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Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.
Multi-satellite sensor study on precipitation-induced emission pulses of NOx from soils in semi-arid ecosystems

We present a top-down approach to infer and quantify rain-induced emission pulses of NOx ( ≡  NO + NO2), stemming from biotic emissions of NO from soils, from satellite-borne measurements of NO2. This is achieved by synchronizing time series at single grid pixels according to the first day of rain after a dry spell of prescribed duration. The full track of the temporal evolution several weeks before and after a rain pulse is retained with daily resolution. These are needed for a sophisticated background correction, which accounts for seasonal variations in the time series and allows for improved quantification of rain-induced soil emissions. The method is applied globally and provides constraints on pulsed soil emissions of NOx in regions where the NOx budget is seasonally dominated by soil emissions. We find strong peaks of enhanced NO2 vertical column densities (VCDs) induced by the first intense precipitation after prolonged droughts in many semi-arid regions of the world, in particular in the Sahel. Detailed investigations show that the rain-induced NO2 pulse detected by the OMI (Ozone Monitoring Instrument), GOME-2 and SCIAMACHY satellite instruments could not be explained by other sources, such as biomass burning or lightning, or by retrieval artefacts (e.g. due to clouds). For the Sahel region, absolute enhancements of the NO2 VCDs on the first day of rain based on OMI measurements 2007–2010 are on average 4 × 1014  molec cm−2 and exceed 1 × 1015  molec cm−2 for individual grid cells. Assuming a NOx lifetime of 4 h, this corresponds to soil NOx emissions in the range of 6 up to 65 ng N m−2 s−1, which is in good agreement with literature values. Apart from the clear first-day peak, NO2 VCDs are moderately enhanced (2 × 1014  molec cm−2) compared to the background over the following 2 weeks, suggesting potential further emissions during that period of about 3.3 ng N m−2 s−1. The pulsed emissions contribute about 21–44 % to total soil NOx emissions over the Sahel.
Conditions for super-adiabatic droplet growth after entrainment mixing

Cloud droplet response to entrainment and mixing between a cloud and its environment is considered, accounting for subsequent droplet growth during adiabatic ascent following a mixing event. The vertical profile for liquid water mixing ratio after a mixing event is derived analytically, allowing the reduction to be predicted from the mixing fraction and from the temperature and humidity for both the cloud and environment. It is derived for the limit of homogeneous mixing. The expression leads to a critical height above the mixing level: at the critical height the cloud droplet radius is the same for both mixed and unmixed parcels, and the critical height is independent of the updraft velocity and mixing fraction. Cloud droplets in a mixed parcel are larger than in an unmixed parcel above the critical height, which we refer to as the “super-adiabatic” growth region. Analytical results are confirmed with a bin microphysics cloud model. Using the model, we explore the effects of updraft velocity, aerosol source in the environmental air, and polydisperse cloud droplets. Results show that the mixed parcel is more likely to reach the super-adiabatic growth region when the environmental air is humid and clean. It is also confirmed that the analytical predictions are matched by the volume-mean cloud droplet radius for polydisperse size distributions. The findings have implications for the origin of large cloud droplets that may contribute to onset of collision–coalescence in warm clouds.
Spectroscopic evidence of large aspherical β-NAT particles involved in denitrification in the December 2011 Arctic stratosphere

We analyze polar stratospheric cloud (PSC) signatures in airborne MIPAS-STR (Michelson Interferometer for Passive Atmospheric Sounding – STRatospheric aircraft) observations in the spectral regions from 725 to 990 and 1150 to 1350 cm−1 under conditions suitable for the existence of nitric acid trihydrate (NAT) above northern Scandinavia on 11 December 2011. The high-resolution infrared limb emission spectra of MIPAS-STR show a characteristic “shoulder-like” signature in the spectral region around 820 cm−1, which is attributed to the ν2 symmetric deformation mode of NO3− in β-NAT. Using radiative transfer calculations involving Mie and T-Matrix methods, the spectral signatures of spherical and aspherical particles are simulated. The simulations are constrained using collocated in situ particle measurements. Simulations assuming highly aspherical spheroids with aspect ratios (AR) of 0.1 or 10.0 and a lognormal particle mode with a mode radius of 4.8 µm reproduce the observed spectra to a high degree. A smaller lognormal mode with a mode radius of 2.0 µm, which is also taken into account, plays only a minor role. Within the scenarios analyzed, the best overall agreement is found for elongated spheroids with AR = 0.1. Simulations of spherical particles and spheroids with AR  =  0.5 and 2.0 return results very similar to each other and do not allow us to reproduce the signature around 820 cm−1. The observed “shoulder-like” signature is explained by the combination of the absorption/emission and scattering characteristics of large highly aspherical β-NAT particles. The size distribution supported by our results corresponds to ∼ 9 ppbv of gas-phase equivalent HNO3 at the flight altitude of ∼ 18.5 km. The results are compared with the size distributions derived from the in situ observations, a corresponding Chemical Lagrangian Model of the Stratosphere (CLaMS) simulation, and excess gas-phase HNO3 observed in a nitrification layer directly below the observed PSC. The presented results suggest that large highly aspherical β-NAT particles involved in denitrification of the polar stratosphere can be identified by means of passive infrared limb emission measurements.
Co-benefits of global and regional greenhouse gas mitigation for US air quality in 2050

Policies to mitigate greenhouse gas (GHG) emissions will not only slow climate change but can also have ancillary benefits of improved air quality. Here we examine the co-benefits of both global and regional GHG mitigation for US air quality in 2050 at fine resolution, using dynamical downscaling methods, building on a previous global co-benefits study (West et al., 2013). The co-benefits for US air quality are quantified via two mechanisms: through reductions in co-emitted air pollutants from the same sources and by slowing climate change and its influence on air quality, following West et al. (2013). Additionally, we separate the total co-benefits into contributions from domestic GHG mitigation vs. mitigation in foreign countries. We use the Weather Research and Forecasting (WRF) model to dynamically downscale future global climate to the regional scale and the Sparse Matrix Operator Kernel Emissions (SMOKE) program to directly process global anthropogenic emissions to the regional domain, and we provide dynamical boundary conditions from global simulations to the regional Community Multi-scale Air Quality (CMAQ) model. The total co-benefits of global GHG mitigation from the RCP4.5 scenario compared with its reference are estimated to be higher in the eastern US (ranging from 0.6 to 1.0 µg m−3) than the west (0–0.4 µg m−3) for fine particulate matter (PM2.5), with an average of 0.47 µg m−3 over the US; for O3, the total co-benefits are more uniform at 2–5 ppb, with a US average of 3.55 ppb. Comparing the two mechanisms of co-benefits, we find that reductions in co-emitted air pollutants have a much greater influence on both PM2.5 (96 % of the total co-benefits) and O3 (89 % of the total) than the second co-benefits mechanism via slowing climate change, consistent with West et al. (2013). GHG mitigation from foreign countries contributes more to the US O3 reduction (76 % of the total) than that from domestic GHG mitigation only (24 %), highlighting the importance of global methane reductions and the intercontinental transport of air pollutants. For PM2.5, the benefits of domestic GHG control are greater (74 % of total). Since foreign contributions to co-benefits can be substantial, with foreign O3 benefits much larger than those from domestic reductions, previous studies that focus on local or regional co-benefits may greatly underestimate the total co-benefits of global GHG reductions. We conclude that the US can gain significantly greater domestic air quality co-benefits by engaging with other nations to control GHGs.
Trends in normalized difference vegetation index (NDVI) associated with urban development in northern West Siberia

Exploration and exploitation of oil and gas reserves of northern West Siberia has promoted rapid industrialization and urban development in the region. This development leaves significant footprints on the sensitive northern environment, which is already stressed by the global warming. This study reports the region-wide changes in the vegetation cover as well as the corresponding changes in and around 28 selected urbanized areas. The study utilizes the normalized difference vegetation index (NDVI) from high-resolution (250 m) MODIS data acquired for summer months (June through August) over 15 years (2000–2014). The results reveal the increase of NDVI (or “greening”) over the northern (tundra and tundra-forest) part of the region. Simultaneously, the southern, forested part shows the widespread decrease of NDVI (or “browning”). These region-wide patterns are, however, highly fragmented. The statistically significant NDVI trends occupy only a small fraction of the region. Urbanization destroys the vegetation cover within the developed areas and at about 5–10 km distance around them. The studied urbanized areas have the NDVI values by 15 to 45 % lower than the corresponding areas at 20–40 km distance. The largest NDVI reduction is typical for the newly developed areas, whereas the older areas show recovery of the vegetation cover. The study reveals a robust indication of the accelerated greening near the older urban areas. Many Siberian cities become greener even against the wider browning trends at their background. Literature discussion suggests that the observed urban greening could be associated not only with special tending of the within-city green areas but also with the urban heat islands and succession of more productive shrub and tree species growing on warmer sandy soils.
Impact of crop field burning and mountains on heavy haze in the North China Plain: a case study

With the provincial statistical data and crop field burning (CFB) activities captured by Moderate Resolution Imaging Spectroradiometer (MODIS), we extracted a detailed CFB emission inventory in the North China Plain (NCP). The WRF-CHEM model was applied to investigate the impact of CFB on air pollution during the period from 6 to 12 October 2014, corresponding to a heavy haze incident with high concentrations of PM2.5 (particulate matter with aerodynamic diameter less than 2.5 µm). The WRF-CHEM model generally performed well in simulating the surface species concentrations of PM2.5, O3 and NO2 compared to the observations; in addition, it reasonably reproduced the observed temporal variations of wind speed, wind direction and planetary boundary layer height (PBLH). It was found that the CFB that occurred in southern NCP (SNCP) had a significant effect on PM2.5 concentrations locally, causing a maximum of 34 % PM2.5 increase. Under continuous southerly wind conditions, the CFB pollution plume went through a long-range transport to northern NCP (NNCP; with several mega cities, including Beijing, the capital city of China), where few CFBs occurred, resulting in a maximum of 32 % PM2.5 increase. As a result, the heavy haze in Beijing was enhanced by the CFB, which occurred in SNCP. Mountains also play significant roles in enhancing the PM2.5 pollution in NNCP through the blocking effect. The mountains blocked and redirected the airflows, causing the pollutant accumulations along the foothills of mountains. This study suggests that the prohibition of CFB should be strict not only in or around Beijing, but also on the ulterior crop growth areas of SNCP. PM2.5 emissions in SNCP should be significantly limited in order to reduce the occurrences of heavy haze events in the NNCP region.
Hydroxyl radical in/on illuminated polar snow: formation rates, lifetimes, and steady-state concentrations

While the hydroxyl radical (<mo>•</mo>OH) in the snowpack is likely a dominant oxidant for organic species and bromide, little is known about the kinetics or steady-state concentrations of <mo>•</mo>OH on/in snow and ice. Here we measure the formation rate, lifetime, and concentration of <mo>•</mo>OH for illuminated polar snow samples studied in the laboratory and in the field. Laboratory studies show that <mo>•</mo>OH kinetics and steady-state concentrations are essentially the same for a given sample studied as ice and liquid; this is in contrast to other photooxidants, which show a concentration enhancement in ice relative to solution as a result of kinetic differences in the two phases. The average production rate of <mo>•</mo>OH in samples studied at Summit, Greenland, is 5 times lower than the average measured in the laboratory, while the average <mo>•</mo>OH lifetime determined in the field is 5 times higher than in the laboratory. These differences indicate that the polar snows we studied in the laboratory are affected by contamination, despite significant efforts to prevent this; our results suggest similar contamination may be a widespread problem in laboratory studies of ice chemistry. Steady-state concentrations of <mo>•</mo>OH in clean snow studied in the field at Summit, Greenland, range from (0.8 to 3) × 10−15 M, comparable to values reported for midlatitude cloud and fog drops, rain, and deliquesced marine particles, even though impurity concentrations in the snow samples are much lower. Partitioning of firn air <mo>•</mo>OH to the snow grains will approximately double the steady-state concentration of snow-grain hydroxyl radical, leading to an average [<mo>•</mo>OH] in near-surface, summer Summit snow of approximately 4 × 10−15 M. At this concentration, the <mo>•</mo>OH-mediated lifetimes of organics and bromide in Summit snow grains are approximately 3 days and 7 h, respectively, suggesting that hydroxyl radical is a major oxidant for both species.
Variation in global chemical composition of PM2.5: emerging results from SPARTAN

The Surface PARTiculate mAtter Network (SPARTAN) is a long-term project that includes characterization of chemical and physical attributes of aerosols from filter samples collected worldwide. This paper discusses the ongoing efforts of SPARTAN to define and quantify major ions and trace metals found in fine particulate matter (PM2.5). Our methods infer the spatial and temporal variability of PM2.5 in a cost-effective manner. Gravimetrically weighed filters represent multi-day averages of PM2.5, with a collocated nephelometer sampling air continuously. SPARTAN instruments are paired with AErosol RObotic NETwork (AERONET) sun photometers to better understand the relationship between ground-level PM2.5 and columnar aerosol optical depth (AOD). We have examined the chemical composition of PM2.5 at 12 globally dispersed, densely populated urban locations and a site at Mammoth Cave (US) National Park used as a background comparison. So far, each SPARTAN location has been active between the years 2013 and 2016 over periods of 2–26 months, with an average period of 12 months per site. These sites have collectively gathered over 10 years of quality aerosol data. The major PM2.5 constituents across all sites (relative contribution ± SD) are ammoniated sulfate (20 % ± 11 %), crustal material (13.4 % ± 9.9 %), equivalent black carbon (11.9 % ± 8.4 %), ammonium nitrate (4.7 % ± 3.0 %), sea salt (2.3 % ± 1.6 %), trace element oxides (1.0 % ± 1.1 %), water (7.2 % ± 3.3 %) at 35 % RH, and residual matter (40 % ± 24 %). Analysis of filter samples reveals that several PM2.5 chemical components varied by more than an order of magnitude between sites. Ammoniated sulfate ranges from 1.1 µg m−3 (Buenos Aires, Argentina) to 17 µg m−3 (Kanpur, India in the dry season). Ammonium nitrate ranged from 0.2 µg m−3 (Mammoth Cave, in summer) to 6.8  µg m−3 (Kanpur, dry season). Equivalent black carbon ranged from 0.7 µg m−3 (Mammoth Cave) to over 8 µg m−3 (Dhaka, Bangladesh and Kanpur, India). Comparison of SPARTAN vs. coincident measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network at Mammoth Cave yielded a high degree of consistency for daily PM2.5 (r2 = 0.76, slope  =  1.12), daily sulfate (r2 = 0.86, slope  =  1.03), and mean fractions of all major PM2.5 components (within 6 %). Major ions generally agree well with previous studies at the same urban locations (e.g. sulfate fractions agree within 4 % for 8 out of 11 collocation comparisons). Enhanced anthropogenic dust fractions in large urban areas (e.g. Singapore, Kanpur, Hanoi, and Dhaka) are apparent from high Zn : Al ratios. The expected water contribution to aerosols is calculated via the hygroscopicity parameter κv for each filter. Mean aggregate values ranged from 0.15 (Ilorin) to 0.28 (Rehovot). The all-site parameter mean is 0.20 ± 0.04. Chemical composition and water retention in each filter measurement allows inference of hourly PM2.5 at 35 % relative humidity by merging with nephelometer measurements. These hourly PM2.5 estimates compare favourably with a beta attenuation monitor (MetOne) at the nearby US embassy in Beijing, with a coefficient of variation r2 =  0.67 (n = 3167), compared to r2 = 0.62 when κv was not considered. SPARTAN continues to provide an open-access database of PM2.5 compositional filter information and hourly mass collected from a global federation of instruments.
Physics of Stratocumulus Top (POST): turbulence characteristics

Turbulence observed during the Physics of Stratocumulus Top (POST) research campaign is analyzed. Using in-flight measurements of dynamic and thermodynamic variables at the interface between the stratocumulus cloud top and free troposphere, the cloud top region is classified into sublayers, and the thicknesses of these sublayers are estimated. The data are used to calculate turbulence characteristics, including the bulk Richardson number, mean-square velocity fluctuations, turbulence kinetic energy (TKE), TKE dissipation rate, and Corrsin, Ozmidov and Kolmogorov scales. A comparison of these properties among different sublayers indicates that the entrainment interfacial layer consists of two significantly different sublayers: the turbulent inversion sublayer (TISL) and the moist, yet hydrostatically stable, cloud top mixing sublayer (CTMSL). Both sublayers are marginally turbulent, i.e., the bulk Richardson number across the layers is critical. This means that turbulence is produced by shear and damped by buoyancy such that the sublayer thicknesses adapt to temperature and wind variations across them. Turbulence in both sublayers is anisotropic, with Corrsin and Ozmidov scales as small as ∼  0.3 and ∼  3 m in the TISL and CTMSL, respectively. These values are ∼  60 and ∼  15 times smaller than typical layer depths, indicating flattened large eddies and suggesting no direct mixing of cloud top and free-tropospheric air. Also, small scales of turbulence are different in sublayers as indicated by the corresponding values of Kolmogorov scales and buoyant and shear Reynolds numbers.