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Comparison of ice cloud properties simulated by the Community Atmosphere Model (CAM5) with in-situ observations

Detailed measurements of ice crystals in cirrus clouds were used to compare with results from the Community Atmospheric Model Version 5 (CAM5) global climate model. The observations are from two different field campaigns with contrasting conditions: Atmospheric Radiation Measurements Spring Cloud Intensive Operational Period in 2000 (ARM-IOP), which was characterized primarily by midlatitude frontal clouds and cirrus, and Tropical Composition, Cloud and Climate Coupling (TC4), which was dominated by anvil cirrus. Results show that the model typically overestimates the slope parameter of the exponential size distributions of cloud ice and snow, while the variation with temperature (height) is comparable. The model also overestimates the ice/snow number concentration (0th moment of the size distribution) and underestimates higher moments (2nd through 5th), but compares well with observations for the 1st moment. Overall the model shows better agreement with observations for TC4 than for ARM-IOP in regards to the moments. The mass-weighted terminal fall speed is lower in the model compared to observations for both ARM-IOP and TC4, which is partly due to the overestimation of the size distribution slope parameter. Sensitivity tests with modification of the threshold size for cloud ice to snow autoconversion (Dcs) do not show noticeable improvement in modeled moments, slope parameter and mass weighed fall speed compared to observations. Further, there is considerable sensitivity of the cloud radiative forcing to Dcs, consistent with previous studies, but no value of Dcs improves modeled cloud radiative forcing compared to measurements. Since the autoconversion of cloud ice to snow using the threshold size Dcs has little physical basis, future improvement to combine cloud ice and snow into a single category, eliminating the need for autoconversion, is suggested.
Chemical mass balance of 300 °C non-volatile particles at the tropospheric research site Melpitz, Germany

In the fine-particle mode (aerodynamic diameter < 1 μm) non-volatile material has been associated with black carbon (BC) and low-volatile organics and, to a lesser extent, with sea salt and mineral dust. This work analyzes non-volatile particles at the tropospheric research station Melpitz (Germany), combining experimental methods such as a mobility particle-size spectrometer (3–800 nm), a thermodenuder operating at 300 °C, a multi-angle absorption photometer (MAAP), and an aerosol mass spectrometer (AMS). The data were collected during two atmospheric field experiments in May–June 2008 as well as February–March 2009. As a basic result, we detected average non-volatile particle–volume fractions of 11 ± 3% (2008) and 17 ± 8% (2009). In both periods, BC was in close linear correlation with the non-volatile fraction, but not sufficient to quantitatively explain the non-volatile particle mass concentration. Based on the assumption that BC is not altered by the heating process, the non-volatile particle mass fraction could be explained by the sum of black carbon (47% in summer, 59% in winter) and a non-volatile organic contribution estimated as part of the low-volatility oxygenated organic aerosol (LV-OOA) (53% in summer, 41% in winter); the latter was identified from AMS data by factor analysis. Our results suggest that LV-OOA was more volatile in summer (May–June 2008) than in winter (February–March 2009) which was linked to a difference in oxidation levels (lower in summer). Although carbonaceous compounds dominated the sub-μm non-volatile particle mass fraction most of the time, a cross-sensitivity to partially volatile aerosol particles of maritime origin could be seen. These marine particles could be distinguished, however from the carbonaceous particles by a characteristic particle volume–size distribution. The paper discusses the uncertainty of the volatility measurements and outlines the possible merits of volatility analysis as part of continuous atmospheric aerosol measurements.
On the impact of the temporal variability of the collisional quenching process on the mesospheric OH emission layer: a study based on SD-WACCM4 and SABER

The mesospheric OH Meinel emissions are subject of many theoretical and observational studies devoted to this part of the atmosphere. Depending on the initial vibrational level of excitation the altitude of the considered OH Meinel emission is systematically shifted, which has important implications for the intercomparison of different studies considering different transition bands. Previous model studies suggest that these vertical shifts are essentially caused by the process of collisional quenching with atomic oxygen. Following this hypothesis, a recent study found experimental evidence of a coherent seasonality at tropical latitudes between vertical shifts of different OH Meinel bands and changes in atomic oxygen concentrations. Despite the consistent finding of the above mentioned hypothesis, it cannot be excluded that the actual temporal variability of the vertical shifts between different OH Meinel bands may in addition be controlled or even dominated by other processes. It remains an open question whether the observed temporal evolution is indeed mainly controlled by the modulation of the collisional quenching process with atomic oxygen. By means of a sensitivity study which employs a quenching model to simulations made with the SD-WACCM4 chemistry climate model, we aim at assessing this question. From this study we find that the observed seasonality of vertical OH Meinel shifts is only partially controlled by temporal changes in atomic oxygen concentrations, while molecular oxygen has another noticeable impact on the vertical OH Meinel shifts. This in particular becomes evident for the diurnal variability of vertical OH Meinel shifts, which reveal only a poor correlation with the atomic oxygen species. Furthermore, changes in the H + O3 source gases provide another mechanism that can potentially affect the diurnal variability in addition. By comparison with limb radiance observations from the SABER/TIMED satellite this provides an explanation for the less evident diurnal response between changes in O concentrations and vertical OH Meinel shifts. On the other hand, at seasonal timescales the coherency between both quantities is again evident in SABER/TIMED but less pronounced compared to our model simulations.
Intercontinental transport and deposition patterns of atmospheric mercury from anthropogenic emissions

Global policies that regulate anthropogenic mercury emissions to the environment require quantitative and comprehensive source–receptor relationships for mercury emissions, transport and deposition among major continental regions. In this study, we use the GEOS-Chem global chemical transport model to establish source–receptor relationships among 11 major continental regions worldwide. Source–receptor relationships for surface mercury concentrations (SMC) show that some regions (e.g., East Asia, the Indian subcontinent, and Europe) should be responsible for their local surface Hg(II) and Hg(P) concentrations due to near-field transport and deposition contributions from their local anthropogenic emissions (up to 64 and 71% for Hg(II) and Hg(P), respectively, over East Asia). We define the region of primary influence (RPI) and the region of secondary influence (RSI) to establish intercontinental influence patterns. Results indicate that East Asia is the SMC RPI for almost all other regions, while Europe, Russia, and the Indian subcontinent also make some contributions to SMC over some receptor regions because they are dominant RSI source regions. Source–receptor relationships for mercury deposition show that approximately 16 and 17% of dry and wet deposition, respectively, over North America originate from East Asia, indicating that transpacific transport of East Asian emissions is the major foreign source of mercury deposition in North America. Europe, Southeast Asia, and the Indian subcontinent are also important mercury deposition sources for some receptor regions because they are the dominant RSIs. We also quantify seasonal variation on mercury deposition contributions over other regions from East Asia. Results show that mercury deposition (including dry and wet) contributions from East Asia over the Northern Hemisphere receptor regions (e.g., North America, Europe, Russia, the Middle East, and Middle Asia) vary seasonally, with the maximum values in summer and minimum values in winter. The opposite seasonal pattern occurs on mercury dry deposition contributions over Southeast Asia and the Indian subcontinent.
Modeling analysis of the seasonal characteristics of haze formation in Beijing

The air quality modeling system RAMS-CMAQ (Regional Atmospheric Modeling System–Community Multiscale Air Quality), coupled with an aerosol optical property scheme, was applied to simulate the meteorological field, major aerosol components (sulfate, nitrate, ammonium, black carbon, organic carbon, dust, and sea salt), and surface visibility over the North China Plain (NCP) in 2011. The modeled results in February and July 2011 were selected and analyzed to obtain an in-depth understanding of the haze formation mechanism in Beijing for different seasons. The simulation results showed that the visibility was below 10 km for most regions of the NCP, and dropped to less than 5 km over the megacities of Beijing and Tianjin, the whole of Hebei Province, and the northwest part of Shandong Province during pollution episodes in February and July. The heavy mass concentration of PM2.5 ranged from 120 to 300 μg m−3 and was concentrated in the areas with low visibility. The haze formation mechanism in Beijing in winter was different from that in summer. The mass concentration of PM2.5 was higher, and the components more complicated, in winter. While the mass concentration of PM2.5 in summer was lower than that in winter, the mass concentrations of hygroscopic inorganic salts were comparable with those in winter, and the relative humidity was, as expected, higher. Therefore, the water uptake of hygroscopic aerosols played a key role in summer. Moreover, the analysis showed that the influence of the PM2.5 mass burden on visibility was very weak when its value was larger than 100 μg m−3. Only when the mass burden of PM2.5 decreased to a certain threshold interval did the visibility increase rapidly. This indicates that, when emission reduction measures are taken to control haze occurrence, the mass burden of PM2.5 must be cut to below this threshold interval. The relationship between the threshold of haze occurrence and the relative humidity in Beijing was fitted by an exponential function, and the resulting fitting curves could provide a new theoretical basis to understand and control haze formation in Beijing.
Horizontal distributions of aerosol constituents and their mixing states in Antarctica during the JASE traverse

Measurements of aerosol number concentrations and direct aerosol sampling were conducted on continental Antarctica during the traverse of the Japanese–Swedish joint Antarctic expedition (JASE) from 14 November 2007 until 24 January 2008. Aerosol concentrations in background conditions decreased gradually with latitude in inland regions during the traverse. The lowest aerosol number concentrations were 160 L−1 in Dp > 0.3 μm, and 0.5 L−1 in Dp 2 μm. In contrast, aerosol concentrations reached 3278 L−1 in Dp > 0.3 μm, and 215 L−1 in Dp > 2 μm under strong wind conditions. The estimated aerosol mass concentrations were 0.04–5.7 μg m−3. Single particle analysis of aerosol particles collected during the JASE traverse was conducted using a scanning electron microscope equipped with an energy dispersive x ray spectrometer. Major aerosol constituents were sulfates in fine mode, and sulfate, sea salts, modified sea salts, and fractionated sea salts in coarse mode. K-rich sulfates, Mg-rich sulfate, Ca-rich sulfates, and minerals were identified as minor aerosol constituents. Horizontal features of Cl / Na ratios imply that sea-salt modification (i.e. Cl loss) occurred on the Antarctic continent during the summer. Most sea-salt particles in the continental region near the coast were modified with acidic sulfur species such as H2SO4 and CH3SO3H. By contrast, acidic species other than the acidic sulfur species (likely HNO3) contributed markedly to sea-salt modification in inland areas during the traverse. Mg-rich sea-salt particles and Mg-free sea-salt particles were present in coarse and fine modes from the coast to inland areas. These sea-salt particles might be associated with sea-salt fractionation on the snow surface of continental Antarctica.
Submicron aerosols at thirteen diversified sites in China: size distribution, new particle formation and corresponding contribution to cloud condensation nuclei production

Understanding the particle number size distributions in diversified atmospheric environments is important in order to design mitigation strategies related to submicron particles and their effects on regional air quality, haze and human health. In this study, we conducted 15 different field measurement campaigns between 2007 and 2011 at 13 individual sites in China, including five urban sites, four regional sites, three coastal/background sites and one ship cruise measurement along eastern coastline of China. Size resolved particles were measured in the 15–600 nm size range. The median particle number concentrations (PNCs) were found to vary in the range of 1.1−2.2 × 104 cm−3 at urban sites, 0.8−1.5 × 104 cm−3 at regional sites, 0.4−0.6 × 104 cm−3 at coastal/background sites, and 0.5 × 104 cm−3 during cruise measurement. Peak diameters at each of these sites varied greatly from 24 to 115 nm. Particles in the 15–25 nm (nucleation mode), 25–100 nm (Aitken mode) and 100–600 nm (accumulation mode) range showed different characteristics at each sites, indicating the features of primary emissions and secondary formation in these diversified atmospheric environments. Diurnal variations show a build-up of accumulation mode particles belt at regional sites, suggesting the contribution of regional secondary aerosol pollution. Frequencies of new particle formation (NPF) events were much higher at urban and regional sites than at coastal sites and during cruise measurement. The average growth rates (GRs) of nucleation mode particles were 8.0–10.9 nm h−1 at urban sites, 7.4–13.6 nm h−1 at regional sites and 2.8–7.5 nm h−1 at coastal sites and during cruise measurement. The high gaseous precursors and strong oxidation at urban and regional sites not only favored the formation of particles, but also accelerated the growth rate of the nucleation mode particles. No significant difference in condensation sink (CS) during NPF days were observed among different site types, suggesting that the NPF events in background areas were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal sites and during cruise measurement had little impact on potential production of CCN. This study provides a large data set of particle size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particle formation and corresponding CCN activity of submicron aerosols in Chinese environments.
Size-resolved cloud condensation nuclei (CCN) activity and closure analysis at the HKUST Supersite in Hong Kong

The cloud condensation nuclei (CCN) properties of atmospheric aerosols were measured on 1–30 May 2011 at the HKUST (Hong Kong University of Science and Technology) Supersite, a coastal site in Hong Kong. Size-resolved CCN activation curves, the ratio of number concentration of CCN (NCCN) to aerosol concentration (NCN) as a function of particle size, were obtained at supersaturation (SS) = 0.15, 0.35, 0.50, and 0.70% using a DMT (Droplet Measurement Technologies) CCN counter (CCNc) and a TSI scanning mobility particle sizer (SMPS). The mean bulk size-integrated NCCN ranged from ~500 cm−3 at SS = 0.15% to ~2100 cm−3 at SS = 0.70%, and the mean bulk NCCN / NCN ratio ranged from 0.16 at SS = 0.15% to 0.65 at SS = 0.70%. The average critical mobility diameters (D50) at SS = 0.15, 0.35, 0.50, and 0.70% were 116, 67, 56, and 46 nm, respectively. The corresponding average hygroscopic parameters (κCCN) were 0.39, 0.36, 0.31, and 0.28. The decrease in κCCN can be attributed to the increase in organic to inorganic volume ratio as particle size decreases, as measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The κCCN correlates reasonably well with κAMS_SR based on size-resolved AMS measurements: κAMS_SR = κorg × forg + κinorg × finorg, where forg and finorg are the organic and inorganic volume fractions, respectively, κorg = 0.1 and κinorg = 0.6, with a R2 of 0.51. In closure analysis, NCCN was estimated by integrating the measured size-resolved NCN for particles larger than D50 derived from κ assuming internal mixing state. Estimates using κAMS_SR show that the measured and predicted NCCN were generally within 10% of each other at all four SS. The deviation increased to 26% when κAMS was calculated from bulk PM1 AMS measurements of particles because PM1 was dominated by particles of 200 to 500 nm in diameter, which had a larger inorganic fraction than those of D50 (particle diameter < 200 nm). A constant κ = 0.33 (the average value of κAMS_SR over the course of campaign) was found to give an NCCN prediction within 12% of the actual measured values. We also compared NCCN estimates based on the measured average D50 and the average size-resolved CCN activation ratio to examine the relative importance of hygroscopicity and mixing state. NCCN appears to be relatively more sensitive to the mixing state and hygroscopicity at a high SS = 0.70% and a low SS = 0.15%, respectively.
Linking climate and air quality over Europe: effects of meteorology on PM2.5 concentrations

The effects of various meteorological parameters such as temperature, wind speed, absolute humidity, precipitation and mixing height on PM2.5 concentrations over Europe were examined using a three-dimensional chemical transport model, PMCAMx-2008. Our simulations covered three periods, representative of different seasons (summer, winter, and fall). PM2.5 appears to be more sensitive to temperature changes compared to the other meteorological parameters in all seasons. PM2.5 generally decreases as temperature increases, although the predicted changes vary significantly in space and time, ranging from −700 ng m−3 K−1 (−8% K−1) to 300 ng m−3 K−1 (7% K−1). The predicted decreases of PM2.5 are mainly due to evaporation of ammonium nitrate, while the higher biogenic emissions and the accelerated gas-phase reaction rates increase the production of organic aerosol (OA) and sulfate, having the opposite effect on PM2.5. The predicted responses of PM2.5 to absolute humidity are also quite variable, ranging from −130 ng m−3 %−1 (−1.6% %−1) to 160 ng m−3 %−1 (1.6% %−1) dominated mainly by changes in inorganic PM2.5 species. An increase in absolute humidity favors the partitioning of nitrate to the aerosol phase and increases the average PM2.5 during summer and fall. Decreases in sulfate and sea salt levels govern the average PM2.5 response to humidity during winter. A decrease of wind speed (keeping the emissions constant) increases all PM2.5 species (on average 40 ng m−3 %−1) due to changes in dispersion and dry deposition. The wind speed effects on sea salt emissions are significant for PM2.5 concentrations over water and in coastal areas. Increases in precipitation have a negative effect on PM2.5 (decreases up to 110 ng m−3 %−1) in all periods due to increases in wet deposition of PM2.5 species and their gas precursors. Changes in mixing height have the smallest effects (up to 35 ng m−3 %−1) on PM2.5 . Regarding the relative importance of each of the meteorological parameters in a changed future climate, the projected changes in precipitation are expected to have the largest impact on PM2.5 levels during all periods (changes up to 2 μg m−3 in the fall). The expected effects in future PM2.5 levels due to wind speed changes are similar in all seasons and quite close to those resulting from future precipitation changes (up to 1.4 μg m−3). The expected increases in absolute humidity in the future can lead to large changes in PM2.5 levels (increases up to 2 μg m−3) mainly in the fall due to changes in particulate nitrate levels. Despite the high sensitivity of PM2.5 levels to temperature, the small expected increases of temperature in the future will lead to modest PM2.5 changes and will not dominate the overall change.
The balances of mixing ratios and segregation intensity: a case study from the field (ECHO 2003)

An inhomogeneous mixing of reactants causes a reduction of their chemical removal compared to the homogeneously mixed case in turbulent atmospheric flows. This can be described by the intensity of segregation IS being the covariance of the mixing ratios of two species divided by the product of their means. Both terms appear in the balance equation of the mixing ratio and are discussed for the reaction between isoprene and OH for data of the field study ECHO 2003 above a deciduous forest. For most of these data, IS is negatively correlated with the fraction of mean OH mixing ratio reacting with isoprene. IS is also negatively correlated with the isoprene standard deviation. Both findings agree with model results discussed by Patton et al. (2001) and others. The correlation coefficient between OH and isoprene and, therefore, IS increases with increasing mean reaction rate. In addition, the balance equation of the covariance between isoprene and OH is applied as the theoretical framework for the analysis of the same field data. The storage term is small, and, therefore, a diagnostic equation for this covariance can be derived. The chemical reaction term Rij is dominated by the variance of isoprene times the quotient of mixing ratios of OH and isoprene. Based on these findings a new diagnostic equation for IS is formulated. Comparing different terms of this equation, IS and Rij show a relation also to the normalised isoprene standard deviation. It is shown that not only chemistry but also turbulent and convective mixing and advection – considered in a residual term – influence IS. Despite this finding, a detection of the influence of coherent eddy transport above the forest according to Katul et al. (1997) on IS fails, but a relation to the turbulent and advective transport of isoprene variance is determined. The largest values of IS are found for most unstable conditions with increasing buoyant production, confirming qualitatively model predictions by Ouwersloot et al. (2011).