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Modulation of Saharan dust export by the North African dipole

We have studied the relationship between the long-term interannual variability in large-scale meteorology in western North Africa – the largest and most active dust source worldwide – and Saharan dust export in summer, when enhanced dust mobilization in the hyper-arid Sahara results in maximum dust impacts throughout the North Atlantic. We address this issue by analyzing 28 years (1987–2014) of summer averaged dust concentrations at the high-altitude Izaña observatory (~ 2400 m a.s.l.) on Tenerife, and satellite and meteorological reanalysis data. The summer meteorological scenario in North Africa (aloft 850 hPa) is characterized by a high over the the subtropical Sahara and a low over the tropics linked to the monsoon. We measured the variability of this high–low dipole-like pattern in terms of the North African dipole intensity (NAFDI): the difference of geopotential height anomalies averaged over the subtropics (30–32° N, Morocco) and the tropics (10–13° N, Bamako region) close to the Atlantic coast (at 5–8° W). We focused on the 700 hPa standard level due to dust export off the coast of North Africa tending to occur between 1 and 5 km a.s.l. Variability in the NAFDI is associated with displacements of the North African anticyclone over the Sahara and this has implications for wind and dust export. The correlations we found between the 1987–2014 summer mean of NAFDI with dust at Izaña, satellite dust observations and meteorological re-analysis data indicate that increases in the NAFDI (i) result in higher wind speeds at the north of the Inter-Tropical Convergence Zone that are associated with enhanced dust export over the subtropical North Atlantic, (ii) influence the long-term variability of the size distribution of exported dust particles (increasing the load of coarse dust) and (iii) are associated with enhanced rains in the tropical and northern shifts of the tropical rain band that may affect the southern Sahel. Interannual variability in NAFDI is also connected to spatial distribution of dust over the North Atlantic; high NAFDI summers are associated with major dust export (linked to winds) in the subtropics and minor dust loads in the tropics (linked to higher rainfall), and vice versa. The evolution of the summer NAFDI values since 1950 to the present day shows connections to climatic variability (through the Sahelian drought, ENSO (El Niño–Southern Oscillation) and winds) that have implications for dust export paths. Efforts to anticipate how dust export may evolve in future decades will require a better understanding of how the large-scale meteorological systems represented by the NAFD will evolve.
Stably stratified canopy flow in complex terrain

Stably stratified canopy flow in complex terrain has been considered a difficult condition for measuring net ecosystem–atmosphere exchanges of carbon, water vapor, and energy. A long-standing advection error in eddy-flux measurements is caused by stably stratified canopy flow. Such a condition with strong thermal gradient and less turbulent air is also difficult for modeling. To understand the challenging atmospheric condition for eddy-flux measurements, we use the renormalized group (RNG) k–ϵ turbulence model to investigate the main characteristics of stably stratified canopy flows in complex terrain. In this two-dimensional simulation, we imposed persistent constant heat flux at ground surface and linearly increasing cooling rate in the upper-canopy layer, vertically varying dissipative force from canopy drag elements, buoyancy forcing induced from thermal stratification and the hill terrain. These strong boundary effects keep nonlinearity in the two-dimensional Navier–Stokes equations high enough to generate turbulent behavior. The fundamental characteristics of nighttime canopy flow over complex terrain measured by the small number of available multi-tower advection experiments can be reproduced by this numerical simulation, such as (1) unstable layer in the canopy and super-stable layers associated with flow decoupling in deep canopy and near the top of canopy; (2) sub-canopy drainage flow and drainage flow near the top of canopy in calm night; (3) upward momentum transfer in canopy, downward heat transfer in upper canopy and upward heat transfer in deep canopy; and (4) large buoyancy suppression and weak shear production in strong stability.
Secondary organic aerosol formation from the β-pinene+NO3 system: effect of humidity and peroxy radical fate

The formation of secondary organic aerosol (SOA) from the oxidation of β-pinene via nitrate radicals is investigated in the Georgia Tech Environmental Chamber (GTEC) facility. Aerosol yields are determined for experiments performed under both dry (relative humidity (RH) < 2 %) and humid (RH = 50 % and RH = 70 %) conditions. To probe the effects of peroxy radical (RO2) fate on aerosol formation, "RO2 + NO3 dominant" and "RO2 + HO2 dominant" experiments are performed. Gas-phase organic nitrate species (with molecular weights of 215, 229, 231, and 245 amu, which likely correspond to molecular formulas of C10H17NO4, C10H15NO5, C10H17NO5, and C10H15NO6, respectively) are detected by chemical ionization mass spectrometry (CIMS) and their formation mechanisms are proposed. The NO+ (at m/z 30) and NO2+ (at m/z 46) ions contribute about 11 % to the combined organics and nitrate signals in the typical aerosol mass spectrum, with the NO+ : NO2+ ratio ranging from 4.8 to 10.2 in all experiments conducted. The SOA yields in the "RO2 + NO3 dominant" and "RO2 + HO2 dominant" experiments are comparable. For a wide range of organic mass loadings (5.1–216.1 μg m−3), the aerosol mass yield is calculated to be 27.0–104.1 %. Although humidity does not appear to affect SOA yields, there is evidence of particle-phase hydrolysis of organic nitrates, which are estimated to compose 45–74 % of the organic aerosol. The extent of organic nitrate hydrolysis is significantly lower than that observed in previous studies on photooxidation of volatile organic compounds in the presence of NOx. It is estimated that about 90 and 10 % of the organic nitrates formed from the β-pinene+NO3 reaction are primary organic nitrates and tertiary organic nitrates, respectively. While the primary organic nitrates do not appear to hydrolyze, the tertiary organic nitrates undergo hydrolysis with a lifetime of 3–4.5 h. Results from this laboratory chamber study provide the fundamental data to evaluate the contributions of monoterpene + NO3 reaction to ambient organic aerosol measured in the southeastern United States, including the Southern Oxidant and Aerosol Study (SOAS) and the Southeastern Center for Air Pollution and Epidemiology (SCAPE) study.
A modified micrometeorological gradient method for estimating O3 dry depositions over a forest canopy

Small pollutant concentration gradients between levels above a plant canopy result in large uncertainties in estimated air–surface exchange fluxes when using existing micrometeorological gradient methods, including the aerodynamic gradient method (AGM) and the modified Bowen ratio method (MBR). A modified micrometeorological gradient method (MGM) is proposed in this study for estimating O3 dry deposition fluxes over a forest canopy using concentration gradients between a level above and a level below the canopy top, taking advantage of relatively large gradients between these levels due to significant pollutant uptake in the top layers of the canopy. The new method is compared with the AGM and MBR methods and is also evaluated using eddy-covariance (EC) flux measurements collected at the Harvard Forest Environmental Measurement Site, Massachusetts, during 1993–2000. All three gradient methods (AGM, MBR, and MGM) produced similar diurnal cycles of O3 dry deposition velocity (Vd(O3)) to the EC measurements, with the MGM method being the closest in magnitude to the EC measurements. The multi-year average Vd(O3) differed significantly between these methods, with the AGM, MBR, and MGM method being 2.28, 1.45, and 1.18 times that of the EC, respectively. Sensitivity experiments identified several input parameters for the MGM method as first-order parameters that affect the estimated Vd(O3). A 10% uncertainty in the wind speed attenuation coefficient or canopy displacement height can cause about 10% uncertainty in the estimated Vd(O3). An unrealistic leaf area density vertical profile can cause an uncertainty of a factor of 2.0 in the estimated Vd(O3). Other input parameters or formulas for stability functions only caused an uncertainly of a few percent. The new method provides an alternative approach to monitoring/estimating long-term deposition fluxes of similar pollutants over tall canopies.
Deposition and immersion-mode nucleation of ice by three distinct samples of volcanic ash

Ice nucleation of volcanic ash controls both ash aggregation and cloud glaciation, which affect atmospheric transport and global climate. Previously, it has been suggested that there is one characteristic ice nucleation efficiency for all volcanic ash, regardless of its composition, when accounting for surface area; however, this claim is derived from data from only two volcanic eruptions. In this work, we have studied the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman microscopy coupled to an environmental cell. Ash from the Fuego (basaltic ash, Guatemala), Soufrière Hills (andesitic ash, Montserrat), and Taupo (Oruanui eruption, rhyolitic ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. In the present study, we find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice from 225 to 235 K at ice saturation ratios of 1.05 ± 0.01, comparable to the mineral dust proxy kaolinite. Since depositional ice nucleation will be more important at colder temperatures, fine volcanic ash may represent a global source of cold-cloud ice nuclei. For immersion freezing relevant to mixed-phase clouds, however, only the Oruanui ash exhibited appreciable heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.
Wet scavenging limits the detection of aerosol effects on precipitation

Satellite studies of aerosol–cloud interactions usually make use of retrievals of both aerosol and cloud properties, but these retrievals are rarely spatially co-located. While it is possible to retrieve aerosol properties above clouds under certain circumstances, aerosol properties are usually only retrieved in cloud-free scenes. Generally, the smaller spatial variability of aerosols compared to clouds reduces the importance of this sampling difference. However, as precipitation generates an increase in spatial variability of aerosols, the imperfect co-location of aerosol and cloud property retrievals may lead to changes in observed aerosol–cloud–precipitation relationships in precipitating environments. In this work, we use a regional-scale model, satellite observations and reanalysis data to investigate how the non-coincidence of aerosol, cloud and precipitation retrievals affects correlations between them. We show that the difference in the aerosol optical depth (AOD)–precipitation relationship between general circulation models (GCMs) and satellite observations can be explained by the wet scavenging of aerosol. Using observations of the development of precipitation from cloud regimes, we show how the influence of wet scavenging can obscure possible aerosol influences on precipitation from convective clouds. This obscuring of aerosol–cloud–precipitation interactions by wet scavenging suggests that even if GCMs contained a perfect representation of aerosol influences on convective clouds, the difficulty of separating the "clear-sky" aerosol from the "all-sky" aerosol in GCMs may prevent them from reproducing the correlations seen in satellite data.
Technical Note: Using DEG-CPCs at upper tropospheric temperatures

Over the last few years, several condensation particle counters (CPCs) capable of measuring in the sub-3 nm size range have been developed. Here we study the performance of CPCs based on diethylene glycol (DEG) at different temperatures during Cosmics Leaving OUtdoor Droplets (CLOUD) measurements at CERN. The data shown here are the first set of verification measurements for sub-3 nm CPCs under upper tropospheric temperatures using atmospherically relevant aerosol particles. To put the results in perspective we calibrated the DEG-CPC at room temperature, resulting in a cut-off diameter of 1.4 nm. All diameters refer to mobility equivalent diameters in this paper. At upper tropospheric temperatures ranging from 246.15 K to 207.15 K, we found cut-off sizes relative to a particle size magnifier in the range of 2.5 to 2.8 nm. Due to low number concentration after size classification, the cut-off diameters have a high uncertainty (±0.3 nm) associated with them. Operating two laminar flow DEG-CPCs with different cut-off sizes together with other aerosol instruments, we looked at the growth rates of aerosol population in the CLOUD chamber for particles smaller than 10 nm at different temperatures. A more consistent picture emerged when we normalized the growth rates to a fixed gas-phase sulfuric acid concentration. All of the instruments detected larger growth rates at lower temperatures, and the observed growth rates decreased as a function of temperature, showing a similar trend for all instruments. The theoretical calculations had a similar but much smaller temperature dependency.
The role of blowing snow in the activation of bromine over first-year Antarctic sea ice

It is well known that during polar springtime halide sea salt ions, in particular Br-, are photochemically activated into reactive halogen species (e.g., Br and BrO), where they break down tropospheric ozone. This research investigated the role of blowing snow in transporting salts from the sea ice/snow surface into reactive bromine species in the air. At two different locations over first-year ice in the Ross Sea, Antarctica, collection baskets captured blowing snow at different heights. In addition, sea ice cores and surface snow samples were collected throughout the month-long campaign. Over this time, sea ice and surface snow Br- / Cl- mass ratios remained constant and equivalent to seawater, and only in lofted snow did bromide become depleted relative to chloride. This suggests that replenishment of bromide in the snowpack occurs faster than bromine activation in mid-strength wind conditions (approximately 10 m s−1) or that blowing snow represents only a small portion of the surface snowpack. Additionally, lofted snow was found to be depleted in sulfate and enriched in nitrate relative to surface snow.
Reassessing the ratio of glyoxal to formaldehyde as an indicator of hydrocarbon precursor speciation

The yield of formaldehyde (HCHO) and glyoxal (CHOCHO) from oxidation of volatile organic compounds (VOCs) depends on precursor VOC structure and the concentration of NOx (NOx = NO + NO2). Previous work has proposed that the ratio of CHOCHO to HCHO (RGF) can be used as an indicator of precursor VOC speciation, and absolute concentrations of the CHOCHO and HCHO as indicators of NOx. Because this metric is measurable by satellite, it is potentially useful on a global scale; however, absolute values and trends in RGF have differed between satellite and ground-based observations. To investigate potential causes of previous discrepancies and the usefulness of this ratio, we present measurements of CHOCHO and HCHO over the southeastern United States (SE US) from the 2013 SENEX (Southeast Nexus) flight campaign, and compare these measurements with OMI (Ozone Monitoring Instrument) satellite retrievals. High time-resolution flight measurements show that high RGF is associated with monoterpene emissions, low RGF is associated with isoprene oxidation, and emissions associated with oil and gas production can lead to small-scale variation in regional RGF. During the summertime in the SE US, RGF is not a reliable diagnostic of anthropogenic VOC emissions, as HCHO and CHOCHO production are dominated by isoprene oxidation. Our results show that the new CHOCHO retrieval algorithm reduces the previous disagreement between satellite and in situ RGF observations. As the absolute values and trends in RGF observed during SENEX are largely reproduced by OMI observations, we conclude that satellite-based observations of RGF can be used alongside knowledge of land use as a global diagnostic of dominant hydrocarbon speciation.
The relationship between cloud condensation nuclei (CCN) concentration and light extinction of dried particles: indications of underlying aerosol processes and implications for satellite-based CCN estimates

We examine the relationship between the number concentration of boundary-layer cloud condensation nuclei (CCN) and light extinction to investigate underlying aerosol processes and satellite-based CCN estimates. For a variety of airborne and ground-based observations not dominated by dust, regression identifies the CCN (cm−3) at 0.4 ± 0.1% supersaturation with 100.3α +1.3σ0.75 where σ (Mm−1) is the 500 nm extinction coefficient by dried particles and α is the Angstrom exponent. The deviation of 1 km horizontal average data from this approximation is typically within a factor of 2.0. ∂logCCN / ∂logσ is less than unity because, among other explanations, growth processes generally make aerosols scatter more light without increasing their number. This, barring special meteorology–aerosol connections, associates a doubling of aerosol optical depth with less than a doubling of CCN, contrary to previous studies based on heavily averaged measurements or a satellite algorithm.