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On I(5577 Å) and I (7620 Å) auroral emissions and atomic oxygen densities

A model of auroral electron deposition processes has been developed using Monte Carlo techniques to simulate electron transport and energy loss. The computed differential electron flux and pitch angle were compared with in situ auroral observations to provide a check on the accuracy of the model. As part of the energy loss process, a tally was kept of electronic excitation and ionization of the important atomic and molecular states. The optical emission rates from these excited states were computed and compared with auroral observations of η(3914 Å), η(5577 Å), η(7620 Å) and η(N2VK). In particular, the roles played by energy transfer from N2(A3Σ+u) and by other processes in the excitation of O(1S) and O2(b1Σ+g) were investigated in detail. It is concluded that the N2(A3Σ+u) mechanism is dominant for the production of OI(5577 Å) in the peak emission region of normal aurora, although the production efficiency is much smaller than the measured laboratory value; above 150 km electron impact on atomic oxygen is dominant. Atomic oxygen densities in the range of 0.75±0.25 MSIS-86 [O] were derived from the optical comparisons for auroral latitudes in mid-winter for various levels of solar and magnetic activity.
Diagnosis of cirrus cloud occurrence using large-scale analysis data and a cloud-scale model

The development of cirrus clouds is governed by large-scale synoptic movements such as updraft regions in convergence zones, but also by smaller scale features, for instance microphysical phenomena, entrainment, small-scale turbulence and radiative field, fall-out of the ice phase or wind shear. For this reason, the proper handling of cirrus life cycles is not an easy task using a large-scale model alone. We present some results from a small-scale cirrus cloud model initialized by ECMWF first-guess data, which prove more convenient for this task than the analyzed ones. This model is Starr's 2-D cirrus cloud model, where the rate of ice production/destruction is parametrized from environmental data. Comparison with satellite and local observations during the ICE89 experiment (North Sea) shows that such an efficient model using large-scale data as input provides a reasonable diagnosis of cirrus occurrence in a given meteorological field. The main driving features are the updraft provided by the large-scale model, which enhances or inhibits the cloud development according to its sign, and the water vapour availability. The cloud fields retrieved are compared to satellite imagery. Finally, the use of a small-scale model in large-scale numerical studies is examined.
Analysis of laminated structure in ozone vertical profiles in central Europe

Using statistical techniques, we study the relationship between the long-term changes in the laminar structure of the ozone vertical profile at two central-European stations - Hohenpeissenberg and Lindenberg - and other quantities potentially affecting the state of the lower stratosphere, and total-ozone content. We consider only positive laminae greater than 30 nbar. Laminae contribute non-negligibly to total ozone, and this contribution varies strongly with season. The maximum laminae-occurrence frequency in late winter/early spring is five-times higher than the minimum in early autumn. The main result of the paper is the discovery of a strong negative trend in the frequency of laminae occurrence, about –15% per decade, and even a slightly stronger negative trend in ozone content in laminae. Strong negative trends in laminae occurrence imply negative changes in total ozone as well. No pronounced effect of the quasi-biennial oscillation and solar cycle on laminae was found, whereas the 100-hPa temperature had a clear effect, and there was an indication of substantial effects of volcanic eruptions and El Niño southern oscillation events. Long-term changes in individual time series of meteorological parameters measured over Hohenpeissenberg do not indicate their significant role in the observed trend in laminae occurrence. On the other hand, there is some increase in the occurrence of very zonal circulation patterns, as well as slight decrease in very meridional circulation patterns. Together with other indications this allows us to say that dynamical effects are expected to be a principal contributor. Thus changes in laminae occurrence will probably be able to serve as an indicator/tracer of long-term changes in lower-stratospheric dynamics.
Disturbed vertical E×B plasma drifts in the equatorial F2 region at solar minimum deduced from observed NmF2 and hmF2 variations

Ground-based ionosonde and magnetic-field observations on the equatorial station Huancayo, ESRO4 neutral-composition measurements, and theoretical model calculations were used to analyze disturbed E×B vertical plasma drift during the phase of solar minimum in 1973. Vertical drifts calculated for disturbed days do not show the systematic decrease often mentioned in publications, and demonstrate strong dependence on IMF-Bz changes. It is confirmed with the help of our drift calculations that Bz turnings to a northward direction result in a decrease (up to reversal) of normal Sq (eastward during daytime and westward at nighttime) in the zonal component of electric field. Southward Bz excursions enhance normal Ey both in daytime and nighttime hours. Model predictions of Ey's reaction to IMF-Bz changes are discussed.
Equatorial ionospheric response to the 10.7 cm radio flux over two sunspot cycles (1969−1991)

It is evident that fluctuations in a standard ionospheric parameter, the minimum (virtual) height (h´F) of the equatorial F-region in the African (Ouagadougou), Asian (Manila) and American (Huancayo) longitudinal sectors, closely resemble changes in solar activity as deduced from the 10.7 cm solar flux index (S), over two solar cycles (1969–91). The monthly median hourly value of h´F, particularly in the post-sunset period (18–20 LT), are positively correlated with the monthly average S. The value of h´F can be deduced from an empirical formula: h´F=0.68S+218.3, with the correlation coefficient (r) between h´F and S being 0.78. The diurnal distribution of r during daytime (06–14 LT) was radically different for the African and Asian longitudinal sectors during 1980-1991, with the most pronounced difference in the post-noon period (12–14 LT) when the correlation coefficients r for the Asian and African sectors are 0.8 and 0.2, respectively. Thus, the daytime F-region in the African sector responded far less to changes in solar activity than the Asian F-region during this cycle. This longitudinal anomaly was however absent in the preceding cycle (1969–1979) when the African and Asian sectors were both characterised by low daytime and pronounced post-sunset correlation coefficient r. The American sector appears to have a high correlation coefficient r in daytime increasing to a small maximum in the post-sunset interval. The post-sunset enhancement in r is a characteristic feature for equatorial stations only (corrected geomagnetic latitude <10°).
Estimation of fossil-fuel CO2 emissions using satellite measurements of "proxy" species

Fossil-fuel (FF) burning releases carbon dioxide (CO2) together with many other chemical species, some of which, such as nitrogen dioxide (NO2) and carbon monoxide (CO), are routinely monitored from space. This study examines the feasibility of estimation of FF CO2 emissions from large industrial regions by using NO2 and CO column retrievals from satellite measurements in combination with simulations by a mesoscale chemistry transport model (CTM). To this end, an inverse modeling method is developed that allows estimating FF CO2 emissions from different sectors of the economy, as well as the total CO2 emissions, in a given region. The key steps of the method are (1) inferring "top-down" estimates of the regional budget of anthropogenic NOx and CO emissions from satellite measurements of proxy species (NO2 and CO in the case considered) without using formal a priori constraints on these budgets, (2) the application of emission factors (the NOx-to-CO2 and CO-to-CO2 emission ratios in each sector) that relate FF CO2 emissions to the proxy species emissions and are evaluated by using data of "bottom-up" emission inventories, and (3) cross-validation and optimal combination of the estimates of CO2 emission budgets derived from measurements of the different proxy species. Uncertainties in the top-down estimates of the NOx and CO emissions are evaluated and systematic differences between the measured and simulated data are taken into account by using original robust techniques validated with synthetic data. To examine the potential of the method, it was applied to the budget of emissions for a western European region including 12 countries by using NO2 and CO column amounts retrieved from, respectively, the OMI and IASI satellite measurements and simulated by the CHIMERE mesoscale CTM, along with the emission conversion factors based on the EDGAR v4.2 emission inventory. The analysis was focused on evaluation of the uncertainty levels for the top-down NOx and CO emission estimates and "hybrid" estimates (that is, those based on both atmospheric measurements of a given proxy species and respective bottom-up emission inventory data) of FF CO2 emissions, as well as on examining consistency between the FF NO2 emission estimates derived from measurements of the different proxy species. It is found that NO2 measurements can provide much stronger constraints to the total annual FF CO2 emissions in the study region than CO measurements, the accuracy of the NO2-measurement-based CO2 emission estimate being mostly limited by the uncertainty in the top-down NOx emission estimate. Nonetheless, CO measurements are also found to be useful as they provide additional constraints to CO2 emissions and enable evaluation of the hybrid FF CO2 emission estimates obtained from NO2 measurements. Our most reliable estimate for the total annual FF CO2 emissions in the study region in 2008 (2.71 ± 0.30 Pg CO2) is found to be about 11 and 5 % lower than the respective estimates based on the EDGAR v.4.2 (3.03 Pg CO2) and CDIAC (2.86 Pg CO2) emission inventories, with the difference between our estimate and the CDIAC inventory data not being statistically significant. In general, the results of this study indicate that the proposed method has the potential to become a useful tool for identification of possible biases and/or inconsistencies in the bottom-up emission inventory data regarding CO2, NOx, and CO emissions from fossil-fuel burning in different regions of the world.
Why do models overestimate surface ozone in the Southeast United States?

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NOx  ≡  NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC4RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25°  ×  0.3125° horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NOx from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC4RS observations of NOx and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NOx emissions from mobile and industrial sources must be reduced by 30–60 %, dependent on the assumption of the contribution by soil NOx emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NOx emissions. We find that only half of isoprene oxidation proceeds by the high-NOx pathway to produce ozone; this fraction is only moderately sensitive to changes in NOx emissions because isoprene and NOx emissions are spatially segregated. GEOS-Chem with reduced NOx emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NOx oxidation products. However, the model is still biased high by 6 ± 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.
Global and regional radiative forcing from 20 % reductions in BC, OC and SO4 – an HTAP2 multi-model study

In the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise, a range of global atmospheric general circulation and chemical transport models performed coordinated perturbation experiments with 20 % reductions in emissions of anthropogenic aerosols, or aerosol precursors, in a number of source regions. Here, we compare the resulting changes in the atmospheric load and vertically resolved profiles of black carbon (BC), organic aerosols (OA) and sulfate (SO4) from 10 models that include treatment of aerosols. We use a set of temporally, horizontally and vertically resolved profiles of aerosol forcing efficiency (AFE) to estimate the impact of emission changes in six major source regions on global radiative forcing (RF) pertaining to the direct aerosol effect, finding values between. 51.9 and 210.8 mW m−2 Tg−1 for BC, between −2.4 and −17.9 mW m−2 Tg−1 for OA and between −3.6 and −10.3 W m−2 Tg−1 for SO4. In most cases, the local influence dominates, but results show that mitigations in south and east Asia have substantial impacts on the radiative budget in all investigated receptor regions, especially for BC. In Russia and the Middle East, more than 80 % of the forcing for BC and OA is due to extra-regional emission reductions. Similarly, for North America, BC emissions control in east Asia is found to be more important than domestic mitigations, which is consistent with previous findings. Comparing fully resolved RF calculations to RF estimates based on vertically averaged AFE profiles allows us to quantify the importance of vertical resolution to RF estimates. We find that locally in the source regions, a 20 % emission reduction strengthens the radiative forcing associated with SO4 by 25 % when including the vertical dimension, as the AFE for SO4 is strongest near the surface. Conversely, the local RF from BC weakens by 37 % since BC AFE is low close to the ground. The fraction of BC direct effect forcing attributable to intercontinental transport, on the other hand, is enhanced by one-third when accounting for the vertical aspect, because long-range transport primarily leads to aerosol changes at high altitudes, where the BC AFE is strong. While the surface temperature response may vary with the altitude of aerosol change, the analysis in the present study is not extended to estimates of temperature or precipitation changes.
Effects of urban agglomeration on surface-UV doses: a comparison of Brewer measurements in Warsaw and Belsk, Poland, for the period 2013–2015

Specific aerosols and cloud properties over large urban regions seem to generate an island, similar to the well-known urban heat island, leading to lower ultraviolet (UV) radiation intensity compared to the surrounding less polluted areas, thus creating a shield against excessive human exposure to UV radiation. The present study focuses on differences between erythemal and UVA (324 nm) doses measured by the Brewer spectrophotometers in Warsaw (52.3° N, 21.0° E) and Belsk (51.8° N, 20.8° E). The latter is a rural region located about 60 km south-west of the city. Ratios between erythemal and UVA partly daily doses, obtained during all-sky and cloudless-sky conditions for the period May 2013–December 2015, were analysed to infer a specific cloud and aerosol forcing on the surface UV doses over Warsaw. Radiative model simulations were carried out to find sources of the observed differences between the sites. It was found that Warsaw urban agglomeration induced 8 and 6 % attenuation of the erythemal and UVA doses respectively. This is mostly due to the lower sun elevation in Warsaw during the near-noon measurements and the larger optical depth of the city aerosols and increased cloudiness. It could be hypothesised that the expected stronger absorption of the solar UV radiation by urban aerosols is compensated for here by a higher surface reflectivity over the city.
Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD

New particle formation driven by acid–base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10–30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid–base pairs in particles as small as 10 nm.