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The structure of the atmospheric boundary layer (ABL) and its influence on regional air quality over the Pearl River Delta (PRD) were examined through two intensive observations in October 2004 and July 2006. Analytical results show the presence of two types of typical weather conditions associated with poor air quality over the PRD. The first is the warm period before a cold front (WPBCF) and the second is the subsidence period controlled by a tropical cyclone (SPCTC). Two typical low air quality situations, which are affected by WPBCF and SPCTC, and one high air quality situation were analysed in detail. Results showed that continuously low or calm ground winds resulted in the accumulation of pollutants, and sea-land breezes had an important role during low air quality conditions. Data on recirculation factors showed that recirculation was significant during low air quality conditions, and steady transportation occurred during high air quality conditions. The ventilation index and the 24 h average ventilation index during high air quality conditions were significantly higher than those during low air quality conditions. Deep and stable inversion layers inside the ABL remarkably affected low air quality. Surface and low-altitude inversions were usually observed during WPBCF, contrary to during SPCTC, during which only the low-altitude inversion appeared frequently.
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This paper provides compelling evidence for the importance of heterogeneous nucleation, likely on solid particles of meteoritic origin, and of small-scale temperature fluctuations, for the formation of ice particles in the Arctic stratosphere. During January 2010, ice PSCs (polar stratospheric clouds) were shown by CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) to have occurred on a synoptic scale (~1000 km dimension). CALIPSO observations also showed widespread PSCs containing NAT (nitric acid trihydrate) particles in December 2009, prior to the occurrence of synoptic-scale regions of ice PSCs during mid-January 2010. We demonstrate by means of detailed microphysical modeling along air parcel trajectories that the formation of these PSCs is not readily reconciled with expectations from the conventional understanding of PSC nucleation mechanisms. The measurements are at odds with the previous laboratory-based understanding of PSC formation, which deemed direct heterogeneous nucleation of NAT and ice on preexisting solid particles unlikely. While a companion paper (Part 1) addresses the heterogeneous nucleation of NAT during December 2009, before the existence of ice PSCs, this paper shows that also the large-scale occurrence of stratospheric ice in January 2010 cannot be explained merely by homogeneous ice nucleation but requires the heterogeneous nucleation of ice, e.g. on meteoritic dust or preexisting NAT particles. The required efficiency of the ice nuclei is surprisingly high, namely comparable to that of known tropospheric ice nuclei such as mineral dust particles. To gain model agreement with the ice number densities inferred from observations, the presence of small-scale temperature fluctuations, with wavelengths unresolved by the numerical weather prediction models, is required. With the derived rate parameterization for heterogeneous ice nucleation we are able to explain and reproduce CALIPSO observations throughout the entire Arctic winter 2009/2010.
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We aim to reconcile the recently published, apparently contrasting results regarding the relative importance of tropical upwelling versus horizontal transport for the seasonality of ozone above the tropical tropopause. Different analysis methods in the literature (Lagrangian versus Eulerian, and isentropic versus pressure vertical coordinates) yield different perspectives of ozone transport, and the results must be carefully compared in equivalent terms to avoid misinterpretation. By examining the Lagrangian calculations in the Eulerian formulation, we show here that the results are in fact consistent with each other and with a common understanding of the ozone transport processes near and above the tropical tropopause. <br><br> We further emphasize that the complementary approaches are suited for answering two different scientific questions: (1) what drives the observed seasonal cycle in ozone at a particular level above the tropical tropopause? and (2) how important is horizontal transport from mid-latitudes for ozone concentrations in the tropical lower stratosphere? Regarding the first question, the analysis of the transformed Eulerian mean (TEM) ozone budget shows that the annual cycle in tropical upwelling is the main forcing of the ozone seasonality at altitudes with large vertical gradients in the tropical lower stratosphere. To answer the second question a Lagrangian framework must be used, and the results show that a large fraction (~50%) of the ozone molecules ascending through the tropical lower stratosphere is of extra-tropical origin and has been in-mixed from mid-latitudes.
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The CRISTA-NF (Cryogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers) instrument is an airborne infrared limb sounder operated aboard the Russian research aircraft M55-Geophysica. The instrument successfully participated in a large Arctic aircraft campaign within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) project in Kiruna (Sweden) from January to March 2010. <br><br> This paper concentrates on the measurements taken during one flight of the campaign, which took place on 2 March in the vicinity of the polar vortex. We present two-dimensional cross-sections of derived volume mixing ratios for the trace gases CFC-11, O<sub>3</sub>, and ClONO<sub>2</sub> with an unprecedented vertical resolution of about 500 to 600 m for a large part of the observed altitude range (≈ 6–19 km) and a dense horizontal sampling along flight direction of ≈ 15 km. The trace gas distributions show several structures, for example a part of the polar vortex and a vortex filament, which can be identified by means of O<sub>3</sub>–CFC-11 tracer–tracer correlations. <br><br> The observations made during this flight are interpreted using the chemistry and transport model CLaMS (Chemical Lagrangian Model of the Stratosphere). Comparisons of the observations with the model results are used to assess the performance of the model with respect to advection, mixing, and the chemistry in the polar vortex. These comparisons confirm the capability of CLaMS to reproduce even very small-scale structures in the atmosphere, which partly have a vertical extent of only 1 km. Based on the good agreement between simulation and observation, we use artificial (passive) tracers, which represent different air mass origins (e.g. vortex, tropics), to further analyse the CRISTA-NF observations in terms of the composition of air mass origins. These passive tracers clearly illustrate the observation of filamentary structures that include tropical air masses. A characteristic of the Arctic winter 2009/10 was a sudden stratospheric warming in December that led to a split of the polar vortex. The vortex re-established at the end of December. Our passive tracer simulations suggest that large parts of the re-established vortex consisted to about 45% of high- and mid-latitude air.
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Atmospheric mercury is a toxic air and water pollutant that is of significant concern because of its effects on human health and ecosystems. A mechanistic representation of the atmospheric mercury cycle is developed for the state-of-the-art global climate-chemistry model, CAM-Chem (Community Atmospheric Model with Chemistry). The model simulates the emission, transport, transformation and deposition of atmospheric mercury (Hg) in three forms: elemental mercury (Hg(0)), reactive mercury (Hg(II)), and particulate mercury (PHg). Emissions of mercury include those from human, land, ocean, biomass burning and volcano related sources. Land emissions are calculated based on surface solar radiation flux and skin temperature. A simplified air–sea mercury exchange scheme is used to calculate emissions from the oceans. The chemistry mechanism includes the oxidation of Hg(0) in gaseous phase by ozone with temperature dependence, OH, H<sub>2</sub>O<sub>2</sub> and chlorine. Aqueous chemistry includes both oxidation and reduction of Hg(0). Transport and deposition of mercury species are calculated through adapting the original formulations in CAM-Chem. The CAM-Chem model with mercury is driven by present meteorology to simulate the present mercury air quality during the 1999–2001 period. The resulting surface concentrations of total gaseous mercury (TGM) are then compared with the observations from worldwide sites. Simulated wet depositions of mercury over the continental United States are compared to the observations from 26 Mercury Deposition Network stations to test the wet deposition simulations. The evaluations of gaseous concentrations and wet deposition confirm a strong capability for the CAM-Chem mercury mechanism to simulate the atmospheric mercury cycle. The general reproduction of global TGM concentrations and the overestimation on South Africa indicate that model simulations of TGM are seriously affected by emissions. The comparison to wet deposition indicates that wet deposition patterns of mercury are more affected by the spatial variability of precipitation. The sensitivity experiments show that 22% of total mercury deposition and 25% of TGM concentrations in the United States result from domestic anthropogenic sources, but only 9% of total mercury deposition and 7% of TGM concentrations are contributed by transpacific transport. However, the contributions of domestic and transpacific sources on the western United States levels of mercury are of comparable magnitude.
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Recently, a new Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm was developed for the MODerate Resolution Imaging Spectroradiometer (MODIS), which provides aerosol optical depth (AOD) at 1 km resolution. The relationship between MAIAC AOD and PM<sub>2.5</sub> as measured by 84 EPA ground monitoring stations in the entire New England and the Harvard super site during 2002–2008 was investigated and also compared to the AOD–PM<sub>2.5</sub> relationship using conventional MODIS 10 km AOD retrieval from Aqua platform (MYD04) for the same days and locations. The correlations for MYD04 and for MAIAC are <i>r</i> = 0.62 and 0.65, respectively, suggesting that AOD is a reasonable proxy for PM<sub>2.5</sub> ground concentrations. The slightly higher correlation coefficient (<i>r</i>) for MAIAC can be related to its finer resolution resulting in better correspondence between AOD and EPA monitoring sites. Regardless of resolution, AOD–PM<sub>2.5</sub> relationship varies daily, and under certain conditions it can be negative (due to several factors such as an EPA site location (proximity to road) and the lack of information about the aerosol vertical profile). By investigating MAIAC AOD data, we found a substantial increase, by 50–70% in the number of collocated AOD–PM<sub>2.5</sub> pairs, as compared to MYD04, suggesting that MAIAC AOD data are more capable in capturing spatial patterns of PM<sub>2.5</sub>. Importantly, the performance of MAIAC AOD retrievals is slightly degraded but remains reliable under partly cloudy conditions when MYD04 data are not available, and it can be used to increase significantly the number of days for PM<sub>2.5</sub> spatial pattern prediction based on satellite observations.
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Aircraft at cruise levels can cause two kinds of contrails, the well known exhaust contrails and the less well-known aerodynamic contrails. While the possible climate impact of exhaust contrails has been studied for many years, research on aerodynamic contrails began only a few years ago and nothing is known about a possible contribution of these ice clouds to climate impact. In order to make progress in this respect, we first need a climatology of their formation conditions and this is given in the present paper. <br><br> Aerodynamic contrails are defined here as line shaped ice clouds caused by aerodynamically triggered cooling over the wings of an aircraft in cruise which become visible immediately at the trailing edge of the wing or close to it. Effects at low altitudes like condensation to liquid droplets and their potential heterogeneous freezing are excluded from our definition. We study atmospheric conditions that allow formation of aerodynamic contrails. These conditions are stated and then applied to atmospheric data: first to a special case where an aerodynamic contrail was actually observed and then to a full year of global reanalysis data. We show where, when (seasonal variation), and how frequently (probability) aerodynamic contrails can form, and how this relates to actual patterns of air traffic. We study the formation of persistent aerodynamic contrails as well. Furthermore, we check whether aerodynamic and exhaust contrails can coexist in the atmosphere. We show that visible aerodynamic contrails are possible only in an altitude range between roughly 540 and 250 hPa, and that the ambient temperature is the most important parameter, not the relative humidity. Finally, we argue that currently aerodynamic contrails have a much smaller climate effect than exhaust contrails, which may however change in future with more air traffic in the tropics.
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All the representative concentration pathways (RCPs) include declining aerosol emissions during the 21st century, but the effects of these declines on climate projections have had little attention. Here we assess the global and hemispheric-scale effects of declining anthropogenic aerosols in RCP4.5 in CSIRO-Mk3.6, a model from the Coupled Model Intercomparison Project Phase 5 (CMIP5). Results from this model are then compared with those from other CMIP5 models. <br><br> We calculate the aerosol effective radiative forcing (ERF, including indirect effects) in CSIRO-Mk3.6 relative to 1850, using a series of atmospheric simulations with prescribed sea-surface temperatures (SST). Global-mean aerosol ERF at the top of the atmosphere is most negative in 2005 (−1.47 W m<sup>−2</sup>). Between 2005 and 2100 it increases by 1.46 W m<sup>−2</sup>, i.e., it approximately returns to 1850 levels. Although increasing greenhouse gases (GHGs) and declining aerosols both exert a positive ERF at the top of the atmosphere during the 21st century, they have opposing effects on radiative heating of the atmosphere: increasing GHGs warm the atmosphere, whereas declining aerosols cool the atmosphere due to reduced absorption of shortwave radiation by black carbon (BC). <br><br> We then compare two projections for 2006–2100, using the coupled atmosphere-ocean version of the model. One (RCP45) follows the usual RCP4.5; the other (RCP45A2005) has identical forcing, except that emissions of anthropogenic aerosols and precursors are fixed at 2005 levels. The global-mean surface warming in RCP45 is 2.3 °C per 95 yr, of which almost half (1.1 °C) is caused by declining aerosols. The warming due to declining aerosols is almost twice as strong in the Northern Hemisphere as in the Southern Hemisphere, whereas that due to increasing GHGs is similar in the two hemispheres. <br><br> For precipitation changes, the effects of declining aerosols are larger than those of increasing GHGs due to decreasing atmospheric absorption by black carbon: 63% of the projected global-mean precipitation increase of 0.16 mm per day is caused by declining aerosols. In the Northern Hemisphere, precipitation increases by 0.29 mm per day, of which 72% is caused by declining aerosols. <br><br> Comparing 13 CMIP5 models, we find a correlation of –0.54 (significant at 5%) between aerosol ERF in the present climate and projected global-mean surface warming in RCP4.5; thus, models that have more negative aerosol ERF in the present climate tend to project stronger warming during 2006–2100. A similar correlation (–0.56) is found between aerosol ERF and projected changes in global-mean precipitation. <br><br> These results suggest that aerosol forcing substantially modulates projected climate response in RCP4.5. In some respects, the effects of declining aerosols are quite distinct from those of increasing GHGs. Systematic efforts are needed to better quantify the role of declining aerosols in climate projections.
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Deep convective clouds (DCCs) have been widely studied because of their association with heavy precipitation and severe weather events. Changes in the properties of DCCs are likely in a changing climate. Ten years of data collected by Atmospheric Infrared Sounder (AIRS) allow us to identify decadal trends in frequency of occurrence of DCCs over land and ocean. In the past, DCCs have been identified in the thermal infrared by three methods: (1) thresholds based on the absolute value of an atmospheric window channel brightness temperature; (2) thresholds based on the difference between the brightness temperature in an atmospheric window channel and the brightness temperature centered on a strong water vapor absorption line; and (3) a threshold using the difference between the window channel brightness temperature and the tropopause temperature based on climatology. Simultaneous observations of these infrared identified DCCs with the Advanced Microwave Sounding Unit–Humidity Sounder for Brazil (AMSU-HSB) using 183 GHz water channels provide a statistical correlation with microwave deep convection and overshooting convection. In the past 10 years, the frequency of occurrence of DCCs has decreased for the tropical ocean, while it has increased for tropical land. The area of the tropical zone associated with DCCs is typically much less than 1%. We find that the least frequent, more extreme DCCs show the largest trend in frequency of occurrence, increasing over land and decreasing over ocean. <br><br> The trends for land and ocean closely balance, such that the DCC frequency changed at an insignificant rate for the entire tropical zone. This pattern of essentially zero trend for the tropical zone, but opposite land/ocean trends, is consistent with measurements of global precipitation. The changes in frequency of occurrence of the DCCs are correlated with the Niño34 index, which defines the sea surface temperature (SST) anomaly in the east-central Pacific. This is also consistent with patterns seen in global precipitation. This suggests that the observed changes in the frequency are part of a decadal variability characterized by shifts in the main tropical circulation patterns, which does not fully balance in the 10-year AIRS data record. The regional correlations and anti-correlations of the DCC frequency anomaly with the Multivariate ENSO Index (MEI) provide a new perspective for the regional analysis of past events, since the SST anomaly in the Nino34 region is available in the form of the extended MEI from 1871.
