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A cloud-resolving model (CRM) coupled to a new intermediate-complexity bulk aerosol scheme is used to study aerosol–boundary-layer–cloud–precipitation interactions and the development of pockets of open cells (POCs) in subtropical stratocumulus cloud layers. The aerosol scheme prognoses mass and number concentration of a single lognormal accumulation mode with surface and entrainment sources, evolving subject to processing of activated aerosol and scavenging of dry aerosol by clouds and rain. <br><br> The CRM with the aerosol scheme is applied to a range of steadily forced cases idealized from a well-observed POC. The long-term system evolution is explored with extended two-dimensional (2-D) simulations of up to 20 days, mostly with diurnally averaged insolation and 24 km wide domains, and one 10 day three-dimensional (3-D) simulation. Both 2-D and 3-D simulations support the Baker–Charlson hypothesis of two distinct aerosol–cloud "regimes" (deep/high-aerosol/non-drizzling and shallow/low-aerosol/drizzling) that persist for days; transitions between these regimes, driven by either precipitation scavenging or aerosol entrainment from the free-troposphere (FT), occur on a timescale of ten hours. The system is analyzed using a two-dimensional phase plane with inversion height and boundary layer average aerosol concentrations as state variables; depending on the specified subsidence rate and availability of FT aerosol, these regimes are either stable equilibria or distinct legs of a slow limit cycle. <br><br> The same steadily forced modeling framework is applied to the coupled development and evolution of a POC and the surrounding overcast boundary layer in a larger 192 km wide domain. An initial 50% aerosol reduction is applied to half of the model domain. This has little effect until the stratocumulus thickens enough to drizzle, at which time the low-aerosol portion transitions into open-cell convection, forming a POC. Reduced entrainment in the POC induces a negative feedback between the areal fraction covered by the POC and boundary layer depth changes. This stabilizes the system by controlling liquid water path and precipitation sinks of aerosol number in the overcast region, while also preventing boundary layer collapse within the POC, allowing the POC and overcast to coexist indefinitely in a quasi-steady equilibrium.
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The atmospheric organic aerosol composition is characterized by a great diversity of functional groups and chemical species, challenging simple classification schemes. Traditional offline chemical methods identify chemical classes based on the retention behaviour on chromatographic columns and absorbing beds. Such an approach led to the isolation of complex mixtures of compounds such as the humic-like substances (HULIS). More recently, online aerosol mass spectrometry (AMS) was employed to identify chemical classes by extracting fragmentation patterns from experimental data series using statistical methods (factor analysis), providing simplified schemes for the classification of oxygenated organic aerosols (OOAs) on the basis of the distribution of oxygen-containing functionalities. The analysis of numerous AMS data sets suggested the occurrence of very oxidized OOAs which were postulated to correspond to HULIS. However, only a few efforts were made to test the correspondence of the AMS classes of OOAs with the traditional classifications from the offline methods. In this paper, we consider a case study representative of polluted continental regional background environments. We examine the AMS factors for OOAs identified by positive matrix factorization (PMF) and compare them to chemical classes of water-soluble organic carbon (WSOC) analysed offline on a set of filters collected in parallel. WSOC fractionation was performed by means of factor analysis applied to proton nuclear magnetic resonance (NMR) spectroscopic data, and by applying an ion-exchange chromatographic method for direct quantification of HULIS. Results show that the very oxidized low-volatility OOAs from AMS correlate with the NMR factor showing HULIS features and also with true "chromatographic" HULIS. On the other hand, UV/VIS-absorbing polyacids (or HULIS {sensu stricto}) isolated on ion-exchange beds were only a fraction of the AMS and NMR organic carbon fractions showing functional groups attributable to highly substituted carboxylic acids, suggesting that unspeciated low-molecular weight organic acids contribute to HULIS in the broad sense.
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The use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability, and the sustainability of fuel sources. Concurrent reductions in particulate emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January–February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer–Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. <br><br> Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions in mass of 86% averaged over all powers) and blended fuels (66%) relative to the JP-8 baseline with the largest reductions at idle conditions. At 7% power, this corresponds to a reduction from 7.6 mg kg<sup>−1</sup> for JP-8 to 1.2 mg kg<sup>−1</sup> for the natural gas FT fuel. At full power, soot emissions were reduced from 103 to 24 mg kg<sup>−1</sup> (JP-8 and natural gas FT, respectively). The alternative fuels also produced smaller soot (e.g., at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the natural gas FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. <br><br> As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30–44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near zero for FT fuels) due to decreased fuel sulfur content. <br><br> To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (−4 to 20 °C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to −8 × 10<sup>14</sup> particles (kg fuel)<sup>−1</sup> °C<sup>−1</sup> for particle number emissions and −10 mm<sup>3</sup> (kg fuel)<sup>−1</sup> °C<sup>−1</sup> for particle volume emissions. The temperature dependency of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft-produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols, with a smaller fraction as a soot coating. Conversion efficiencies of up to 2.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO<sub>2</sub>) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.
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We examine spatial variations in the weekday–weekend pattern of NO<sub>2</sub> over the Los Angeles metropolitan area using the Ozone Monitoring Instrument (OMI) and then compare the observations to calculations using the WRF-Chem model. We find that the spatial pattern of the weekday–weekend variations of the NO<sub>2</sub> column in the model is significantly different than observed. A sensitivity study shows that the contrasting spatial pattern of NO<sub>2</sub> on weekdays and weekends is a useful diagnostic of emissions and chemistry. These improvements suggest that constraints from space-based observations of the processes affecting urban photochemistry (e.g., spatial patterns of emissions, ratios of VOC to NO<sub>x</sub> emissions, rate constants) are possible at a level of detail not previously described.
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The interaction between marine boundary layer cellular cloudiness and surface fluxes of sensible and latent heat is investigated. The investigation focuses on the non-precipitating closed-cell state and the precipitating open-cell state at low geostrophic wind speed. The Advanced Research WRF (Weather Research and Forecasting) model is used to conduct cloud system-resolving simulations with interactive surface fluxes of sensible heat, latent heat, and of sea salt aerosol, and with a detailed representation of the interaction between aerosol particles and clouds. The mechanisms responsible for the temporal evolution and spatial distribution of the surface heat fluxes in the closed- and open-cell state are investigated and explained. It is found that the closed-cell state imposes its horizontal spatial structure on surface air temperature and water vapor, and, to a lesser degree, on the surface sensible and latent heat flux. The responsible mechanism is the entrainment of dry, free tropospheric air into the boundary layer. The open-cell state is associated with oscillations in surface air temperature, water vapor, and in the surface fluxes of sensible heat, latent heat, and of sea salt aerosol. Here, the responsible mechanism is the periodic formation of clouds, rain, and of cold and moist pools with elevated wind speed. Open-cell cloud formation, cloud optical depth and liquid water path, and cloud and rain water path are identified as good predictors of the horizontal spatial structure of surface air temperature and sensible heat flux, but not of surface water vapor and latent heat flux. It is shown that the open-cell state creates conditions conducive to its maintenance by enhancing the surface sensible heat flux. The open-cell state also enhances the sea salt flux relative to the closed-cell state. While the open-cell state under consideration is not depleted in aerosol and is insensitive to variations in sea salt fluxes, in aerosol-depleted conditions, the enhancement of the sea salt flux may replenish the aerosol needed for cloud formation and hence contribute to the maintenance of the open-cell state. Spatial homogenization of the surface fluxes is found to have only a small effect on cloud properties in the investigated cases.
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This study tests a novel methodology to add value to satellite data sets. This methodology, data fusion, is similar to data assimilation, except that the background model-based field is replaced by a satellite data set, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these data sets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS–TES and AIRS–MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20–30% and above 20%, respectively) as compared with AIRS-only version 5 CO retrievals, and improved daily coverage compared with TES and MLS CO data.
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The terrestrial biosphere is currently acting as a net carbon sink on the global scale, exhibiting significant interannual variability in strength. To reliably predict the future strength of the land sink and its role in atmospheric CO<sub>2</sub> growth, the underlying biogeochemical processes and their response to a changing climate need to be well understood. In particular, better knowledge of the impact of key climate variables such as temperature or precipitation on the biospheric carbon reservoir is essential. <br><br> It is demonstrated using nearly a decade of SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) nadir measurements that years with higher temperatures during the growing season can be robustly associated with larger growth rates in atmospheric CO<sub>2</sub> and smaller seasonal cycle amplitudes for northern mid-latitudes. We find linear relationships between warming and CO<sub>2</sub> growth as well as seasonal cycle amplitude at the 98% significance level. This suggests that the terrestrial carbon sink is less efficient at higher temperatures during the analysed time period. Unless the biosphere has the ability to adapt its carbon storage under warming conditions in the longer term, such a temperature response entails the risk of potential future sink saturation via a positive carbon-climate feedback. <br><br> Quantitatively, the covariation between the annual CO<sub>2</sub> growth rates derived from SCIAMACHY data and warm season surface temperature anomaly amounts to 1.25 ± 0.32 ppm yr<sup>−1</sup> K<sup>−1</sup> for the Northern Hemisphere, where the bulk of the terrestrial carbon sink is located. In comparison, this relationship is less pronounced in the Southern Hemisphere. The covariation of the seasonal cycle amplitudes retrieved from satellite measurements and temperature anomaly is −1.30 ± 0.31 ppm K<sup>−1</sup> for the north temperate zone. These estimates are consistent with those from the CarbonTracker data assimilated CO<sub>2</sub> data product, indicating that the temperature dependence of the model surface fluxes is realistic.
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Observations show that the Mediterranean troposphere is characterized by a marked enhancement in summertime ozone, with a maximum over the eastern Mediterranean. This has been linked to enhanced photochemical ozone production and subsidence under cloud-free anticyclonic conditions. The eastern Mediterranean is among the regions with the highest levels of background tropospheric ozone worldwide. A 12 yr climatological analysis (1998–2009) of free-tropospheric ozone was carried out over the region based on the ECMWF (European Centre for Medium-Range Weather Forecasts) ERA-Interim reanalysis data and simulations with the EMAC (ECHAM5–MESSy) atmospheric chemistry–climate model. EMAC is nudged towards the ECMWF analysis data and includes a stratospheric ozone tracer. A characteristic summertime pool with high ozone concentrations is found in the middle troposphere over the eastern Mediterranean–Middle East (EMME) in the ERA-Interim ozone data, Tropospheric Emission Spectrometer (TES) satellite ozone data and simulations with EMAC. The enhanced ozone over the EMME during summer is a robust feature, extending down to lower free-tropospheric levels. The investigation of ozone in relation to potential vorticity and water vapour and the stratospheric ozone tracer indicates that the dominant mechanism causing the free-tropospheric ozone pool is the downward transport from the upper troposphere and lower stratosphere, in association with the enhanced subsidence and the limited horizontal divergence observed over the region. The implications of these high free-tropospheric ozone levels on the seasonal cycle of near-surface ozone over the Mediterranean are discussed.
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Mineral dust aerosols often observed over California in winter and spring, associated with long-range transport from Asia and the Sahara, have been linked to enhanced precipitation based on observations. Local anthropogenic pollution, on the other hand, was shown in previous observational and modeling studies to reduce precipitation. Here we incorporate recent developments in ice nucleation parameterizations to link aerosols with ice crystal formation in a spectral-bin cloud microphysical model coupled with the Weather Research and Forecasting (WRF) model in order to examine the relative and combined impacts of dust and local pollution particles on cloud properties and precipitation type and intensity. Simulations are carried out for two cloud cases (from the CalWater 2011 field campaign) with contrasting meteorology and cloud dynamics that occurred on 16 February (FEB16) and 2 March (MAR02). In both cases, observations show the presence of dust and biological particles in a relative pristine environment. The simulated cloud microphysical properties and precipitation show reasonable agreement with aircraft and surface measurements. Model sensitivity experiments indicate that in the pristine environment, the dust and biological aerosol layers increase the accumulated precipitation by 10–20% from the Central Valley to the Sierra Nevada for both FEB16 and MAR02 due to a ~40% increase in snow formation, validating the observational hypothesis. Model results show that local pollution increases precipitation over the windward slope of the mountains by a few percent due to increased snow formation when dust is present, but reduces precipitation by 5–8% if dust is removed on FEB16. The effects of local pollution on cloud microphysics and precipitation strongly depend on meteorology, including cloud dynamics and the strength of the Sierra Barrier Jet. This study further underscores the importance of the interactions between local pollution, dust, and environmental conditions for assessing aerosol effects on cold-season precipitation in California.
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Light scattering by single, inhomogeneous mineral dust particles was simulated based on shapes and compositions derived directly from measurements of real dust particles instead of using a mathematical shape model. We demonstrate the use of the stereogrammetric shape retrieval method in the context of single-scattering modelling of mineral dust for four different dust types – all of them inhomogeneous – ranging from compact, equidimensional shapes to very elongated and aggregate shapes. The three-dimensional particle shapes were derived from stereo pairs of scanning-electron microscope images, and inhomogeneous composition was determined by mineralogical interpretation of localized elemental information based on energy-dispersive spectroscopy. Scattering computations were performed for particles of equal-volume diameters, from 0.08 μm up to 2.8 μm at 550 nm wavelength, using the discrete-dipole approximation. Particle-to-particle variation in scattering by mineral dust was found to be quite considerable and was not well reproduced by simplified shapes of homogeneous spheres, spheroids, or Gaussian random spheres. Effective-medium approximation results revealed that particle inhomogeneity should be accounted for even for small amounts of absorbing media (here up to 2% of the volume), especially when considering scattering by inhomogeneous particles at size parameters 3<<i>x</i><8. When integrated over a log-normal size distribution, the linear depolarization ratio and single-scattering albedo were also found to be sensitive to inhomogeneity. The methodology applied is work-intensive and the light-scattering method used quite limited in terms of size parameter coverage. It would therefore be desirable to find a sufficiently accurate but simpler approach with fewer limitations for single-scattering modelling of dust. For validation of such a method, the approach presented here could be used for producing reference data when applied to a suitable set of target particles.
