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Satellite observations of cirrus clouds in the Northern Hemisphere lowermost stratosphere

Here we present observations of the Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA) of cirrus cloud and water vapour in August 1997 in the upper troposphere and lower stratosphere (UTLS). The observations indicate a considerable flux of moisture from the upper tropical troposphere into the extratropical lowermost stratosphere (LMS), resulting in the occurrence of high-altitude optically thin cirrus clouds in the LMS. The locations of the LMS cloud events observed by CRISTA are consistent with the tropopause height determined from coinciding radiosonde data. For a hemispheric analysis in tropopause relative coordinates an improved tropopause determination has been applied to the European Centre for Medium-Range Weather Forecasts (ECMWF) temperature profiles. We found that a significant fraction of the cloud occurrences in the tropopause region are located in the LMS, even if a conservative overestimate of the cloud top height (CTH) determination by CRISTA of 500 m is assumed. The results show rather high occurrence frequencies (~ 5%) up to high northern latitudes (70° N) and altitudes well above the tropopause (> 500 m at ~350 K and above) in large areas at mid- and high latitudes. Comparisons with model runs of the Chemical Lagrangian Model of the Stratosphere (CLaMS) over the CRISTA period show a reasonable consistency in the retrieved cloud pattern. For this purpose a limb ray tracing approach was applied through the 3-D model fields to obtain integrated measurement information through the atmosphere along the limb path of the instrument. The simplified cirrus scheme implemented in CLaMS seems to cause a systematic underestimation in the CTH occurrence frequencies in the LMS with respect to the observations. The observations together with the model results demonstrate the importance of isentropic, quasi-horizontal transport of water vapour from the subtropics and the potential for the occurrence of cirrus clouds in the lowermost stratosphere and tropopause region.
Influence of aerosol chemical composition on N2O5 uptake: airborne regional measurements in northwestern Europe

Aerosol chemical composition was found to influence nighttime atmospheric chemistry during a series of airborne measurements in northwestern Europe in summer conditions, which has implications for regional air quality and climate. The uptake of dinitrogen pentoxide, γ (N2O5), to particle surfaces was found to be modulated by the amount of water content and ammonium nitrate present in the aerosol. The conditions prevalent in this study suggest that the net uptake rate of N2O5 to atmospheric aerosols was relatively efficient compared to previous studies, with γ (N2O5) values in the range 0.01–0.03. This is likely a consequence of the elevated relative humidity in the region, which promotes greater aerosol water content. Increased nitrate concentrations relative to particulate water were found to suppress N2O5 uptake. The results presented here contrast with previous ambient studies of N2O5 uptake, which have generally taken place in low-nitrate environments in the USA. Comparison of the N2O5 uptake derived from the measurements with a parameterised scheme that is based on the ratio of particulate water to nitrate yielded reasonably good agreement in terms of the magnitude and variation in uptake, provided the effect of chloride was neglected. An additional suppression of the parameterised uptake is likely required to fully capture the variation in N2O5 uptake, which could be achieved via the known suppression by organic aerosol. However, existing parameterisations representing the suppression by organic aerosol were unable to fully represent the variation in N2O5 uptake. These results provide important ambient measurement constraint on our ability to predict N2O5 uptake in regional and global aerosol models. N2O5 uptake is a potentially important source of nitrate aerosol and a sink of the nitrate radical, which is the main nocturnal oxidant in the atmosphere. The results further highlight the importance of ammonium nitrate in northwestern Europe as a key component of atmospheric composition in the region.
Secondary organic aerosol formation from hydroxyl radical oxidation and ozonolysis of monoterpenes

Oxidation by hydroxyl radical (OH) and ozonolysis are the two major pathways of daytime biogenic volatile organic compound (BVOC) oxidation and secondary organic aerosol (SOA) formation. In this study, we investigated the particle formation of several common monoterpenes (α-pinene, β-pinene and limonene) by OH-dominated oxidation, which has seldom been investigated. OH oxidation experiments were carried out in the SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction) chamber in Jülich, Germany, at low NOx (0.01 ~ 1 ppbV) and low ozone (O3) concentration (< 20 ppbV). OH concentration and total OH reactivity (kOH) were measured directly, and through this the overall reaction rate of total organics with OH in each reaction system was quantified. Multi-generation reaction process, particle growth, new particle formation (NPF), particle yield and chemical composition were analyzed and compared with that of monoterpene ozonolysis. Multi-generation products were found to be important in OH-dominated SOA formation. The relative role of functionalization and fragmentation in the reaction process of OH oxidation was analyzed by examining the particle mass and the particle size as a function of OH dose. We developed a novel method which quantitatively links particle growth to the reaction rate of OH with total organics in a reaction system. This method was also used to analyze the evolution of functionalization and fragmentation of organics in the particle formation by OH oxidation. It shows that functionalization of organics was dominant in the beginning of the reaction (within two lifetimes of the monoterpene) and fragmentation started to play an important role after that. We compared particle formation from OH oxidation with that from pure ozonolysis. In individual experiments, growth rates of the particle size did not necessarily correlate with the reaction rate of monoterpene with OH and O3. Comparing the size growth rates at the similar reaction rates of monoterpene with OH or O3 indicates that, generally, OH oxidation and ozonolysis had similar efficiency in particle growth. The SOA yield of α-pinene and limonene by ozonolysis was higher than that of OH oxidation. Aerosol mass spectrometry (AMS) shows SOA elemental composition from OH oxidation follows a slope shallower than −1 in the O / C vs. H / C diagram, also known as Van Krevelen diagram, indicating that oxidation proceeds without significant loss of hydrogen. SOA from OH oxidation had higher H / C ratios than SOA from ozonolysis. In ozonolysis, a process with significant hydrogen loss seemed to play an important role in SOA formation.
Atmospheric wet and dry deposition of trace elements at 10 sites in Northern China

Atmospheric deposition is considered to be a major process that removes pollutants from the atmosphere and an important source of nutrients and contaminants for ecosystems. Trace elements (TEs), especially toxic metals deposited on plants and into soil or water, can cause substantial damage to the environment and human health due to their transfer and accumulation in food chains. Despite public concerns, quantitative knowledge of metal deposition from the atmosphere to ecosystems remains scarce. To advance our understanding of the spatiotemporal variations in the magnitudes, pathways, compositions and impacts of atmospherically deposited TEs, precipitation (rain and snow) and dry-deposited particles were collected simultaneously at 10 sites in Northern China from December 2007 to November 2010. The measurements showed that the wet and dry depositions of TEs in the target areas were orders of magnitude higher than previous observations within and outside China, generating great concern over the potential risks. The spatial distribution of the total (wet plus dry) deposition flux was consistent with that of the dry deposition, with a significant decrease from industrial and urban areas to suburban, agricultural and rural sites, while the wet deposition exhibited less spatial variation. In addition, the seasonal variation of wet deposition was also different from that of dry deposition, although they were both governed by the precipitation and emission patterns. For the majority of TEs that exist as coarse particles, dry deposition dominated the total flux at each site. This was not the case for potassium, nickel, arsenic, lead, zinc, cadmium, selenium, silver and thallium, for which the relative importance between wet and dry deposition fluxes varied by site. Whether wet deposition is the major atmospheric cleansing mechanism for the TEs depends on the size distribution of the particles. We found that atmospheric inputs of copper, lead, zinc, cadmium, arsenic and selenium were of the same magnitude as their increases in the topsoil of agricultural systems. At a background forest site in Northern China, the total deposition flux of lead observed in this study (14.1 mg m−2 yr−1) was twice that of the critical load calculated for temperate forest ecosystems in Europe. These findings provide baseline data needed for future targeting policies to protect various ecosystems from long-term heavy metal input via atmospheric deposition.
Correlation slopes of GEM / CO, GEM / CO2, and GEM / CH4 and estimated mercury emissions in China, South Asia, the Indochinese Peninsula, and Central Asia derived from observations in northwestern and southwestern China

Correlation analyses between atmospheric mercury (Hg) and other trace gases are useful for identification of sources and constraining regional Hg emissions. Emissions of Hg in Asia contribute significantly to the global budget of atmospheric Hg. However, due to the lack of reliable data on the source strength, large uncertainties remain in the emission inventories of Hg in Asia. In the present study, we calculated the correlation slopes of GEM / CO, GEM / CO2, and GEM / CH4 for mainland China, South Asia, the Indochinese Peninsula, and Central Asia using the ground-based observations at three remote sites in northwestern and southwestern China, and applied these values to estimate GEM emissions in the four source regions. The geometric mean GEM / CO correlation slopes for mainland China, South Asia, the Indochinese Peninsula, and Central Asia were 7.3 ± 4.3, 7.8 ± 6.4, 7.8 ± 5.0, and 13.4 ± 9.5 pg m−3 ppb−1, respectively, and values in the same source regions were 33.3 ± 30.4, 27.4 ± 31.0, 23.5 ± 15.3, and 20.5 ± 10.0 pg m−3 ppb−1 for the GEM / CH4 correlation slopes, respectively. The geometric means of GEM / CO2 correlation slopes for mainland China, South Asia, and Central Asia were 240 ± 119, 278 ± 164, 315 ± 289 pg m−3 ppm−1, respectively. These values were the first reported correlation slopes of GEM / CO, GEM / CO2, and GEM / CH4 in four important source regions of Asia, not including the GEM / CO ratios in mainland China. The correlation slopes of GEM / CO, GEM / CO2, and GEM / CH4 in Asia were relatively higher than those observed in Europe, North America, and South Africa, which may highlight GEM emissions from non-ferrous smelting, large-scale and artisanal mercury and gold production, natural sources, and historically deposited mercury (re-emission) in Asia. Using the observed GEM / CO and GEM / CO2 slopes, and the recently reported emission inventories of CO and CO2, the annual GEM emissions in mainland China, South Asia, the Indochinese Peninsula, and Central Asia were estimated to be in the ranges of 1071–1187, 340–470, 125, and 54–90 t, respectively. The estimated quantity of GEM emissions from the GEM / CH4 correlation slopes is significantly larger, which may be due to the larger uncertainties in CH4 emissions in Asia as well as insufficient observations of GEM / CH4 correlation slopes, therefore leading to an overestimate of GEM emissions. Our estimates of GEM emissions in the four Asian regions were significantly higher (3–4 times) than the anthropogenic GEM emissions reported in recent studies. This discrepancy could come from a combination of reasons including underestimates of anthropogenic and natural GEM emissions; large uncertainties related to CO, CO2, and CH4 emission inventories; and inherent limitations of the correlation slope method.
Joint analysis of continental and regional background environments in the western Mediterranean: PM1 and PM10 concentrations and composition

The complete chemical composition of atmospheric particulate matter (PM1 and PM10) from a continental (Montsec, MSC, 1570 m a.s.l.) and a regional (Montseny, MSY, 720 m a.s.l) background site in the western Mediterranean Basin (WMB) were jointly studied for the first time over a relatively long-term period (January 2010–March 2013). Differences in average PMX concentration and composition between both sites were attributed to distance to anthropogenic sources, altitude, and different influence of atmospheric episodes. All these factors result in a continental-to-regional background increase of 4.0 μg m−3 for PM10 and 1.1 μg m−3 for PM1 in the WMB. This increase is mainly constituted by organic matter, sulfate, nitrate, and sea salt. However, higher mineral matter concentrations were measured at the continental background site owing to the higher influence of long-range transport of dust and dust resuspension. Seasonal variations of aerosol chemical components were attributed to evolution of the planetary boundary layer (PBL) height throughout the year, variations in the air mass origin, and differences in meteorology. During warmer months, weak pressure gradients and elevated insolation generate recirculation of air masses and enhance the development of the PBL, causing the aging of aerosols and incrementing pollutant concentrations over a large area in the WMB, including the continental background. This is reflected in a more similar relative composition and absolute concentrations of continental and regional background aerosols. Nevertheless, during colder months the thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the time, whereas MSY is more influenced by regional pollutants accumulated under winter anticyclonic conditions. This results in much lower concentrations of PMX components at the continental background site with respect to those at the regional background site. The influence of certain atmospheric episodes caused different impacts at regional and continental scales. When long-range transport from central and eastern Europe and from north Africa occurs, the continental background site is frequently more influenced, thus indicating a preferential transport of pollutants at high altitude layers. Conversely, the regional background site was more influenced by regional processes. Continental and regional aerosol chemical composition from the WMB revealed (a) high relevance of African dust transport and regional dust resuspension; (b) low biomass burning contribution; (c) high organic matter contribution; (d) low summer nitrate concentrations; and (e) high aerosol homogenization in summer.
Inclusion of mountain-wave-induced cooling for the formation of PSCs over the Antarctic Peninsula in a chemistry–climate model

An important source of polar stratospheric clouds (PSCs), which play a crucial role in controlling polar stratospheric ozone depletion, is from the temperature fluctuations induced by mountain waves. However, this formation mechanism is usually missing in chemistry–climate models because these temperature fluctuations are neither resolved nor parameterised. Here, we investigate the representation of stratospheric mountain-wave-induced temperature fluctuations by the UK Met Office Unified Model (UM) at climate scale and mesoscale against Atmospheric Infrared Sounder satellite observations for three case studies over the Antarctic Peninsula. At a high horizontal resolution (4 km) the regional mesoscale configuration of the UM correctly simulates the magnitude, timing, and location of the measured temperature fluctuations. By comparison, at a low horizontal resolution (2.5° × 3.75°) the global climate configuration fails to resolve such disturbances. However, it is demonstrated that the temperature fluctuations computed by a mountain wave parameterisation scheme inserted into the climate configuration (which computes the temperature fluctuations due to unresolved mountain waves) are in relatively good agreement with the mesoscale configuration responses for two of the three case studies. The parameterisation was used to include the simulation of mountain-wave-induced PSCs in the global chemistry–climate configuration of the UM. A subsequent sensitivity study demonstrated that regional PSCs increased by up to 50% during July over the Antarctic Peninsula following the inclusion of the local mountain-wave-induced cooling phase.
On the relationship between the scattering phase function of cirrus and the atmospheric state

This is the first paper to investigate the relationship between the shape of the scattering phase function of cirrus and the relative humidity with respect to ice (RHi, using space-based solar radiometric angle-dependent measurements. The relationship between RHi and the complexity of ice crystals has been previously studied using data from aircraft field campaigns and laboratory cloud chambers. However, to the best of our knowledge, there have been no studies to date that explore this relationship through the use of remotely sensed space-based angle-dependent solar radiometric measurements. In this paper, one case study of semi-transparent cirrus, which occurred on 25 January 2010 off the north-east coast of Scotland, is used to explore the possibility of such a relationship. Moreover, for the first time, RHi fields predicted by a high-resolution numerical weather prediction (NWP) model are combined with satellite retrievals of ice crystal complexity. The NWP model was initialised at midnight, on 25 January 2010, and the mid-latitude RHi field was extracted from the NWP model at 13:00 UTC. At about the same time, there was a PARASOL (Polarization and Anisotropy of Reflectance for Atmospheric science coupled with Observations from a Lidar) overpass, and the PARASOL swath covered the NWP-model-predicted RHi field. The cirrus case was located over Scotland and the North Sea. From the satellite channel based at 0.865 μm, the directionally averaged and directional spherical albedos were retrieved between the scattering angles of about 80 and 130°. An ensemble model of cirrus ice crystals is used to predict phase functions that vary between phase functions that exhibit optical features (referred to as pristine) and featureless phase functions. For each of the PARASOL pixels, the phase function that best minimised differences between the spherical albedos was selected. This paper reports, for this one case study, an association between the most featureless phase function model and the highest values of NWP-predicted RHi (i.e. when RHi > 1.0). For pixels associated with NWP-model-predicted RHi < 1, it was impossible to generally discriminate between phase function models at the 5% significance level. It is also shown that the NWP model prediction of the vertical profile of RHi is in good agreement with dropsonde, in situ measurements and independent aircraft-based physical retrievals of RHi. Furthermore, the NWP model prediction of the cirrus cloud-top height and its vertical extent is also found to be in good agreement with aircraft-based lidar measurements.
A regional carbon data assimilation system and its preliminary evaluation in East Asia

In order to optimize surface CO2 fluxes at grid scales, a regional surface CO2 flux inversion system (Carbon Flux Inversion system and Community Multi-scale Air Quality, CFI-CMAQ) has been developed by applying the ensemble Kalman filter (EnKF) to constrain the CO2 concentrations and applying the ensemble Kalman smoother (EnKS) to optimize the surface CO2 fluxes. The smoothing operator is associated with the atmospheric transport model to constitute a persistence dynamical model to forecast the surface CO2 flux scaling factors. In this implementation, the "signal-to-noise" problem can be avoided; plus, any useful observed information achieved by the current assimilation cycle can be transferred into the next assimilation cycle. Thus, the surface CO2 fluxes can be optimized as a whole at the grid scale in CFI-CMAQ. The performance of CFI-CMAQ was quantitatively evaluated through a set of Observing System Simulation Experiments (OSSEs) by assimilating CO2 retrievals from GOSAT (Greenhouse Gases Observing Satellite). The results showed that the CO2 concentration assimilation using EnKF could constrain the CO2 concentration effectively, illustrating that the simultaneous assimilation of CO2 concentrations can provide convincing CO2 initial analysis fields for CO2 flux inversion. In addition, the CO2 flux optimization using EnKS demonstrated that CFI-CMAQ could, in general, reproduce true fluxes at grid scales with acceptable bias. Two further sets of numerical experiments were conducted to investigate the sensitivities of the inflation factor of scaling factors and the smoother window. The results showed that the ability of CFI-CMAQ to optimize CO2 fluxes greatly relied on the choice of the inflation factor. However, the smoother window had a slight influence on the optimized results. CFI-CMAQ performed very well even with a short lag-window (e.g. 3 days).
Carbonaceous aerosols recorded in a southeastern Tibetan glacier: analysis of temporal variations and model estimates of sources and radiative forcing

High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956–2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of BC and OC with higher respective concentrations but a lower OC / BC ratio in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source–receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia has the largest contribution to the present-day (1996–2005) mean BC deposition at the ice-core drilling site during the non-monsoon season (October to May) (81%) and all year round (74%), followed by East Asia (14% to the non-monsoon mean and 21% to the annual mean). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from the late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia (as the primary contributor to annual mean BC deposition). Moreover, the increasing trend of the OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and/or biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing potential influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice-core record.