Changes in the aerosol direct radiative forcing from 2001 to 2015: observational constraints and regional mechanisms

We present estimates of changes in the direct aerosol effects (DRE) and its anthropogenic component (DRF) from 2001 to 2015 using the GFDL chemistry–climate model AM3 driven by CMIP6 historical emissions. AM3 is evaluated against observed changes in the clear-sky shortwave direct aerosol effect (DREswclr) derived from the Clouds and the Earth's Radiant Energy System (CERES) over polluted regions. From 2001 to 2015, observations suggest that DREclrsw increases (i.e., less radiation is scattered to space by aerosols) over western Europe (0.7–1&thinsp;W&thinsp;m−2&thinsp;decade−1) and the eastern US (0.9–1.4&thinsp;W&thinsp;m−2&thinsp;decade−1), decreases over India (−1 to −1.6&thinsp;W&thinsp;m−2&thinsp;decade−1), and does not change significantly over eastern China. AM3 captures these observed regional changes in DREclrsw well in the US and western Europe, where they are dominated by the decline of sulfate aerosols, but not in Asia, where the model overestimates the decrease of DREclrsw. Over India, the model bias can be partly attributed to a decrease of the dust optical depth, which is not captured by our model and offsets some of the increase of anthropogenic aerosols. Over China, we find that the decline of SO2 emissions after 2007 is not represented in the CMIP6 emission inventory. Accounting for this decline, using the Modular Emission Inventory for China, and for the heterogeneous oxidation of SO2 significantly reduces the model bias. For both India and China, our simulations indicate that nitrate and black carbon contribute more to changes in DREclrsw than in the US and Europe. Indeed, our model suggests that black carbon (+0.12&thinsp;W&thinsp;m−2) dominates the relatively weak change in DRF from 2001 to 2015 (+0.03&thinsp;W&thinsp;m−2). Over this period, the changes in the forcing from nitrate and sulfate are both small and of the same magnitude (−0.03&thinsp;W&thinsp;m−2 each). This is in sharp contrast to the forcing from 1850 to 2001 in which forcings by sulfate and black carbon largely cancel each other out, with minor contributions from nitrate. The differences between these time periods can be well understood from changes in emissions alone for black carbon but not for nitrate and sulfate; this reflects non-linear changes in the photochemical production of nitrate and sulfate associated with changes in both the magnitude and spatial distribution of anthropogenic emissions.</p

Representing sub-grid scale variations in nitrogen deposition associated with land use in a global Earth system model: implications for present and future nitrogen deposition fluxes over North America

Reactive nitrogen (N) emissions have increased over the last 150 years as a result of greater fossil fuel combustion and food production. The resulting increase in N deposition can alter the function of ecosystems, but characterizing its ecological impacts remains challenging, in part because of uncertainties in model-based estimates of N dry deposition. Here, we use the Geophysical Fluid Dynamics Laboratory (GFDL) atmospheric chemistry–climate model (AM3) coupled with the GFDL land model (LM3) to estimate dry deposition velocities. We leverage the tiled structure of LM3 to represent the impact of physical, hydrological, and ecological heterogeneities on the surface removal of chemical tracers. We show that this framework can be used to estimate N deposition at more ecologically relevant scales (e.g., natural vegetation, water bodies) than from the coarse-resolution global model AM3. Focusing on North America, we show that the faster removal of N over forested ecosystems relative to cropland and pasture implies that coarse-resolution estimates of N deposition from global models systematically underestimate N deposition to natural vegetation by 10&thinsp;% to 30&thinsp;% in the central and eastern US. Neglecting the sub-grid scale heterogeneity of dry deposition velocities also results in an underestimate (overestimate) of the amount of reduced (oxidized) nitrogen deposited to water bodies. Overall, changes in land cover associated with human activities are found to slow down the removal of N from the atmosphere, causing a reduction in the dry oxidized, dry reduced, and total (wet+dry) N deposition over the contiguous US of 8&thinsp;%, 26&thinsp;%, and 6&thinsp;%, respectively. We also find that the reduction in the overall rate of removal of N associated with land-use change tends to increase N deposition on the remaining natural vegetation and facilitate N export to Canada. We show that sub-grid scale differences in the surface removal of oxidized and reduced nitrogen imply that projected near-term (2010–2050) changes in oxidized (−47&thinsp;%) and reduced (+40&thinsp;%) US N emissions will cause opposite changes in N deposition to water bodies (increase) and natural vegetation (decrease) in the eastern US, with potential implications for acidification and ecosystems.</p

Interannual variability in ozone removal by a temperate deciduous forest

The ozone (O3) dry depositional sink and its contribution to observed variability in tropospheric O3 are both poorly understood. Distinguishing O3 uptake through plant stomata versus other pathways is relevant for quantifying the O3 influence on carbon and water cycles. We use a decade of O3, carbon, and energy eddy covariance (EC) fluxes at Harvard Forest to investigate interannual variability (IAV) in O3 deposition velocities ( math formula). In each month, monthly mean math formula for the highest year is twice that for the lowest. Two independent stomatal conductance estimates, based on either water vapor EC or gross primary productivity, vary little from year to year relative to canopy conductance. We conclude that nonstomatal deposition controls the substantial observed IAV in summertime math formula during the 1990s over this deciduous forest. The absence of obvious relationships between meteorology and math formula implies a need for additional long-term, high-quality measurements and further investigation of nonstomatal mechanisms

Reactive intermediates revealed in secondary organic aerosol formation from isoprene

Isoprene is a significant source of atmospheric organic aerosol; however, the oxidation pathways that lead to secondary organic aerosol (SOA) have remained elusive. Here, we identify the role of two key reactive intermediates, epoxydiols of isoprene (IEPOX = β-IEPOX + δ-IEPOX) and methacryloylperoxynitrate (MPAN), which are formed during isoprene oxidation under low- and high-NO_x conditions, respectively. Isoprene low-NO_x SOA is enhanced in the presence of acidified sulfate seed aerosol (mass yield 28.6%) over that in the presence of neutral aerosol (mass yield 1.3%). Increased uptake of IEPOX by acid-catalyzed particle-phase reactions is shown to explain this enhancement. Under high-NO_x conditions, isoprene SOA formation occurs through oxidation of its second-generation product, MPAN. The similarity of the composition of SOA formed from the photooxidation of MPAN to that formed from isoprene and methacrolein demonstrates the role of MPAN in the formation of isoprene high-NO_x SOA. Reactions of IEPOX and MPAN in the presence of anthropogenic pollutants (i.e., acidic aerosol produced from the oxidation of SO_2 and NO_2, respectively) could be a substantial source of “missing urban SOA” not included in current atmospheric models

Hidden Symmetries and Dirac Fermions

In this paper, two things are done. First, we analyze the compatibility of Dirac fermions with the hidden duality symmetries which appear in the toroidal compactification of gravitational theories down to three spacetime dimensions. We show that the Pauli couplings to the p-forms can be adjusted, for all simple (split) groups, so that the fermions transform in a representation of the maximal compact subgroup of the duality group G in three dimensions. Second, we investigate how the Dirac fermions fit in the conjectured hidden overextended symmetry G++. We show compatibility with this symmetry up to the same level as in the pure bosonic case. We also investigate the BKL behaviour of the Einstein-Dirac-p-form systems and provide a group theoretical interpretation of the Belinskii-Khalatnikov result that the Dirac field removes chaos.Comment: 30 page

K(E10), Supergravity and Fermions

We study the fermionic extension of the E10/K(E10) coset model and its relation to eleven-dimensional supergravity. Finite-dimensional spinor representations of the compact subgroup K(E10) of E(10,R) are studied and the supergravity equations are rewritten using the resulting algebraic variables. The canonical bosonic and fermionic constraints are also analysed in this way, and the compatibility of supersymmetry with local K(E10) is investigated. We find that all structures involving A9 levels 0,1 and 2 nicely agree with expectations, and provide many non-trivial consistency checks of the existence of a supersymmetric extension of the E10/K(E10) coset model, as well as a new derivation of the `bosonic dictionary' between supergravity and coset variables. However, there are also definite discrepancies in some terms involving level 3, which suggest the need for an extension of the model to infinite-dimensional faithful representations of the fermionic degrees of freedom.Comment: 50 page

Atmospheric Peroxyacetyl Nitrate (PAN): A Global Budget and Source Attribution

Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) is the principal tropospheric reservoir for nitrogen oxide radicals $(NO_x = NO + NO_2)$. PAN enables the transport and release of $NO_x$ to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44% of the global source), methylglyoxal (30%), acetone (7%), and a suite of other isoprene and terpene oxidation products (19%). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37%) and alkanes (14%). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning $NO_x$ is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.Engineering and Applied Science

The topology of U-duality (sub-)groups

We discuss the topology of the symmetry groups appearing in compactified (super-)gravity, and discuss two applications. First, we demonstrate that for 3 dimensional sigma models on a symmetric space G/H with G non-compact and H the maximal compact subgroup of G, the possibility of oxidation to a higher dimensional theory can immediately be deduced from the topology of H. Second, by comparing the actual symmetry groups appearing in maximal supergravities with the subgroups of SL(32,R) and Spin(32), we argue that these groups cannot serve as a local symmetry group for M-theory in a formulation of de Wit-Nicolai type.Comment: 18 pages, LaTeX, 1 figure, 2 table

Sources of nitrogen deposition in Federal Class I areas in the US

It is desired to control excessive reactive nitrogen (Nr) deposition due to its detrimental impact on ecosystems. Using a three-dimensional atmospheric chemical transport model, GEOS-Chem, Nr deposition in the contiguous US and eight selected Class I areas (Voyageurs (VY), Smoky Mountain (SM), Shenandoah (SD), Big Bend (BB), Rocky Mountain (RM), Grand Teton (GT), Joshua Tree (JT), and Sequoia (SQ)) is investigated. First, modeled Nr deposition is compared with National Trends Network (NTN) and Clean Air Status and Trends Network (CASTNET) deposition values. The seasonality of measured species is generally well represented by the model (R2 &gt; 0.6), except in JT. While modeled Nr is generally within the range of seasonal observations, large overestimates are present in sites such as SM and SD in the spring and summer (up to 0.6 kg N ha month−1), likely owing to model high-biases in surface HNO3. The contribution of non-measured species (mostly dry deposition of NH3) to total modeled Nr deposition ranges from 1 to 55 %. The spatial distribution of the origin of Nr deposited in each Class I area and the contributions of individual emission sectors are estimated using the GEOS-Chem adjoint model. We find the largest role of long-range transport for VY, where 50 % (90 %) of annual Nr deposition originates within 670 (1670) km of the park. In contrast, the Nr emission footprint is most localized for SQ, where 50 % (90 %) of the deposition originates from within 130 (370) km. Emissions from California contribute to the Nr deposition in remote areas in the western US (RM, GT). Mobile NOx and livestock NH3 are found to be the major sources of Nr deposition in all sites except BB, where contributions of NOx from lightning and soils to natural levels of Nr deposition are significant (∼ 40 %). The efficiency in terms of Nr deposition per kg emissions of NH3-N, NOx-N, and SO2-S are also estimated. Unique seasonal features are found in JT (opposing efficiency distributions for winter and summer), RM (large fluctuations in the range of effective regions), and SD (upwind NH3 emissions hindering Nr deposition). We also evaluate the contributions of emissions to the total area of Class I regions in critical load exceedance, and to the total magnitude of exceedance. We find that while it is effective to control emissions in the western US to reduce the area of regions in CL exceedance, it can be more effective to control emissions in the eastern US to reduce the magnitude of Nr deposition above the CL. Finally, uncertainty in the nitrogen deposition caused by uncertainty in the NH3 emission inventory is explored by comparing results based on two different NH3 inventories; noticeable differences in the emission inventories and thus sensitivities of up to a factor of four found in individual locations

Influence of Dynamic Ozone Dry Deposition on Ozone Pollution

Identifying the contributions of chemistry and transport to observed ozone pollution using regional-to-global models relies on accurate representation of ozone dry deposition. We use a recently developed configuration of the NOAA GFDL chemistry-climate model - in which the atmosphere and land are coupled through dry deposition-to investigate the influence of ozone dry deposition on ozone pollution over northern midlatitudes. In our model, deposition pathways are tied to dynamic terrestrial processes, such as photosynthesis and water cycling through the canopy and soil. Small increases in winter deposition due to more process-based representation of snow and deposition to surfaces reduce hemispheric-scale ozone throughout the lower troposphere by 5-12 ppb, improving agreement with observations relative to a simulation with the standard configuration for ozone dry deposition. Declining snow cover by the end of the 21st-century tempers the previously identified influence of rising methane on winter ozone. Dynamic dry deposition changes summer surface ozone by -4 to +7 ppb. While previous studies emphasize the importance of uptake by plant stomata, new diagnostic tracking of depositional pathways reveals a widespread impact of nonstomatal deposition on ozone pollution. Daily variability in both stomatal and nonstomatal deposition contribute to daily variability in ozone pollution. Twenty-first century changes in summer deposition result from a balance among changes in individual pathways, reflecting differing responses to both high carbon dioxide (through plant physiology versus biomass accumulation) and water availability. Our findings highlight a need for constraints on the processes driving ozone dry deposition to test representation in regional-to-global models.Peer reviewe