It is well recognized that the atmospheric deposition of iron (Fe) affects ocean productivity, atmospheric CO2 uptake, ecosystem diversity, and overall climate. Despite significant advances in ...measurement techniques and modeling efforts, discrepancies persist between observations and models that hinder accurate predictions of processes and their global effects. Here, we provide an assessment report on where the current state of knowledge is and where future research emphasis would have the highest impact in furthering the field of Fe atmosphere-ocean biogeochemical cycle. These results were determined through consensus reached by diverse researchers from the oceanographic and atmospheric science communities with backgrounds in laboratory and in situ measurements, modeling, and remote sensing. We discuss i) novel measurement methodologies and instrumentation that allow detection and speciation of different forms and oxidation states of Fe in deliquesced mineral aerosol, cloud/rainwater, and seawater; ii) oceanic models that treat Fe cycling with several external sources and sinks, dissolved, colloidal, particulate, inorganic, and organic ligand-complexed forms of Fe, as well as Fe in detritus and phytoplankton; and iii) atmospheric models that consider natural and anthropogenic sources of Fe, mobilization of Fe in mineral aerosols due to the dissolution of Fe-oxides and Fe-substituted aluminosilicates through proton-promoted, organic ligand-promoted, and photo-reductive mechanisms. In addition, the study identifies existing challenges and disconnects (both fundamental and methodological) such as i) inconsistencies in Fe nomenclature and the definition of bioavailable Fe between oceanic and atmospheric disciplines, and ii) the lack of characterization of the processes controlling Fe speciation and residence time at the atmosphere-ocean interface. Such challenges are undoubtedly caused by extremely low concentrations, short lifetime, and the myriad of physical, (photo)chemical, and biological processes affecting global biogeochemical cycling of Fe. However, we also argue that the historical division (separate treatment of Fe biogeochemistry in oceanic and atmospheric disciplines) and the classical funding structures (that often create obstacles for transdisciplinary collaboration) are also hampering the advancement of knowledge in the field. Finally, the study provides some specific ideas and guidelines for laboratory studies, field measurements, and modeling research required for improved characterization of global biogeochemical cycling of Fe in relationship with other trace elements and essential nutrients. The report is intended to aid scientists in their work related to Fe biogeochemistry as well as program managers at the relevant funding agencies.
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•Unified nomenclature of the Fe-related terminology is proposed for atmospheric and oceanic communities.•A strategic science prioritization matrix is offered for conducting and facilitating new research.•Mechanistic treatments are needed for aerosol Fe interaction with atmospheric and oceanic DOM.
We describe the baseline model configuration and simulation characteristics of the Geophysical Fluid Dynamics Laboratory (GFDL)'s Atmosphere Model version 4.1 (AM4.1), which builds on developments at ...GFDL over 2013–2018 for coupled carbon‐chemistry‐climate simulation as part of the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL's AM4.0 development effort, which focused on physical and aerosol interactions and which is used as the atmospheric component of CM4.0, AM4.1 focuses on comprehensiveness of Earth system interactions. Key features of this model include doubled horizontal resolution of the atmosphere (~200 to ~100 km) with revised dynamics and physics from GFDL's previous‐generation AM3 atmospheric chemistry‐climate model. AM4.1 features improved representation of atmospheric chemical composition, including aerosol and aerosol precursor emissions, key land‐atmosphere interactions, comprehensive land‐atmosphere‐ocean cycling of dust and iron, and interactive ocean‐atmosphere cycling of reactive nitrogen. AM4.1 provides vast improvements in fidelity over AM3, captures most of AM4.0's baseline simulations characteristics, and notably improves on AM4.0 in the representation of aerosols over the Southern Ocean, India, and China—even with its interactive chemistry representation—and in its manifestation of sudden stratospheric warmings in the coldest months. Distributions of reactive nitrogen and sulfur species, carbon monoxide, and ozone are all substantially improved over AM3. Fidelity concerns include degradation of upper atmosphere equatorial winds and of aerosols in some regions.
Plain Language Summary
GFDL has developed a coupled chemistry‐climate Atmospheric Model (AM4.1) as part of its fourth‐generation coupled model development activities. AM4.1 includes comprehensive atmospheric chemistry for representing ozone and aerosols and has been developed for use in chemistry and air quality applications, including advanced land‐atmosphere‐ocean coupling. With fidelity near to that of AM4.0, AM4.1 features vastly improved representation of climate mean patterns and variability from previous GFDL atmospheric chemistry‐climate models.
Key Points
A new atmospheric chemistry‐climate model (AM4.1) has been developed for the Geophysical Fluid Dynamics Laboratory (GFDL)'s fourth‐generation model suite
AM4.1 includes an advanced dynamical core and physical parameterizations, with enhanced vertical resolution and revised aerosol and chemistry interactions
The AM4.1 model exhibits substantially enhanced fidelity compared to previous‐generation GFDL atmospheric models
Biomass burning is one of the largest sources of trace gases and aerosols to the atmosphere and has profound influence on tropospheric oxidants and radiative forcing. Using a fully coupled ...chemistry‐climate model (GFDL AM3), we find that co‐emission of trace gases and aerosol from present‐day biomass burning increases the global tropospheric ozone burden by 5.1% and decreases global mean OH by 6.3%. Gas and aerosol emissions combine to increase CH4 lifetime nonlinearly. Heterogeneous processes are shown to contribute partly to the observed lower ΔO3/ΔCO ratios in northern high latitudes versus tropical regions. The radiative forcing from biomass burning is shown to vary nonlinearly with biomass burning strength. At present‐day emission levels, biomass burning produces a net radiative forcing of −0.19 W/m2 (−0.29 from short‐lived species, mostly aerosol direct and indirect effects, +0.10 from CH4‐ and CH4‐induced changes in O3 and stratospheric H2O) but increases emissions to over 5 times present levels would result in a positive net forcing.
We implement a new isoprene oxidation mechanism in a global 3‐D chemical transport model (GEOS‐Chem). Model results are evaluated with observations for ozone, isoprene oxidation products, and related ...species from the International Consortium for Atmospheric Research on Transport and Transformation aircraft campaign over the eastern United States in summer 2004. The model achieves an unbiased simulation of ozone in the boundary layer and the free troposphere, reflecting canceling effects from recent model updates for isoprene chemistry, bromine chemistry, and HO2 loss to aerosols. Simulation of the ozone‐CO correlation is improved relative to previous versions of the model, and this is attributed to a lower and reversible yield of isoprene nitrates, increasing the ozone production efficiency per unit of nitrogen oxides (NOx ≡ NO + NO2). The model successfully reproduces the observed concentrations of organic nitrates (∑ANs) and their correlations with HCHO and ozone. ∑ANs in the model is principally composed of secondary isoprene nitrates, including a major contribution from nighttime isoprene oxidation. The correlations of ∑ANs with HCHO and ozone then provide sensitive tests of isoprene chemistry and argue in particular against a fast isomerization channel for isoprene peroxy radicals. ∑ANs can provide an important reservoir for exporting NOx from the U.S. boundary layer. We find that the dependence of surface ozone on isoprene emission is positive throughout the U.S., even if NOx emissions are reduced by a factor of 4. Previous models showed negative dependences that we attribute to erroneous titration of OH by isoprene.
Key Points
The model achieves an unbiased simulation of ozone over eastern US
The model reproduces ∑ANs and their correlations with HCHO and ozone
∑ANs can provide an important reservoir for exporting NOx
An approach for analysis and modeling of global atmospheric chemistry is developed for application to measurements that provide a tropospheric climatology of those heterogeneously distributed, ...reactive species that control the loss of methane and the production and loss of ozone. We identify key species (e.g., O3, NOx, HNO3, HNO4, C2H3NO5, H2O, HOOH, CH3OOH, HCHO, CO, CH4, C2H6, acetaldehyde, acetone) and presume that they can be measured simultaneously in air parcels on the scale of a few km horizontally and a few tenths of a km vertically. As a first step, six global models have prepared such climatologies sampled at the modeled resolution for August with emphasis on the vast central Pacific Ocean basin. Objectives of this paper are to identify and characterize differences in model-generated reactivities as well as species covariances that could readily be discriminated with an unbiased climatology. A primary tool is comparison of multidimensional probability densities of key species weighted by the mass of such parcels or frequency of occurrence as well as by the reactivity of the parcels with respect to methane and ozone. The reactivity-weighted probabilities tell us which parcels matter in this case, and this method shows skill in differentiating among the models' chemistry. Testing 100 km scale models with 2 km measurements using these tools also addresses a core question about model resolution and whether fine-scale atmospheric structures matter to the overall ozone and methane budget. A new method enabling these six global chemistry–climate models to ingest an externally sourced climatology and then compute air parcel reactivity is demonstrated. Such an objective climatology containing these key species is anticipated from the NASA Atmospheric Tomography (ATom) aircraft mission (2015–2020), executing profiles over the Pacific and Atlantic Ocean basins. This modeling study addresses a core part of the design of ATom.
Northern India (23–31° N, 68–90° E) is one of the most densely populated and polluted regions in world. Accurately modeling pollution in the region is difficult due to the extreme conditions with ...respect to emissions, meteorology, and topography, but it is paramount in order to understand how future changes in emissions and climate may alter the region's pollution regime. We evaluate the ability of a developmental version of the new-generation NOAA GFDL Atmospheric Model, version 4 (AM4) to simulate observed wintertime fine particulate matter (PM2.5) and its relationship to meteorology over Northern India. We compare two simulations of GFDL-AM4 nudged to observed meteorology for the period 1980–2016 driven by pollutant emissions from two global inventories developed in support of the Coupled Model Intercomparison Project Phases 5 (CMIP5) and 6 (CMIP6), and compare results with ground-based observations from India's Central Pollution Control Board (CPCB) for the period 1 October 2015–31 March 2016. Overall, our results indicate that the simulation with CMIP6 emissions produces improved concentrations of pollutants over the region relative to the CMIP5-driven simulation. While the particulate concentrations simulated by AM4 are biased low overall, the model generally simulates the magnitude and daily variability of observed total PM2.5. Nitrate and organic matter are the primary components of PM2.5 over Northern India in the model. On the basis of correlations of the individual model components with total observed PM2.5 and correlations between the two simulations, meteorology is the primary driver of daily variability. The model correctly reproduces the shape and magnitude of the seasonal cycle of PM2.5, but the simulated diurnal cycle misses the early evening rise and secondary maximum found in the observations. Observed PM2.5 abundances are by far the highest within the densely populated Indo-Gangetic Plain, where they are closely related to boundary layer meteorology, specifically relative humidity, wind speed, boundary layer height, and inversion strength. The GFDL AM4 model reproduces the overall observed pollution gradient over Northern India as well as the strength of the meteorology–PM2.5 relationship in most locations.
The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean ...tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (Tau CH4) between these models. Annual average Tau CH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in Tau CH4 (Delta Tau CH4) result from variations in chemical mechanisms (Delta Tau CH4 = 0.46 years), the photolysis frequency (J) of O3 yields O(D-1) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The Delta Tau CH4 due to CTM differences in NO(x) (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NO(x). Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.
A comparison of a model using five widely known mechanisms (RACM, CB05, LaRC, SAPRC-99, SAPRC-07, and MCMv3.1) has been conducted based on the TexAQS II Radical and Aerosol Measurement Project ...(TRAMP-2006) field data in 2006. The concentrations of hydroxyl (OH) and hydroperoxy (HO
2) radicals were calculated by a zero-dimensional box model with each mechanism and then compared with the OH and HO
2 measurements. The OH and HO
2 calculated by the model with different mechanisms show similarities and differences with each other and with the measurements. First, measured OH and HO
2 are generally greater than modeled for all mechanisms, with the median modeled-to-measured ratios ranging from about 0.8 (CB05) to about 0.6 (SAPRC-99). These differences indicate that either measurement errors, the effects of unmeasured species or chemistry errors in the model or the mechanisms, with some errors being independent of the mechanism used. Second, the modeled and measured ratios of HO
2/OH agree when NO is about 1 ppbv, but the modeled ratio is too high when NO was less and too low when NO is more, as seen in previous studies. Third, mechanism–mechanism HO
x
differences are sensitive to the environmental conditions – in more polluted conditions, the mechanism–mechanism differences are less. This result suggests that, in polluted conditions, the mechanistic details are less important than in cleaner conditions, probably because of the dominance of reactive nitrogen chemistry under polluted conditions.
OH and HO2 were measured with the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS) as part of a large measurement suite from the NASA DC‐8 aircraft during the Intercontinental Chemical Transport ...Experiment‐A (INTEX‐A). This mission, which was conducted mainly over North America and the western Atlantic Ocean in summer 2004, was an excellent test of atmospheric oxidation chemistry. The HOx results from INTEX‐A are compared to those from previous campaigns and to results for other related measurements from INTEX‐A. Throughout the troposphere, observed OH was generally 0.95 of modeled OH; below 8 km, observed HO2 was generally 1.20 of modeled HO2. This observed‐to‐modeled comparison is similar to that for TRACE‐P, another midlatitude study for which the median observed‐to‐modeled ratio was 1.08 for OH and 1.34 for HO2, and to that for PEM‐TB, a tropical study for which the median observed‐to‐modeled ratio was 1.17 for OH and 0.97 for HO2. HO2 behavior above 8 km was markedly different. The observed‐to‐modeled HO2 ratio increased from ∼1.2 at 8 km to ∼3 at 11 km with the observed‐to‐modeled ratio correlating with NO. Above 8 km, the observed‐to‐modeled HO2 and observed NO were both considerably greater than observations from previous campaigns. In addition, the observed‐to‐modeled HO2/OH, which is sensitive to cycling reactions between OH and HO2, increased from ∼1.5 at 8 km to almost 3.5 at 11 km. These discrepancies suggest a large unknown HOx source and additional reactants that cycle HOx from OH to HO2. In the continental planetary boundary layer, the observed‐to‐modeled OH ratio increased from 1 when isoprene was less than 0.1 ppbv to over 4 when isoprene was greater than 2 ppbv, suggesting that forests throughout the United States are emitting unknown HOx sources. Progress in resolving these discrepancies requires a focused research activity devoted to further examination of possible unknown OH sinks and HOx sources.
We describe and evaluate atmospheric chemistry in the newly developed Geophysical Fluid Dynamics Laboratory chemistry‐climate model (GFDL AM3) and apply it to investigate the net impact of ...preindustrial (PI) to present (PD) changes in short‐lived pollutant emissions (ozone precursors, sulfur dioxide, and carbonaceous aerosols) and methane concentration on atmospheric composition and climate forcing. The inclusion of online troposphere‐stratosphere interactions, gas‐aerosol chemistry, and aerosol‐cloud interactions (including direct and indirect aerosol radiative effects) in AM3 enables a more complete representation of interactions among short‐lived species, and thus their net climate impact, than was considered in previous climate assessments. The base AM3 simulation, driven with observed sea surface temperature (SST) and sea ice cover (SIC) over the period 1981–2007, generally reproduces the observed mean magnitude, spatial distribution, and seasonal cycle of tropospheric ozone and carbon monoxide. The global mean aerosol optical depth in our base simulation is within 5% of satellite measurements over the 1982–2006 time period. We conduct a pair of simulations in which only the short‐lived pollutant emissions and methane concentrations are changed from PI (1860) to PD (2000) levels (i.e., SST, SIC, greenhouse gases, and ozone‐depleting substances are held at PD levels). From the PI to PD, we find that changes in short‐lived pollutant emissions and methane have caused the tropospheric ozone burden to increase by 39% and the global burdens of sulfate, black carbon, and organic carbon to increase by factors of 3, 2.4, and 1.4, respectively. Tropospheric hydroxyl concentration decreases by 7%, showing that increases in OH sinks (methane, carbon monoxide, nonmethane volatile organic compounds, and sulfur dioxide) dominate over sources (ozone and nitrogen oxides) in the model. Combined changes in tropospheric ozone and aerosols cause a net negative top‐of‐the‐atmosphere radiative forcing perturbation (−1.05 W m−2) indicating that the negative forcing (direct plus indirect) from aerosol changes dominates over the positive forcing due to ozone increases, thus masking nearly half of the PI to PD positive forcing from long‐lived greenhouse gases globally, consistent with other current generation chemistry‐climate models.
Key Points
Document and evaluate atmospheric chemistry in GFDL‐AM3
Net forcing from PI to PD short‐lived pollutant emission changes is ‐1.05 Wm‐2
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