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The effects of aerosols on water cloud microphysics and macrophysics based on satellite-retrieved data over East Asia and the North Pacific

This study examines the characteristics of the microphysics and macrophysics of water clouds from East Asia to the North Pacific, using data from active CloudSat radar measurements and passive MODerate-resolution Imaging Spectroradiometer (MODIS) retrievals. Our goals are to clarify differences in microphysics and macrophysics between land and oceanic clouds, seasonal differences unique to the midlatitudes, characteristics of the drizzling process, and cloud vertical structure. In pristine oceanic areas, fractional occurrences of cloud optical thickness (COT) and cloud droplet effective radius (CDR) increase systematically with an increase in drizzle intensity, but these characteristics of the COT and CDR transition are less evident in polluted land areas. In addition, regional and seasonal differences are identified in terms of drizzle intensity as a function of the liquid water path (LWP) and cloud droplet number concentration (Nc). The correlations between drizzle intensity and LWP, and between drizzle intensity and Nc, are both more robust over oceanic areas than over land areas. We also demonstrate regional and seasonal characteristics of the cloud vertical structure. Our results suggest that aerosol–cloud interaction mainly occurs around the cloud base in polluted land areas during the winter season. In addition, a difference between polluted and pristine areas in the efficiency of cloud droplet growth is confirmed. These results suggest that water clouds over the midlatitudes exhibit a different drizzle system to those over the tropics.
Forest canopy interactions with nucleation mode particles

Ultrafine particle size distributions through a deciduous forest canopy indicate that nucleation mode particle concentrations decline with depth into the canopy, such that number concentrations at the bottom of the canopy are an average of 16% lower than those at the top. However, growth rates of nucleation mode particles (diameters 6–30 nm) are invariant with height within the canopy, which implies that the semi-volatile gases contributing to their growth are comparatively well-mixed through the canopy. Growth rates of nucleation mode particles during a meteorological drought year (2012) were substantially lower than during a meteorologically normal year with high soil water potential (2013). This may reflect suppression of actual biogenic volatile organic compound (BVOC) emissions by drought and thus a reduction in the production of condensable products during the drought-affected vegetation season. This hypothesis is supported by evidence that growth rates during the normal year exhibit a positive correlation with emissions of BVOC modeled on observed forest composition, leaf area index, temperature and photosynthetically active radiation (PAR), but particle growth rates during the drought-affected vegetation season are not correlated with modeled BVOC emissions. These data thus provide indirect evidence that drought stress in forests may reduce BVOC emissions and limit growth of nucleation mode particles to climate-relevant sizes.
Forecasting global atmospheric CO2

A new global atmospheric carbon dioxide (CO2) real-time forecast is now available as part of the pre-operational Monitoring of Atmospheric Composition and Climate – Interim Implementation (MACC-II) service using the infrastructure of the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS). One of the strengths of the CO2 forecasting system is that the land surface, including vegetation CO2 fluxes, is modelled online within the IFS. Other CO2 fluxes are prescribed from inventories and from off-line statistical and physical models. The CO2 forecast also benefits from the transport modelling from a state-of-the-art numerical weather prediction (NWP) system initialized daily with a wealth of meteorological observations. This paper describes the capability of the forecast in modelling the variability of CO2 on different temporal and spatial scales compared to observations. The modulation of the amplitude of the CO2 diurnal cycle by near-surface winds and boundary layer height is generally well represented in the forecast. The CO2 forecast also has high skill in simulating day-to-day synoptic variability. In the atmospheric boundary layer, this skill is significantly enhanced by modelling the day-to-day variability of the CO2 fluxes from vegetation compared to using equivalent monthly mean fluxes with a diurnal cycle. However, biases in the modelled CO2 fluxes also lead to accumulating errors in the CO2 forecast. These biases vary with season with an underestimation of the amplitude of the seasonal cycle both for the CO2 fluxes compared to total optimized fluxes and the atmospheric CO2 compared to observations. The largest biases in the atmospheric CO2 forecast are found in spring, corresponding to the onset of the growing season in the Northern Hemisphere. In the future, the forecast will be re-initialized regularly with atmospheric CO2 analyses based on the assimilation of CO2 products retrieved from satellite measurements and CO2 in situ observations, as they become available in near-real time. In this way, the accumulation of errors in the atmospheric CO2 forecast will be reduced. Improvements in the CO2 forecast are also expected with the continuous developments in the operational IFS.
Impact of the representation of marine stratocumulus clouds on the anthropogenic aerosol effect

Stratocumulus clouds are important for climate as they reflect large amounts of solar radiation back into space. However they are difficult to simulate in global climate models because they form under a sharp inversion and are thin. A comparison of model simulations with the ECHAM6-HAM2 global aerosol climate model to observations, reanalysis and literature data revealed too strong turbulent mixing at the top of stratocumulus clouds and a lack of vertical resolution. Further reasons for cloud biases in stratocumulus regions are the too "active" shallow convection scheme, the cloud cover scheme and possibly too low subsidence rates. To address some of these issues and improve the representation of stratocumulus clouds, we made three distinct changes to ECHAM6-HAM2. With a "sharp" stability function in the turbulent mixing scheme we have observed, similar to previous studies, increases in stratocumulus cloud cover and liquid water path. With an increased vertical resolution in the lower troposphere in ECHAM6-HAM2 the stratocumulus clouds form higher up in the atmosphere and their vertical extent agrees better with reanalysis data. The recently implemented in-cloud aerosol processing in stratiform clouds is used to improve the aerosol representation in the model. Including the improvements also affects the anthropogenic aerosol effect. In-cloud aerosol processing in ECHAM6-HAM2 leads to a decrease in the anthropogenic aerosol effect in the global annual mean from −1.19 Wm−2 in the reference simulation to −1.08 Wm−2, while using a "sharp" stability function leads to an increase to −1.34 Wm−2. The results from the simulations with increased vertical resolution are diverse but increase the anthropogenic aerosol effect to −2.08 Wm−2 at 47 levels and −2.30 Wm−2 at 95 levels.
The impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2 photolysis rate coefficient

Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number–size distribution and hygroscopic growth factor (at RH values above 90%) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty of ω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90%). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98% at the height of 1 km increases by 30.4%, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.
Methane sulfonic acid-enhanced formation of molecular clusters of sulfuric acid and dimethyl amine

Over oceans and in coastal regions, methane sulfonic acid (MSA) is present in substantial concentrations in aerosols and in the gas phase. We present an investigation into the effect of MSA on sulfuric acid- and dimethyl amine (DMA)-based cluster formation rates. From systematic conformational scans and well-tested ab initio methods, we optimise the structures of all MSAx (H2SO4)yDMAz clusters where x + y &leq; 3 and z &leq; 2. The resulting thermodynamic data are used in the Atmospheric Cluster Dynamics Code, and the effect of MSA is evaluated by comparing ternary MSA–H2SO4–DMA cluster formation rates to binary H2SO4–DMA cluster formation rates. Within the range of atmospherically relevant MSA concentrations, we find that MSA may increase cluster formation rates by up to 1 order of magnitude, although typically, the increase will be less than 300 % at 258 K, less than 100 % at 278 K and less than 15 % at 298 K. The results are rationalised by a detailed analysis of the main growth paths of the clusters. We find that MSA-enhanced clustering involves clusters containing one MSA molecule, while clusters containing more than one MSA molecule do not contribute significantly to the growth.
Ground-based aerosol characterization during the South American Biomass Burning Analysis (SAMBBA) field experiment

This paper investigates the physical and chemical characteristics of aerosols at ground level at a site heavily impacted by biomass burning. The site is located near Porto Velho, Rondônia, in the southwestern part of the Brazilian Amazon rainforest, and was selected for the deployment of a large suite of instruments, among them an Aerosol Chemical Speciation Monitor. Our measurements were made during the South American Biomass Burning Analysis (SAMBBA) field experiment, which consisted of a combination of aircraft and ground-based measurements over Brazil, aimed to investigate the impacts of biomass burning emissions on climate, air quality, and numerical weather prediction over South America. The campaign took place during the dry season and the transition to the wet season in September/October 2012. During most of the campaign, the site was impacted by regional biomass burning pollution (average CO mixing ratio of 0.6 ppm), occasionally superimposed by intense (up to 2 ppm of CO), freshly emitted biomass burning plumes. Aerosol number concentrations ranged from ~1000 cm−3 to peaks of up to 35 000 cm−3 (during biomass burning (BB) events, corresponding to an average submicron mass mean concentrations of 13.7 μg m−3 and peak concentrations close to 100 μg m−3. Organic aerosol strongly dominated the submicron non-refractory composition, with an average concentration of 11.4 μg m−3. The inorganic species, NH4, SO4, NO3, and Cl, were observed, on average, at concentrations of 0.44, 0.34, 0.19, and 0.01 μg m−3, respectively. Equivalent black carbon (BCe) ranged from 0.2 to 5.5 μg m−3, with an average concentration of 1.3 μg m−3. During BB peaks, organics accounted for over 90% of total mass (submicron non-refractory plus BCe), among the highest values described in the literature. We examined the ageing of biomass burning organic aerosol (BBOA) using the changes in the H : C and O : C ratios, and found that throughout most of the aerosol processing (O : C &cong; 0.25 to O : C &cong; 0.6), no remarkable change is observed in the H : C ratio (~1.35). Such a result contrasts strongly with previous observations of chemical ageing of both urban and Amazonian biogenic aerosols. At higher levels of processing (O : C > 0.6), the H : C ratio changes with a H : C / O : C slope of −0.5, possibly due to the development of a combination of BB (H : C / O : C slope = 0) and biogenic (H : C /O :C slope =−1) organic aerosol (OA). An analysis of the ΔOA /ΔCO mass ratios yields very little enhancement in the OA loading with atmospheric processing, consistent with previous observations. These results indicate that negligible secondary organic aerosol (SOA) formation occurs throughout the observed BB plume processing, or that SOA formation is almost entirely balanced by OA volatilization. Positive matrix factorization (PMF) of the organic aerosol spectra resulted in three factors: fresh BBOA, aged BBOA, and low-volatility oxygenated organic aerosol (LV-OOA). Analysis of the diurnal patterns and correlation with external markers indicates that during the first part of the campaign, OA concentrations are impacted by local fire plumes with some chemical processing occurring in the near-surface layer. During the second part of the campaign, long-range transport of BB plumes above the surface layer, as well as potential SOAs formed aloft, dominates OA concentrations at our ground-based sampling site. This manuscript describes the first ground-based deployment of the aerosol mass spectrometry at a site heavily impacted by biomass burning in the Amazon region, allowing a deeper understanding of aerosol life cycle in this important ecosystem.
Lidar observation of the 2011 Puyehue-Cordón Caulle volcanic aerosols at Lauder, New Zealand

On 4 June 2011, the Puyehue-Cordón Caulle volcanic complex (40.6° S, 72.1° W) in Chile erupted violently and injected volcanic aerosols into the atmosphere. For the safety of civil aviation, continuous lidar observations were made at Lauder, New Zealand (45.0° S, 169.7° E), from 11 June through 6 July 2011. The purpose of our study is to quantify the influence of the volcanic ejections from large eruptions, and we use the data from the ground-based lidar observation. We analyzed lidar data at a wavelength of 532 nm and derived the backscattering ratio and depolarization ratio profiles. During June and July, within the altitude range of 10–15 km, the volcanic aerosols had high depolarization ratios (20–35%), an indication of non-spherical volcanic ash particles. The time series of the backscattering ratio during continuous observations had three peaks occurring at about 12-day intervals: 26.7 at 11.2 km on 11 June, 18.1 at 12.0 km on 23 June, and 5.3 at 11.1 km on 6 July. The optical depth of the volcanic aerosols was 0.45 on 11 June, when the continuous lidar observation started, 0.31 on 23 June, and 0.12 on 6 July. The depolarization ratio values remained high up to a month after the eruption, and the small wavelength exponent calculated from the backscattering coefficients at 532 nm and 1064 nm suggests that a major constituent of the volcanic aerosols was large, non-spherical particles. The presence of volcanic ash in the stratosphere might affect the error in Greenhouse gases Observing SATellite (GOSAT) XCO2 retrieval using the 1.6 μm band. We briefly discuss the influence of the increased aerosols on GOSAT products.
Spatial and temporal variability of sources of ambient fine particulate matter (PM2.5) in California

To identify major sources of ambient fine particulate matter (PM2.5, dp < 2.5 μm) and quantify their contributions in the state of California, a positive matrix factorization (PMF) receptor model was applied on Speciation Trends Network (STN) data, collected between 2002 and 2007 at eight distinct sampling locations, including El Cajon, Rubidoux, Los Angeles, Simi Valley, Bakersfield, Fresno, San Jose, and Sacramento. Between five to nine sources of fine PM were identified at each sampling site, several of which were common among multiple locations. Secondary aerosols, including secondary ammonium nitrate and ammonium sulfate, were the most abundant contributor to ambient PM2.5 mass at all sampling sites, except for San Jose, with an annual average cumulative contribution of 26 to 63%, across the state. On an annual average basis, vehicular emissions (including both diesel and gasoline vehicles) were the largest primary source of fine PM at all sampling sites in southern California (17–18% of total mass), whereas in Fresno and San Jose, biomass burning was the most dominant primary contributor to ambient PM2.5 (27 and 35% of total mass, respectively), in general agreement with the results of previous source apportionment studies in California. In Bakersfield and Sacramento, vehicular emissions and biomass burning displayed relatively equal annual contributions to ambient PM2.5 mass (12 and 25%, respectively). Other commonly identified sources at all sites included aged and fresh sea salt and soil, which contributed to 0.5–13%, 2–27%, and 1–19% of the total mass, respectively, across all sites and seasons. In addition, a few minor sources were identified exclusively at some of the sites (e.g., chlorine sources, sulfate-bearing road dust, and different types of industrial emissions). These sources overall accounted for a small fraction of the total PM mass across the sampling locations (1 to 15%, on an annual average basis).
Characteristics and sources of gravity waves observed in noctilucent cloud over Norway

Four years of noctilucent cloud (NLC) images from an automated digital camera in Trondheim and results from a ray-tracing model are used to extend the climatology of gravity waves to higher latitudes and to identify their sources during summertime. The climatology of the summertime gravity waves detected in NLC between 64 and 74° N is similar to that observed between 60 and 64° N by Pautet et al. (2011). The direction of propagation of gravity waves observed in the NLC north of 64° N is a continuation of the north and northeast propagation as observed in south of 64° N. However, a unique population of fast, short wavelength waves propagating towards the SW is observed in the NLC, which is consistent with transverse instabilities generated in situ by breaking gravity waves (Fritts and Alexander, 2003). The relative amplitude of the waves observed in the NLC Mie scatter have been combined with ray-tracing results to show that waves propagating from near the tropopause, rather than those resulting from secondary generation in the stratosphere or mesosphere, are more likely to be the sources of the prominent wave structures observed in the NLC. The coastal region of Norway along the latitude of 70° N is identified as the primary source region of the waves generated near the tropopause.