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An analysis of pollution plumes emitted from sources in the Northeastern US was based on observations from the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) 2004 field campaign. Particular attention was given to the relation of these plumes to coastal transport patterns in lower tropospheric layers throughout the Gulf of Maine (GOM) and their contribution to large-scale pollution outflow from the North American continent. Using measurements obtained during a series of flights of the NOAA WP-3D and the NASA DC-8, a unique quasi-lagrangian case study was conducted for a freshly emitted plume emanating from the New York City source region in late July 2004. The initial development of this plume stemmed from the accumulation of boundary layer pollutants within a coastal residual layer where weak synoptic forcing triggered its advection by mean southwesterly flow. As the plume tracked into the GOM, analysis showed that the plume layer vertical structure evolved into an internal boundary layer form, with signatures of steep vertical gradients in temperature, moisture and wind speed often resulting in periodic turbulence. This structure remained well-defined during the plume study, allowing for the detachment of the plume layer from the surface and thus minimal deposition and plume-sea surface exchange. In contrast, lateral mixing with other low-level plumes was significant during its transit and facilitated in part by persistent shear driven turbulence which further contributed to the high spatial variability in trace gas mixing ratios. The impact of the plume inland was assessed using observations from the AIRMAP air quality network. This impact was noticeably detected as a contribution to poor surface ozone conditions and significant elevations of other major pollutants to levels equaling the highest observed that summer. Further contributions to larger-scale outflow across the North Atlantic was also observed and analyzed.
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A technique for the tracking of individual clouds in a Large Eddy Simulation (LES) is presented. We use this technique on an LES of a shallow cumulus cloud field based upon the Barbados Oceanographic and Meteorological Experiment (BOMEX) to calculate statistics of cloud height, lifetime, and other physical properties for individual clouds in the model. We also examine the question of nature versus nurture in shallow cumulus clouds: do properties at cloud base determine the upper-level properties of the clouds (nature), or are cloud properties determined by the environmental conditions they encounter (nurture). We find that clouds which ascend through an environment that has been pre-moistened by previous cloud activity are no more likely to reach the inversion than clouds that ascend through a drier environment. Cloud base thermodynamic properties are uncorrelated with upper-level cloud properties, while mean fractional entrainment and detrainment rates display moderate correlations with cloud properties up to the inversion. Conversely, cloud base area correlates well with upper-level cloud area and maximum cloud height. We conclude that cloud thermodynamic properties are primarily influenced by entrainment and detrainment processes, cloud area and height are primarily influenced by cloud base area, and thus nature and nurture both play roles in the dynamics of BOMEX shallow cumulus clouds.
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We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands) was a net exporter of primary organic aerosol (42 kT) and black carbon aerosol (11 kT). We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA), with Borneo being a net exporter of SOA (15 kT). SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%), with smaller contributions from gas-phase oxidation (15%) and advection into the regions (14%). We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD) data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where the model has the least skill at reproducing the data, where the model has a negative bias of 76% and only captures 14% of the observed variability. This model performance reflects the small-scale island-marine environment and the mix of aerosol species, with the model showing more skill at reproducing observed AOD over larger continental regions such as China where AOD is dominated by one aerosol type. The model shows that AOD over Borneo is approximately evenly split between organic and sulphate aerosol with sea salt representing 10–20% during May–September; we find a similar breakdown over continental Southeast Asia but with less sea salt aerosol and more dust aerosol. In contrast, East China AOD is determined mainly by sulphate aerosol and a seasonal source of dust aerosol, as expected. Realistic sensitivity runs, designed to test our underlying assumptions about emissions and chemistry over Borneo, show that model AOD is most sensitive to isoprene emissions and organic gas-phase partitioning but all fail to improve significantly upon the control model calculation. This emphasises the multi-faceted dimension of the problem and the need for concurrent and coordinated development of BVOC emissions, and BVOC chemistry and organic aerosol formation mechanisms.
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Observations of a comprehensive suite of inorganic and organic trace gases, including non-methane hydrocarbons (NMHCs), halogenated organics and oxygenated volatile organic compounds (OVOCs), obtained from the NASA DC-8 over Canada during the ARCTAS aircraft campaign in July 2008 illustrate that convection is important for redistributing both long- and short-lived species throughout the troposphere. Convective outflow events were identified by the elevated mixing ratios of organic species in the upper troposphere relative to background conditions. Several dramatic events were observed in which isoprene and its oxidation products were detected at hundreds of pptv at altitudes higher than 8 km. Two events are studied in detail using detailed experimental data and the NASA Langley Research Center (LaRC) box model. One event had no lightning NO<sub>x</sub> (NO + NO<sub>2</sub>) associated with it and the other had substantial lightning NO<sub>x</sub> (LNO<sub>x</sub> > 1 ppbv). When convective storms transport isoprene from the boundary layer to the upper troposphere and no LNO<sub>x</sub> is present, OH is reduced due to scavenging by isoprene, which serves to slow the chemistry, resulting in longer lifetimes for species that react with OH. Ozone and PAN production is minimal in this case. In the case where isoprene is convected and LNO<sub>x</sub> is present, there is a large effect on the expected ensuing chemistry: isoprene exerts a dominant impact on HO<sub>x</sub> and nitrogen-containing species; the relative contribution from other species to HO<sub>x</sub>, such as peroxides, is insignificant. The isoprene reacts quickly, resulting in primary and secondary products, including formaldehyde and methyl glyoxal. The model predicts enhanced production of alkyl nitrates (ANs) and peroxyacyl nitrate compounds (PANs). PANs persist because of the cold temperatures of the upper troposphere resulting in a large change in the NO<sub>x</sub> mixing ratios which, in turn, has a large impact on the HO<sub>x</sub> chemistry. Ozone production is substantial during the first few hours following the convection to the UT, resulting in a net gain of approximately 10 ppbv compared to the modeled scenario in which LNO<sub>x</sub> is present but no isoprene is present aloft.
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We use observations from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument and a global aerosol-climate model to document an aerosol layer that forms in the vicinity of the tropical tropopause layer (TTL) over the Southern Asian and Indian Ocean region. CALIOP observations suggest that the aerosol layer is present throughout the year and follows the migration of the Intertropical Convergence Zone (ITCZ). The layer is located at about 20° N during boreal summers and at about 15° S in boreal winters. The ECHAM5.5-HAM2 aerosol-climate model reproduces such an aerosol layer close to the TTL but overestimates the observed aerosol extinction. The mismatch between observed and simulated aerosols extinction are discussed in terms of uncertainties related to CALIOP and possible problems in the model. Sensitivity model simulations indicate that (i) sulfate particles resulting from SO<sub>2</sub> and DMS oxidation are the main contributors to the mean aerosol extinction in the layer throughout the year, and (ii) transport of sulfate precursors by convection followed by nucleation is responsible for the formation of the aerosol layer. The reflection of shortwave radiations by aerosols in the TTL may be negligible, however, cloud droplets formed by these aerosols may reflect about 6 W m<sup>−2</sup> back to space. Overall, this study provides new insights in term of composition of the tropical upper troposphere.
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Several different types of parameterization of heterogeneous ice nucleation for cloud and climate models have been developed over the past decades, ranging from empirically-derived expressions to parameterizations of ice crystal nucleation rates derived from theory, including the parameterization developed by the authors that includes simultaneous dependence on the temperature and saturation ratio, hereafter referred to as KC. Parameterizations schemes that address the deliquescence-heterogeneous-freezing (DHetF), which combines the modes of condensation freezing and immersion freezing, are assessed here in the context of thermodynamic constraints, laboratory measurements, and recent field measurements. It is shown that empirical schemes depending only on the ice saturation ratio or only on temperature can produce reasonable crystal concentrations, but ice crystal nucleation is thermodynamically prohibited in certain regions of the temperature-saturation ratio phase space. Some recent empirical parameterizations yield clouds that are almost entire liquid at temperatures as low as −35 °C in contrast to cloud climatology. Reasonable performance of the KC ice nucleation scheme is demonstrated by comparison with numerous data from several recent field campaigns, laboratory data, climatology of cloud phase-state. Several mis-applications of the KC parameterization that appeared recently in the literature are described and corrected. It is emphasized here that a correct application of the KC scheme requires integration of the individual nucleation rates over the measured size spectrum of ice nuclei that represent a fraction or several fractions of the environmental aerosol with specific ice nucleation properties. The concentration in these fractions can be substantially smaller than that of the total aerosol, but greater than the crystal concentration measured by an experimental device. Simulations with temperature-dependent active site area or with several IN fractions having different properties show that ice nucleation in the KC scheme occurs in a wide temperature range of 10–20 °C, which depends on IN properties. Simulation with a spectral bin model and correct application of KC scheme adequately describes ice nucleation via the DHetF mode and yields crystal concentrations and phase state close to those measured in the single-layer stratocumulus cloud observed in the Mixed Phase Arctic Cloud Experiment (MPACE). An assessment of some deficiencies in current parcel modeling methods and cloud chamber observations and their impact on parameterization development and evaluation is provided.
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Deposition nucleation on two mineral species, kaolinite and illite, was studied using a flow cell coupled to an optical microscope. The results show that the <i>S</i><sub>ice</sub> conditions when ice first nucleated, defined as the onset <i>S</i><sub>ice</sub> (<i>S</i><sub>ice,onset</sub>), is a strong function of the surface area available for nucleation, varying from 100% to 125% at temperatures between 242 and 239 K. The surface area dependent data could not be described accurately using classical nucleation theory and the assumption of a single contact angle (defined here as the single-α model). These results suggest that caution should be applied when using contact angles determined from <i>S</i><sub>ice,onset</sub> data and the single-α model. In contrast to the single-α model, the active site model, the deterministic model, and a model with a distribution of contact angles fit the data within experimental uncertainties. Parameters from the fits to the data are presented.
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Project Surya has documented indoor and outdoor concentrations of black carbon (BC) from traditional biomass burning cook stoves in a rural village located in the Indo-Gangetic Plains (IGP) region of N. India from November 2009–September 2010. In this paper, we systematically document the link between local scale aerosol properties and column averaged regional aerosol optical properties and atmospheric radiative forcing. We document observations from the first phase of Project Surya and estimate the source dependent (biomass and fossil fuels) aerosol optical properties from local to regional scale. Data were collected using surface based observations of BC, organic carbon (OC), aerosol light absorption, scattering coefficient at the Surya village (SVI_1) located in IGP region and integrated with satellite and AERONET observations at the regional scale (IGP). The daily mean BC concentrations at SVI_1 showed a large increase of BC during the dry season (December to February) with values reaching 35 μg m<sup>−3</sup>. Space based LIDAR data revealed how the biomass smoke was trapped within the first kilometer during the dry season and extended to above 5 km during the pre-monsoon season. As a result, during the dry season, the variance in the daily mean single scattering albedo (SSA), the ratio of scattering to extinction coefficient, and column aerosol optical properties at the local IGP site correlated (with slopes in the range of 0.85 to 1.06 and <i>R</i><sup>2</sup>>0.4) well with the "IGP_AERONET" (mean of six AERONET sites). The statistically significant correlation suggested that in-situ observations can be used to derive spatial mean forcing, at least for the dry season. The atmospheric forcing due to BC and OC exceeded 20 Wm<sup>−2</sup> during all months from November to May, supporting the deduction that elimination of cook stove smoke emissions through clean cooking technologies will likely have a major positive impact not only on human health but also on regional climate.
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We conducted measurements of the five important short-lived organic bromine species in the marine boundary layer (MBL). Measurements were made in the Northern Hemisphere mid-latitudes (Sylt Island, North Sea) in June 2009 and in the tropical Western Pacific during the TransBrom ship campaign in October 2009. For the one-week time series on Sylt Island, mean mixing ratios of CHBr<sub>3</sub>, CH<sub>2</sub>Br<sub>2</sub>, CHBr<sub>2</sub>Cl and CH<sub>2</sub>BrCl were 2.0, 1.1, 0.2, 0.1 ppt, respectively. We found maxima of 5.8 and 1.6 ppt for the two main components CHBr<sub>3</sub> and CH<sub>2</sub>Br<sub>2</sub>. Along the cruise track in the Western Pacific (between 41° N and 13° S) we measured mean mixing ratios of 0.9, 0.9, 0.2, 0.1 and 0.1 ppt for CHBr<sub>3</sub>, CH<sub>2</sub>Br<sub>2</sub>, CHBrCl<sub>2</sub>, CHBr<sub>2</sub>Cl and CH<sub>2</sub>BrCl. Air samples with coastal influence showed considerably higher mixing ratios than the samples with open ocean origin. Correlation analyses of the two data sets yielded strong linear relationships between the mixing ratios of four of the five species (except for CH<sub>2</sub>BrCl). Using a combined data set from the two campaigns and a comparison with the results from two former studies, rough estimates of the molar emission ratios between the correlated substances were: 9/1/0.35/0.35 for CHBr<sub>3</sub>/CH<sub>2</sub>Br<sub>2</sub>/CHBrCl<sub>2</sub>/CHBr<sub>2</sub>Cl. Additional measurements were made in the tropical tropopause layer (TTL) above Teresina (Brazil, 5° S) in June 2008, using balloon-borne cryogenic whole air sampling technique. Near the level of zero clear-sky net radiative heating (LZRH) at 14.8 km about 2.25 ppt organic bromine was bound to the five short-lived species, making up 13% of total organic bromine (17.82 ppt). CH<sub>2</sub>Br<sub>2</sub> (1.45 ppt) and CHBr<sub>3</sub> (0.56 ppt) accounted for 90% of the budget of short-lived compounds in that region. Near the tropopause (at 17.5 km) organic bromine from these substances was reduced to 1.35 ppt, with 1.07 and 0.12 ppt attributed to CH<sub>2</sub>Br<sub>2</sub> and CHBr<sub>3</sub>, respectively.
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In this paper we analyse aerosol loading and its direct radiative effects over the Bay of Bengal (BoB) and Arabian Sea (AS) regions for the Integrated Campaign on Aerosols, gases and Radiation Budget (ICARB) undertaken during 2006, using satellite data from the MODerate Resolution Imaging Spectroradiometer (MODIS) on board the Terra and Aqua satellites, the Aerosol Index from the Ozone Monitoring Instrument (OMI) on board the Aura satellite, and the European-Community Hamburg (ECHAM5.5) general circulation model extended by Hamburg Aerosol Module (HAM). By statistically comparing with large-scale satellite data sets, we firstly show that the aerosol properties measured during the ship-based ICARB campaign and simulated by the model are representative for the BoB and AS regions and the pre-monsoon season. In a second step, the modelled aerosol distributions were evaluated by a comparison with the measurements from the ship-based sunphotometer, and the satellite retrievals during ICARB. It is found that the model broadly reproduces the observed spatial and temporal variability in aerosol optical depth (AOD) over BoB and AS regions. However, AOD was systematically underestimated during high-pollution episodes, especially in the BoB leg. We show that this underprediction of AOD is mostly because of the deficiencies in the coarse mode, where the model shows that dust is the dominant component. The analysis of dust AOD along with the OMI Aerosol Index indicate that missing dust transport that results from too low dust emission fluxes over the Thar Desert region in the model caused this deficiency. Thirdly, we analysed the spatio-temporal variability of AOD comparing the ship-based observations to the large-scale satellite observations and simulations. It was found that most of the variability along the track was from geographical patterns, with a minor influence by single events. Aerosol fields were homogeneous enough to yield a good statistical agreement between satellite data at a 1° spatial, but only twice-daily temporal resolution, and the ship-based sunphotometer data at a much finer spatial, but daily-average temporal resolution. Examination of the satellite data further showed that the year 2006 is representative for the five-year period for which satellite data were available. Finally, we estimated the clear-sky solar direct aerosol radiative forcing (DARF). We found that the cruise represents well the regional-seasonal mean forcings. Constraining simulated forcings using the observed AOD distributions yields a robust estimate of regional-seasonal mean DARF of −8.6, −21.4 and +12.9 W m<sup>−2</sup> at the top of the atmosphere (TOA), at the surface (SUR) and in the atmosphere (ATM), respectively, for the BoB region, and over the AS, of, −6.8, −12.8, and +6 W m<sup>−2</sup> at TOA, SUR, and ATM, respectively.
