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Atmospheric deposition of anthropogenic soluble iron (Fe) to the ocean has been suggested to modulate primary ocean productivity and thus indirectly affect the climate. A key process contributing to anthropogenic sources of soluble Fe is associated with air pollution, which acidifies Fe-containing mineral aerosols during their transport and leads to Fe transformation from insoluble to soluble forms. However, there is large uncertainty in our estimate of this anthropogenic soluble Fe. In this study, for the first time, we interactively combined laboratory kinetic experiments with global aerosol modeling to more accurately quantify anthropogenic soluble Fe due to air pollution. Firstly, we determined Fe dissolution kinetics of African dust samples at acidic pH values with and without ionic species commonly found in aerosol water (i.e., sulfate and oxalate). Then, by using acidity as a master variable, we constructed a new empirical scheme for Fe release from mineral dust due to inorganic and organic anions in aerosol water. We implemented this new scheme and applied an updated mineralogical emission database in a global atmospheric chemistry transport model to estimate the atmospheric concentration and deposition flux of soluble Fe under preindustrial and modern conditions. Our improved model successfully captured the inverse relationship of Fe solubility and total Fe loading measured over the North Atlantic Ocean (i.e., 1–2 orders of magnitude lower Fe solubility in northern-African- than combustion-influenced aerosols). The model results show a positive relationship between Fe solubility and water-soluble organic carbon (WSOC)/Fe molar ratio, which is consistent with previous field measurements. We estimated that deposition of soluble Fe to the ocean increased from 0.05–0.07 Tg Fe yr−1 in the preindustrial era to 0.11–0.12 Tg Fe yr−1 in the present day, due to air pollution. Over the high-nitrate, low-chlorophyll (HNLC) regions of the ocean, the modeled Fe solubility remains low for mineral dust (

The flux of carbon dioxide from the soil to the atmosphere (soil respiration) is one of the major fluxes in the global carbon cycle. At present, the accumulated field observation data cover a wide range of geographical locations and climate conditions. However, there are still large uncertainties in the magnitude and spatiotemporal variation of global soil respiration. Using a global soil respiration data set, we developed a climate-driven model of soil respiration by modifying and updating Raich's model, and the global spatiotemporal distribution of soil respiration was examined using this model. The model was applied at a spatial resolution of 0.5°and a monthly time step. Soil respiration was divided into the heterotrophic and autotrophic components of respiration using an empirical model. The estimated mean annual global soil respiration was 91 Pg C yr−1 (between 1965 and 2012; Monte Carlo 95 % confidence interval: 87–95 Pg C yr−1) and increased at the rate of 0.09 Pg C yr−2. The contribution of soil respiration from boreal regions to the total increase in global soil respiration was on the same order of magnitude as that of tropical and temperate regions, despite a lower absolute magnitude of soil respiration in boreal regions. The estimated annual global heterotrophic respiration and global autotrophic respiration were 51 and 40 Pg C yr−1, respectively. The global soil respiration responded to the increase in air temperature at the rate of 3.3 Pg C yr−1 °C−1, and Q10 = 1.4. Our study scaled up observed soil respiration values from field measurements to estimate global soil respiration and provide a data-oriented estimate of global soil respiration. The estimates are based on a semi-empirical model parameterized with over one thousand data points. Our analysis indicates that the climate controls on soil respiration may translate into an increasing trend in global soil respiration and our analysis emphasizes the relevance of the soil carbon flux from soil to the atmosphere in response to climate change. Further approaches should additionally focus on climate controls in soil respiration in combination with changes in vegetation dynamics and soil carbon stocks, along with their effects on the long temporal dynamics of soil respiration. We expect that these spatiotemporal estimates will provide a benchmark for future studies and also help to constrain process-oriented models.

We assessed the global terrestrial budget of methane (CH4) by using a process-based biogeochemical model (VISIT) and inventory data for components of the budget that were not included in the model. Emissions from wetlands, paddy fields, biomass burning, and plants, as well as oxidative consumption by upland soils, were simulated by the model. Emissions from ruminant livestock and termites were evaluated by using an inventory approach. These CH4 flows were estimated for each of the model's 0.5° × 0.5° grid cells from 1901 to 2009, while accounting for atmospheric composition, meteorological factors, and land-use changes. Estimation uncertainties were examined through ensemble simulations using different parameterization schemes and input data (e.g., different wetland maps and emission factors). From 1996 to 2005, the average global terrestrial CH4 budget was estimated on the basis of 1152 simulations, and terrestrial ecosystems were found to be a net source of 308.3 ± 20.7 Tg CH4 yr−1. Wetland and livestock ruminant emissions were the primary sources. The results of our simulations indicate that sources and sinks are distributed highly heterogeneously over the Earth's land surface. Seasonal and interannual variability in the terrestrial budget was also assessed. The trend of increasing net emission from terrestrial sources and its relationship with temperature variability imply that terrestrial CH4 feedbacks will play an increasingly important role as a result of future climatic change.

In many science, technology, engineering, and mathematics disciplines, women are outperformed by men in test scores, jeopardizing their success in science-oriented courses and careers. The current study tested the effectiveness of a psychological intervention, called values affirmation, in reducing the gender achievement gap in a college-level introductory physics class. In this randomized double-blind study, 399 students either wrote about their most important values or not, twice at the beginning of the 15-week course. Values affirmation reduced the male-female performance and learning difference substantially and elevated women's modal grades from the C to B range. Benefits were strongest for women who tended to endorse the stereotype that men do better than women in physics. A brief psychological intervention may be a promising way to address the gender gap in science performance and learning.

Significant amounts of carbon and nutrients are released to the atmosphere due to large fires in forests. Characterization of the spatial distribution and temporal variation of the intense fire emissions is crucial for assessing the atmospheric loadings of trace gases and aerosols. This paper discusses issues of the representation of forest fires in the estimation of emissions and the application to an atmospheric chemistry transport model (CTM). The potential contribution of forest fires to the deposition of bioavailable iron (Fe) into the ocean is highlighted, with a focus on mega fires in eastern Siberia. Satellite products of burned area, active fire, and land cover are used to estimate biomass burning emissions in conjunction with a biogeochemical model. Satellite-derived plume height from MISR is used for the injection height of boreal forest fire emissions. This methodology is applied to quantify fire emission rates in each three-dimensional grid location in the high latitude Northern Hemisphere (>30° N latitude) over a 5-yr period from 2001 to 2005. There is large interannual variation in forest burned area during 2001–2005 (13–49 × 103 km2 yr−1) which results in a corresponding variation in the annual emissions of carbon monoxide (CO) (14–81 Tg CO y−1). Satellite observations of CO column from MOPITT are used to evaluate the model performance in simulating the spatial distribution and temporal variation of the fire emissions. The model results for CO enhancements due to eastern Siberian fires are in good agreement with MOPITT observations. These validation results suggest that the model using emission rates estimated in this work is able to describe the interannual changes in CO due to intense forest fires. Bioavailable iron is derived from atmospheric processing of relatively insoluble iron from desert sources by anthropogenic pollutants (mainly sulfuric acid formed from oxidation of SO2) and from direct emissions of soluble iron from combustion sources. Emission scenarios for IPCC AR5 report (Intergovernmental Panel on Climate Change; Fifth Assessment Report) suggest that anthropogenic SO2 emissions are suppressed in the future to improve air quality. In future warmer and drier climate, severe fire years such as 2003 may become more frequent in boreal regions. The fire emission rates estimated in this study are applied to the aerosol chemistry transport model to examine the relative importance of biomass burning sources of soluble iron compared to those from dust sources. The model reveals that extreme fire events contribute to a significant deposition of soluble iron (20–40 %) to downwind regions over the western North Pacific Ocean, compared to the dust sources with no atmospheric processing by acidic species. These results suggest that the supply of nutrients from large forest fires plays a role as a negative biosphere-climate feedback with regards to the ocean fertilization.

Terrestrial ecosystems play a vital role in regulating the accumulation of carbon (C) in the atmosphere. Understanding the factors controlling land C uptake is critical for reducing uncertainties in projections of future climate. The relative importance of changing climate, rising atmospheric CO 2 , and other factors, however, remains unclear despite decades of research. Here, we use an ensemble of land models to show that models disagree on the primary driver of cumulative C uptake for 85% of vegetated land area. Disagreement is largest in model sensitivity to rising atmospheric CO 2 which shows almost twice the variability in cumulative land uptake since 1901 (1 s.d. of 212.8 PgC vs. 138.5 PgC, respectively). We find that variability in CO 2 and temperature sensitivity is attributable, in part, to their compensatory effects on C uptake, whereby comparable estimates of C uptake can arise by invoking different sensitivities to key environmental conditions. Conversely, divergent estimates of C uptake can occur despite being based on the same environmental sensitivities. Together, these findings imply an important limitation to the predictability of C cycling and climate under unprecedented environmental conditions. We suggest that the carbon modeling community prioritize a probabilistic multi-model approach to generate more robust C cycle projections.

There is growing interest in the formation of secondary organic aerosol (SOA) through condensed aqueous-phase reactions. In this study, we use a global model (IMPACT) to investigate the potential formation of SOA in the aqueous phase. We compare results from several multiphase process schemes with detailed aqueous-phase reactions to schemes that use a first-order gas-to-particle formation rate based on uptake coefficients. The predicted net global SOA production rate in cloud water ranges from 13.1 Tg yr−1 to 46.8 Tg yr−1 while that in aerosol water ranges from −0.4 Tg yr−1 to 12.6 Tg yr−1. The predicted global burden of SOA formed in the aqueous phase ranges from 0.09 Tg to 0.51 Tg. A sensitivity test to investigate two representations of cloud water content from two global models shows that increasing cloud water by an average factor of 2.7 can increase the net SOA production rate in cloud water by a factor of 4 at low altitudes (below approximately 900 hPa). We also investigated the importance of including dissolved Fe chemistry in cloud water aqueous reactions. Adding these reactions increases the formation rate of aqueous-phase OH by a factor of 2.6 and decreases the amount of global aqueous SOA formed by 31%. None of the mechanisms discussed here is able to provide a best fit for all observations. Rather, the use of an uptake coefficient method for aerosol water and a multi-phase scheme for cloud water provides the best fit in the Northern Hemisphere and the use of multiphase process scheme for aerosol and cloud water provides the best fit in the tropics. The model with Fe chemistry underpredicts oxalate measurements in all regions. Finally, the comparison of oxygen-to-carbon (O / C) ratios estimated in the model with those estimated from measurements shows that the modeled SOA has a slightly higher O / C ratio than the observed SOA for all cases.

Cold‐season methane (CH4) emissions may be poorly constrained in wetland models. We examined cold‐season CH4 emissions simulated by 16 models participating in the Global Carbon Project model intercomparison and analyzed temporal and spatial patterns in simulation results using prescribed inundation data for 2000–2020. Estimated annual CH4 emissions from northern (>60°N) wetlands averaged 10.0 ± 5.5 Tg CH4 yr−1. While summer CH4 emissions were well simulated compared to in‐situ flux measurement observations, the models underestimated CH4 during September to May relative to annual total (27 ± 9%, compared to 45% in observations) and substantially in the months with subzero air temperatures (5 ± 5%, compared to 27% in observations). Because of winter warming, nevertheless, the contribution of cold‐season emissions was simulated to increase at 0.4 ± 0.8% decade−1. Different parameterizations of processes, for example, freezing–thawing and snow insulation, caused conspicuous variability among models, implying the necessity of model refinement. Plain Language Summary Wetlands in the northern high latitudes are a major source of methane (CH4) to the atmosphere, mainly during the warm season. Previously, models have assumed that cold‐season CH4 emissions are low, but recent observations suggest high‐latitude wetlands can be substantial sources even in winter. We compared CH4 emissions simulated by 16 state‐of‐the‐art wetland models, participating in a model intercomparison project with a focus on the cold‐season in northern wetlands. The model simulations indicated that nearly one third of annual emissions were simulated to occur from September to May, and CH4 emissions to the atmosphere were not negligible even under freezing air temperatures, although the results differed greatly among the models. However, field studies suggest cold‐season emissions account for an even larger fraction of annual emissions. These results highlight the contribution of cold‐season emissions to the annual CH4 budget, which future climatic warming is expected to affect severely, and they also show that simulations of cold‐season CH4 emissions from wetlands need to be improved. Key Points Cold‐season methane (CH4) emissions simulated by 16 Global Carbon Project‐CH4 wetland models were analyzed Most models underestimate the cold‐season emissions in comparison with observational data Further model improvement by including cold‐season processes is required to reduce the model bias and uncertainty

Acidification of dust aerosols may increase aerosol iron (Fe) solubility, which is linked to mineral properties. Combustion aerosols can also elevate aerosol iron solubility when aerosol loading is low. Here, we use an atmospheric chemical transport model to investigate the deposition of filterable iron and its response to changes in anthropogenic emissions of both combustion aerosols and precursor gases. By introducing three classes of iron-containing minerals into the detailed aerosol chemistry model, we provide a theoretical examination of the effects of different dissolution behaviors on the acid mobilization of iron. Comparisons of modeled Fe dissolution curves with the measured dissolution rates for African, east Asian, and Australian dust samples show overall good agreement under acidic conditions. The improved treatment of Fe in mineral dust and its dissolution scheme results in reasonable predictive capability for iron solubility over the oceans in the Northern Hemisphere. Our model results suggest that the improvement of air quality projected in the future will lead to a decrease of the filterable iron deposition from iron-containing mineral dust to the eastern North Pacific due to less acidification in Asian dust, which is mainly associated with the reduction of nitrogen oxides (NOx) emissions. These results could have important implications for iron fertilization of phytoplankton growth, and highlight the necessity of improving the process-based quantitative understanding of the response of the chemical modification in iron-containing minerals to environmental changes.

Atmospheric processing of mineral aerosols by acid gases (e.g., SO2, HNO3, N2O5, and HCl) may play a key role in the transformation of insoluble iron (Fe in the oxidized or ferric (III) form) to soluble forms (e.g., Fe(II), inorganic soluble species of Fe(III), and organic complexes of iron). On the other hand, mineral dust particles have a potential of neutralizing the acidic species due to the alkaline buffer ability of carbonate minerals (e.g., CaCO3 and MgCO3). Here we demonstrate the impact of dust alkalinity on the acid mobilization of iron in a three-dimensional aerosol chemistry transport model that includes a mineral dissolution scheme. In our model simulations, most of the alkaline dust minerals cannot be entirely consumed by inorganic acids during the transport across the North Pacific Ocean. As a result, the inclusion of alkaline compounds in aqueous chemistry substantially limits the iron dissolution during the long-range transport to the North Pacific Ocean: only a small fraction of iron (<0.2%) dissolves from hematite in the coarse-mode dust aerosols with 0.45% soluble iron initially. On the other hand, a significant fraction of iron (1–2%) dissolves in the fine-mode dust aerosols due to the acid mobilization of the iron-containing minerals externally mixed with carbonate minerals. Consequently, the model quantitatively reproduces higher iron solubility in smaller particles as suggested by measurements over the Pacific Ocean. It implies that the buffering effect of alkaline content in dust aerosols might help to explain the inverse relationship between aerosol iron solubility and particle size. We also demonstrate that the iron solubility is sensitive to the chemical specification of iron-containing minerals in dust. Compared with the dust sources, soluble iron from combustion sources contributes to a relatively marginal effect for deposition of soluble iron over the North Pacific Ocean during springtime. Our results suggest that more comprehensive data for chemical specificity of iron-rich dust is needed to improve the predictive capability for size-segregated soluble iron particles.