carbon (DOC) is the largest actively exchanging pool of organic carbon in the ocean, yet its sources and sinks are not well constrained. The average 14C ages of DOC in the deep N. Atlantic and N. Pacific Oceans are 4,000 [Bauer et al., 1992; Druffel et al.,1992] and 6,000 years [Williams and Druffel, 1987], respectively, and represent the beginning and end of the deep ocean conveyor [Broecker, 1991]. Here we report that the deep Southern Ocean DOC has a 14C age (5,600 y) much closer to that of the deep N. Pacific, but its concentration in seawater (41±2 µM) is nearly equal to that of the deep N. Atlantic. The radiocarbon and concentration data indicate that most, but not all, deep DOC is transported conservatively with the ocean's conveyor. A younger (post-bomb) source of DOC to the N. Atlantic is the most likely explanation for the large age difference we observe between deep DOC in the Atlantic and Southern Oceans. Other possibilities are a source of older DOC or a smaller microbial sink in the S. Ocean, or perhaps a possible slowdown of S. Ocean deep water formation during the past century [Broecker et al., 1999].

We present Δ14C measurements of particulate organic carbon (POC) collected on four cruises at our time series site (station M) in the northeast Pacific Ocean. We observe a large gradient with depth in the suspended POC Δ14C values (124–160‰). These profiles display lower Δ14C values (by 20–30‰) in samples between 2500 m and the bottom during June 1992 and July 1993 than those during February and October 1992. Values of Δ14C in sinking POC from deep-moored sediment trap collections suggest a semiannual trend that displays lower overall Δ14C in material collected during periods of high flux. A limited number of Δ14C measurements of small swimmers picked from the trap 650 m above bottom are similar to surface Δ14C measurements of dissolved inorganic carbon (DIC) and suspended POC, indicating a surface carbon source. Overall, we postulate that the major process causing lower Δ14C values of deep suspended and sinking POC is sorption (or biological incorporation) of “old” DOC onto particulate matter. There appears to be a higher ratio of DOC sorbed to sinking particulate matter at times of high flux (late spring and early fall) that can be thought of as a “stripping out” of DOC from the water column. The DIC Δ14C display a small seasonal variation in the surface waters and is not the sole source of the observed seasonality in the POC Δ14C signals.

[1] Rivers transport globally significant amounts of carbon (C) from terrestrial ecosystems to ocean margins. Understanding and quantifying the sources and respective contributions to riverine C has emerged as an important biogeochemical problem that can be approached through natural-abundance isotope mass balance. Traditionally, the sources of riverine C have been identified either qualitatively or quantitatively through application of static mixing models. However, both source signatures and contributions can vary significantly with time. Here we apply two time-based mixing models to a study of six rivers draining the northeast U.S. In the first model, a time-averaged mixing model (TAMM), we vary only the source isotopic (δ13C and Δ14C) signatures. In the second model, a time-varying mixing model (TVMM), we allow both isotopic signatures and contributions to vary with time. Based on results from the TVMM, drivers of variation in riverine particulate organic C (POC), dissolved organic C (DOC), and dissolved inorganic C (DIC) include stream discharge, stream discharge and water temperature, and water temperature and vegetation phenology, respectively. Major sources include C3plant material, algal material and slow-turnover soil OC (“slow SOC”), which together account for 50%–100% (95% CI) of riverine POC; C3plant material and slow SOC, which together typically account for 60%–100% (95% CI) of DOC; and atmospheric exchange which alone typically accounts for 40%–60% (95% CI) of DIC. Seasonal change in relative contributions from algal material, slow SOC, and photosynthesis (in response to the identified drivers) dominates the observed variation in POC, DOC and DIC, respectively. The TVMM is a novel tool to identify component contributions under more realistic non-static conditions, and with potential application to a broad range of biogeochemical studies.

nd 0.22 0.47 0.34 0.29 0.16 0.26 0.24 0.28 WIOC d d 13 C( ‰ )n d � 26.0 � 25.1 � 25.6 � 26.7 � 26.8 � 24.2 � 25.9 � 25.8 D 14 C( ‰ )n d � 45 42 � 1 � 367 � 461 � 231 � 353 � 212 fWIOC nd 0.78 0.53 0.66 0.71 0.84 0.74 0.76 0.72 TSE e d 13 C( ‰) � 27.0 nd � 26.2 � 26.6 nd � 27.3 � 28.2 � 27.6 � 27.2 D 14 C( ‰) � 476 nd � 90 � 283 nd � 430 � 119 � 190 � 227 fTSE 0.67 nd 0.90 0.79 nd 0.43 0.74 0.59 0.69 Aliphatic d 13 C( ‰) � 28.6 � 27.7 nd f � 28.2 nd � 27.3 � 28.9 � 28.1 � 28.1 D 14 C( ‰) � 794 � 820 � 961 � 858 nd � 834 � 858 � 846 � 853 faliphatic 0.007 0.001 0.003 0.0039 nd 0.007 0.002 0.004 0.004 Aromatic d 13 C( ‰) � 27.8 � 29.6 � 28.3 � 28.6 � 28.3 � 28.4 � 27.8 � 28.2 � 28.4 D 14 C( ‰) � 692 � 77 � 446 � 405 � 466 � 540 � 446 � 484 � 444 faromatic 0.015 0.009 0.004 0.009 0.009 0.007 0.003 0.007 0.006 Polar d 13 C( ‰) � 27.8 � 26.1 � 28.0 � 27.3 � 28.6 nd � 26.2 � 27.4 � 27.3 D 14 C( ‰) � 750 24 � 93 � 273 � 168 nd � 240 � 204 � 245 fpolar 0.24 0.039 0.25 0.18 0.063 nd 0.066 0.065 0.13 a All reported d 13 C and D 14 C values were corrected for blank contributions following procedures outlined in the text. b ‘nd’ denotes samples for which values were not determined. c Values represent the fraction of TOC accounted for by the parameter of interest (f

[1] Carbon isotopic signatures (δ13C, Δ14C) of aerosol particulate matter total organic carbon (TOC) and operationally defined organic carbon (OC) components were measured in samples from two background sites in the eastern U.S. TOC and water-soluble OC (WSOC)δ13C values (−27 to −24‰) indicated predominantly terrestrial C3 plant and fossil derived sources. Total solvent extracts (TSE) and their aliphatic, aromatic, and polar OC components were depleted in δ13C (−30 to −26‰) relative to TOC and WSOC. Δ14C signatures of aerosol TOC and TSE (−476 to +25‰) suggest variable fossil contributions (∼5–50%) to these components. Aliphatic OC while comprising a small portion of the TOC (

The CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) layer product is used for a multimodel evaluation of the vertical distribution of aerosols. Annual and seasonal aerosol extinction profiles are analyzed over 13 sub-continental regions representative of industrial, dust, and biomass burning pollution, from CALIOP 2007-2009 observations and from AeroCom (Aerosol Comparisons between Observations and Models) 2000 simulations. An extinction mean height diagnostic (Z-alpha) is defined to quantitatively assess the models' performance. It is calculated over the 0-6 km and 0-10 km altitude ranges by weighting the altitude of each 100 m altitude layer by its aerosol extinction coefficient. The mean extinction profiles derived from CALIOP layer products provide consistent regional and seasonal specificities and a low inter-annual variability. While the outputs from most models are significantly correlated with the observed Z-alpha climatologies, some do better than others, and 2 of the 12 models perform particularly well in all seasons. Over industrial and maritime regions, most models show higher Z-alpha than observed by CALIOP, whereas over the African and Chinese dust source regions, Z-alpha is underestimated during Northern Hemisphere Spring and Summer. The positive model bias in Z-alpha is mainly due to an overestimate of the extinction above 6 km. Potential CALIOP and model limitations, and methodological factors that might contribute to the differences are discussed.

The anthropogenic increase in aerosol concentrations since preindustrial times and its net cooling effect on the atmosphere is thought to mask some of the greenhouse gas-induced warming. Although the overall effect of aerosols on solar radiation and clouds is most certainly negative, some individual forcing agents and feedbacks have positive forcing effects. Recent studies have tried to identify some of those positive forcing agents and their individual emission sectors, with the hope that mitigation policies could be developed to target those emitters. Understanding the net effect of multisource emitting sectors and the involved cloud feedbacks is very challenging, and this paper will clarify forcing and feedback effects by separating direct, indirect, semidirect and surface albedo effects due to aerosols. To this end, we apply the Goddard Institute for Space Studies climate model including detailed aerosol microphysics to examine aerosol impacts on climate by isolating single emission sector contributions as given by the Coupled Model Intercomparison Project Phase 5 (CMIP5) emission data sets developed for Intergovernmental Panel on Climate Change (IPCC) AR5. For the modeled past 150 years, using the climate model and emissions from preindustrial times to present-day, the total global annual mean aerosol radiative forcing is -0.6 W/m(exp 2), with the largest contribution from the direct effect (-0.5 W/m(exp 2)). Aerosol-induced changes on cloud cover often depends on cloud type and geographical region. The indirect (includes only the cloud albedo effect with -0.17 W/m(exp 2)) and semidirect effects (-0.10 W/m(exp 2)) can be isolated on a regional scale, and they often have opposing forcing effects, leading to overall small forcing effects on a global scale. Although the surface albedo effects from aerosols are small (0.016 W/m(exp 2)), triggered feedbacks on top of the atmosphere (TOA) radiative forcing can be 10 times larger. Our results point out that each emission sector has varying impacts by geographical region. For example, the single sector most responsible for a net positive radiative forcing is the transportation sector in the United States, agricultural burning and transportation in Europe, and the domestic emission sector in Asia. These sectors are attractive mitigation targets.

[1] This study evaluates currently available imagery from Landsat, MERIS, MODIS, and AWiFS sensors for their usefulness in regional-scale measurements of lake water clarity and chlorophyll for comprehensive lake management and scientific studies (e.g., modeling). Images from these systems were collected nearly concurrently and processed using methods similar to those developed previously for regional assessments of lake water clarity using Landsat imagery. We tested both atmospherically corrected and uncorrected imagery products; the uncorrected products performed as well as or better than the atmospherically corrected products in empirical relationships to estimate water clarity and chlorophyll. MODIS and MERIS systems, which have large swath widths and high temporal coverage are well suited for regional assessments of large lakes, but their low spatial resolution limits the number of lakes that can be assessed. Landsat imagery allows all lakes ≥4 ha (more than 12,000 in Minnesota) to be assessed, but its low spectral resolution limits assessments to water clarity. The MERIS system, with spectral and spatial resolution suitable for large (>150 ha) lakes, was the only system with a spectral band set that measured key absorption and scattering characteristics of phytoplankton that could be used reliably for regional chlorophyll assessments. Although none of the currently available systems is ideal, the study yielded a better definition of the spectral, spatial, and temporal characteristics of the ideal system for regional-scale water quality remote sensing that may be realized in upcoming satellite systems.

[1] Atmospheric particulate matter samples were collected from mid-Atlantic and northeastern U.S. (Virginia and New York, respectively) sites to assess the fossil versus contemporary sources contributing to aerosol organic carbon (OC) and the implications for its deposition to watersheds. Mean particulate matter total OC (TOC) deposition rates (wet + dry deposition) were calculated to be 1.6 and 2.4 mg C m−2 d−1 for the Virginia and New York sites, respectively. Wet deposition of particulate TOC was determined to be the dominant depositional mode, accounting for >65% (Virginia) and >80% (New York) of total aerosol TOC deposition. Isotopic mass balances suggest that, on average, the deposited aerosol TOC consisted of 66% (Virginia) and 68% (New York) contemporary biomass-derived material. The balance was fossil-derived material (34% and 32% for Virginia and New York, respectively), indicating significant anthropogenic fossil fuel contributions to aerosol TOC. When considered within representative northeastern U.S. watershed OC budgets, aerosol TOC depositional flux was up to 10% of net soil OC accumulation rates, and 5–70% of the OC throughfall flux for forested regions. When scaled to the entire Hudson and York River watersheds, estimated aerosol TOC depositional fluxes ranged from 6.1 to 9.7 × 1010 g C yr−1 and from 8.9 to 14 × 109 g C yr−1, respectively, and were similar in magnitude to the mean annual river OC export for these two systems (Hudson, 7.2 × 1010 g C yr−1; York, 8.4 × 109 g C yr−1). These findings underscore the potential importance of both natural and fossil fuel-derived aerosol OC inputs to watersheds.

Accurately representing aerosol-cloud interactions in global climate models is challenging. As parameterizations evolve, it is important to evaluate their performance with appropriate use of observations. In this investigation we compare aerosols, clouds, and their interactions in three global climate models (Geophysical Fluid Dynamics Laboratory-Atmosphere Model 3 (AM3), National Center for Atmospheric Research-Community Atmosphere Model 5 (CAM5), and Goddard Institute for Space Studies-ModelE2) to Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) satellite observations. Modeled cloud properties are diagnosed using a MODIS simulator. Cloud droplet number concentrations (N) are computed identically from satellite-simulated and MODIS-observed values of liquid cloud optical depth and droplet effective radius. We find that aerosol optical depth (τa) simulated by models is similar to observations in many regions around the globe. For N, AM3 and CAM5 capture the observed spatial pattern of higher values in coastal marine stratocumulus versus remote ocean regions, though modeled values, in general, are higher than observed. Aerosol-cloud interactions were computed as the sensitivity of ln(N) to ln(τa) for coastal marine liquid clouds near South Africa (SAF) and Southeast Asia where τa varies in time. AM3 and CAM5 are more sensitive than observations, while the sensitivity for ModelE2 is statistically insignificant. This widely used sensitivity could be subject to misinterpretation due to the confounding influence of meteorology on both aerosols and clouds. A simple framework for assessing the sensitivity of ln(N) to ln(τa) at constant meteorology illustrates that observed sensitivity can change from positive to statistically insignificant when including the confounding influence of relative humidity. Satellite-simulated versus standard model values of N are compared; for CAM5 in SAF, standard model values are significantly lower than satellite-simulated values with a bias of 83 cm−3.

[1] We investigate the climate forcing from and response to projected changes in short-lived species and methane under an A1B scenario from 2000-2050 in the GISS climate model. We present a meta-analysis of new simulations of the full evolution of gas and aerosol species and other existing experiments with variations of the same model. The comparison highlights the importance of several physical processes in determining radiative forcing, especially the effect of climate change on stratosphere-troposphere exchange, heterogeneous sulfate-nitrate-dust chemistry, and changes in methane oxidation and natural emissions. However, the impact of these fairly uncertain physical effects is substantially less than the difference between alternative emission scenarios for all short-lived species. The net global mean annual average direct radiative forcing from the short-lived species is .02 W/m2 or less in our projections, as substantial positive ozone forcing is largely offset by negative aerosol direct forcing. Since aerosol reductions also lead to a reduced indirect effect, the global mean surface temperature warms by ∼0.07°C by 2030 and ∼0.13°C by 2050, adding 19% and 17%, respectively, to the warming induced by long-lived greenhouse gases. Regional direct forcings are large, up to 3.8 W/m2. The ensemble-mean climate response shows little regional correlation with the spatial pattern of the forcing, however, suggesting that oceanic and atmospheric mixing generally overwhelms the effect of even large localized forcings. Exceptions are the polar regions, where ozone and aerosols may induce substantial seasonal climate changes.

[1] Coating of mineral dust particles by air pollutants leads to core-mantle particles. These composite aerosols could interact differently with atmospheric radiation than the uncoated dust. In our simplified radiative calculations we assumed that a spherical dust core is covered uniformly by a liquid refractive material, such as sulfate or nitrate. Theoretical calculations of optical properties of such particles show that the single-scattering albedo and the asymmetry parameter of core-mantle aerosols only differ significantly from uncoated dust if coating layers exceed 20% of the radius of the dust core. Global simulations of sulfate/nitrate-coated dust particles show that the thickness of the shell can be expected to range from 0 to 20% of the radius of the dust core. The result of this work is that mineral dust particles can be treated as external mixture within radiative calculations but the coating processes lead to changed loads in sulfate, nitrate, and mineral dust aerosol loads and therefore change their impact on Earth radiation. The combined anthropogenic forcing of dust, nitrate, and sulfate aerosols is −0.1 W/m2; however, excluding heterogeneous interactions leads to a 3 times larger negative forcing.

We report concentrations and isotope measurements (radiocarbon and stable carbon) of dissolved inorganic carbon (DIC) and suspended particulate organic carbon (POC) in waters collected from the mouth of the Amazon River and the North Brazil Current. Samples were collected in November 1991, when the Amazon hydrograph was at its annual minimum and the North Brazil Current had retroflected into the equatorial North Atlantic. The DIC Δ14C results revealed postbomb carbon in river and ocean waters, with slightly higher values at the river mouth. The low DIC δ13C signature of the river end-member (−11‰) demonstrates that about half of the DIC originated from the remineralization of terrestrially derived organic matter. A linear relationship between DIC and salinity indicates that DIC was mixed nearly conservatively in the transition zone from the river mouth to the open ocean, though there was a small amount (≤10%) of organic matter remineralization in the mesohaline region. The POC Δ14C values in the river mouth were markedly lower than those values from the western Amazon region (Hedges et al., 1986). We conclude that the dominant source of POC near the river mouth and in the inner Amazon plume during November 1991 was aged, resuspended material of significant terrestrial character derived from shelf sediments, while the outer plume contained mainly marine-derived POC.

[1] We use a global climate model to compare the effectiveness of many climate forcing agents for producing climate change. We find a substantial range in the “efficacy” of different forcings, where the efficacy is the global temperature response per unit forcing relative to the response to CO2 forcing. Anthropogenic CH4 has efficacy ∼110%, which increases to ∼145% when its indirect effects on stratospheric H2O and tropospheric O3 are included, yielding an effective climate forcing of ∼0.8 W/m2 for the period 1750–2000 and making CH4 the largest anthropogenic climate forcing other than CO2. Black carbon (BC) aerosols from biomass burning have a calculated efficacy ∼58%, while fossil fuel BC has an efficacy ∼78%. Accounting for forcing efficacies and for indirect effects via snow albedo and cloud changes, we find that fossil fuel soot, defined as BC + OC (organic carbon), has a net positive forcing while biomass burning BC + OC has a negative forcing. We show that replacement of the traditional instantaneous and adjusted forcings, Fi and Fa, with an easily computed alternative, Fs, yields a better predictor of climate change, i.e., its efficacies are closer to unity. Fs is inferred from flux and temperature changes in a fixed-ocean model run. There is remarkable congruence in the spatial distribution of climate change, normalized to the same forcing Fs, for most climate forcing agents, suggesting that the global forcing has more relevance to regional climate change than may have been anticipated. Increasing greenhouse gases intensify the Hadley circulation in our model, increasing rainfall in the Intertropical Convergence Zone (ITCZ), Eastern United States, and East Asia, while intensifying dry conditions in the subtropics including the Southwest United States, the Mediterranean region, the Middle East, and an expanding Sahel. These features survive in model simulations that use all estimated forcings for the period 1880–2000. Responses to localized forcings, such as land use change and heavy regional concentrations of BC aerosols, include more specific regional characteristics. We suggest that anthropogenic tropospheric O3 and the BC snow albedo effect contribute substantially to rapid warming and sea ice loss in the Arctic. As a complement to a priori forcings, such as Fi, Fa, and Fs, we tabulate the a posteriori effective forcing, Fe, which is the product of the forcing and its efficacy. Fe requires calculation of the climate response and introduces greater model dependence, but once it is calculated for a given amount of a forcing agent it provides a good prediction of the response to other forcing amounts.

A 6-year time series of Δ14C, δ13C, and C/N measurements in deep sinking particulate organic matter (POM) is presented for an abyssal site, Station M in the northeast Pacific Ocean. The Δ14C values revealed that sinking POM at 3450 m depth (650 m above bottom) contained old carbon despite its presumed short transit time in the water column. The isotopic and chemical properties of the sinking POM varied with time and appear to be controlled by more than one major process. In 1993, 1994, and late 1996, isotopic signatures and C/N molar ratios indicate negligible or vertically homogeneous influence of resuspended particles from the bottom or particles laterally transported from the margin to the study site. However, during early 1995 and 1998, Δ14C values were lower than those during other periods and C/N values at three deep depths were not equal, indicating that the study site was influenced by resuspended sediments more severely than during other periods. During mid-1995 to mid-1996, δ13C values decreased abruptly while Δ14C values increased slightly, and C/N values were extremely high (up to ∼80) at 50 and 600 m above bottom; these results suggest input of degraded, modern, terrestrial organic matter. The periods of anomalous isotopic signatures, as well as vertically heterogeneous C/N values [ Smith et al., 2001], were correlated with high discharge periods of California rivers with a time lag of 2 to 4 months. The correlation suggests that regional meteorological events are important in controlling the biogeochemical properties of particles at Station M by varying the intensity of resuspension and transport of organic matter from the continental margin.

meltwater pulse is assumed to have a volume of 1.6 10 14 m 3 and a period of discharge of 2 years on the basis of glaciological modeling of the decay of the Laurentide Ice Sheet (LIS). We present a possible mechanism which can explain the centennial duration of the 8.2 ka cold event. The mechanism is related to the existence of an additional equilibrium climate state with reduced North Atlantic Deep Water (NADW) formation and a southward shift of the NADW formation area. Hints at the additional climate state were obtained from the largely varying duration of the pulse-induced cold episode in response to overlaid random freshwater fluctuations in Monte Carlo simulations. The model equilibrium state was attained by releasing a weak multicentury freshwater flux through the St. Lawrence pathway completed by the meltwater pulse. The existence of such a climate mode appears essential for reproducing climate anomalies in close agreement with paleoclimatic reconstructions of the 8.2 ka event. The results furthermore suggest that the temporal evolution of the cold event was partly a matter of chance. INDEX TERMS: 3344 Meteorology and Atmospheric Dynamics: Paleoclimatology; 4255 Oceanography: General: Numerical modeling; 4532 Oceanography: Physical: General circulation; 4215 Oceanography: General: Climate and interannual variability (3309); 9325 Information Related to Geographic Region: Atlantic Ocean

[1] In the late 1980s, bomb 14C was present in suspended particulate organic carbon (POC) from the North Central Pacific (NCP) and Sargasso Sea (SS) throughout most of the water column, demonstrating that deep POC had exchanged with atmospheric CO2 in the past 30 years. Upon reoccupation of these sites in 1999 and 2000, respectively, we observed that the δ13C values of suspended POC were lower than those measured a decade earlier. This demonstrates that anthropogenic CO2 from fossil fuel and biomass burning has penetrated a major organic matter pool in the deep ocean. Δ14C measured in the suspended POC showed similar or higher values in the deep Sargasso Sea and decreased values in the deep NCP compared to those measured previously. We use a box model to show that the differences in the radiocarbon results are likely due to the presence of resuspended sediment that is laterally advected from the continental margin to the deep Sargasso Sea.

Radiocarbon (Δ14C), δ13C, bulk carbon and organic constituent concentration measurements are presented for dissolved and particulate carbon pools from the North Central Pacific Ocean (NCP) and the Sargasso Sea (SS). We operationally define three overlapping pools of dissolved organic carbon (DOC): (1) DOC that is oxidizable by UV radiation (DOC uv ); (2) “extra” DOC measured by Co/CoO flow-through high-temperature catalytic oxidation (DOC Ft-htc ), which also has low Δ14C values like DOC uv (Bauer et al., 1992a); and (3) a potential residual DOC fraction that is the difference between DOC measured by discrete-injection high-temperature catalytic oxidation (DOC htc ) and DOC Ft-htc , and which has unknown Δ14C signature. The distribution of a large fraction of DOC appears to be controlled by circulation of deep ocean waters between major oceans. The DOC in the SS is slightly younger than would be expected if circulation was the sole process controlling DOC cycling. We propose that there is more bomb 14C in the deep SS DOC to account for this difference. The Δ14C values of suspended, and to a lesser extent sinking particulate organic carbon (POC), decrease with depth, with the suspended POC displaying a much steeper gradient in the SS than in the NCP. These data reflect the incorporation of low-activity organic matter into the POC pool, possibly through incorporation of DOC by physical adsorption and/or biological heterotrophy.