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Detection of dust aerosol by combining CALIPSO active lidar and passive IIR measurements

The version 2 Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) dust layer detection method, which is based only on lidar measurements, misclassified about 43% dust layers (mainly dense dust layers) as cloud layers over the Taklamakan Desert. To address this problem, a new method was developed by combining the CALIPSO Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and passive Infrared Imaging Radiometer (IIR) measurements. This combined lidar and IR measurement (hereafter, CLIM) method uses the IIR tri-spectral IR brightness temperatures to discriminate between ice cloud and dense dust layers, and lidar measurements alone to detect thin dust and water cloud layers. The brightness temperature difference between 10.60 and 12.05 μm (BTD11−12) is typically negative for dense dust and generally positive for ice cloud, but it varies from negative to positive for thin dust layers, which the CALIPSO lidar correctly identifies. Results show that the CLIM method could significantly reduce misclassification rates to as low as ~7% for the active dust season of spring 2008 over the Taklamakan Desert. The CLIM method also revealed 18% more dust layers having greatly intensified backscatter between 1.8 and 4 km altitude over the source region compared to the CALIPSO version 2 data. These results allow a more accurate assessment of the effect of dust on climate.
Quantifying pollution inflow and outflow over East Asia in spring with regional and global models

Understanding the exchange processes between the atmospheric boundary layer and the free troposphere is crucial for estimating hemispheric transport of air pollution. Most studies of hemispheric air pollution transport have taken a large-scale perspective using global chemical transport models with fairly coarse spatial and temporal resolutions. In support of United Nations Task Force on Hemispheric Transport of Air Pollution (TF HTAP; <a href="www.htap.org"target="_blank">www.htap.org</a>), this study employs two high-resolution atmospheric chemistry models (WRF-Chem and CMAQ; 36×36 km) driven with chemical boundary conditions from a global model (MOZART; 1.9×1.9°) to examine the role of fine-scale transport and chemistry processes in controlling pollution export and import over the Asian continent in spring (March 2001). Our analysis indicates the importance of rapid venting through deep convection that develops along the leading edge of frontal system convergence bands, which are not adequately resolved in either of two global models compared with TRACE-P aircraft observations during a frontal event. Both regional model simulations and observations show that frontal outflows of CO, O3 and PAN can extend to the upper troposphere (6–9 km). Pollution plumes in the global MOZART model are typically diluted and insufficiently lofted to higher altitudes where they can undergo more efficient transport in stronger winds. We use sensitivity simulations that perturb chemical boundary conditions in the CMAQ regional model to estimate that the O3 production over East Asia (EA) driven by PAN decomposition contributes 20% of the spatial averaged total O3 response to European (EU) emission perturbations in March, and occasionally contributes approximately 50% of the total O3 response in subsiding plumes at mountain observatories (at approximately 2 km altitude). The response to decomposing PAN of EU origin is strongly affected by the O3 formation chemical regimes, which vary with the model chemical mechanism and NOx/VOC emissions. Our high-resolution models demonstrate a large spatial variability (by up to a factor of 6) in the response of local O3 to 20% reductions in EU anthropogenic O3 precursor emissions. The response in the highly populated Asian megacities is 40–50% lower in our high-resolution models than the global model, suggesting that the source-receptor relationships inferred from the global coarse-resolution models likely overestimate health impacts associated with intercontinental O3 transport. Our results highlight the important roles of rapid convective transport, orographic forcing, urban photochemistry and heterogeneous boundary layer processes in controlling intercontinental transport; these processes may not be well resolved in the large-scale models.
A case study of dust aerosol radiative properties over Lanzhou, China

The vertical distribution of dust aerosol and its radiative properties are analysed using the data measured by the micropulse lidar, profiling microwave radiometer, sunphotometer, particulate monitor, and nephelometer at the Semi-Arid Climate and Environment Observatory of Lanzhou University (SACOL) during a dust storm from 27 March to 29 March 2007. The analysis shows that the dust aerosol mainly exists below 2 km in height, and the dust aerosol extinction coefficient decreases with height. The temporal evolution of aerosol optical depth (AOD) during the dust storm is characterized by a sub-maximum at 22:00 (Beijing Time), 27 March and a maximum at 12:00, 28 March. The AOD respectively derived by lidar and sunphotometer shows a good consistency. The PM10 concentration and aerosol scattering coefficient share similar variation trends, and their maximums both appear at 22:00, 27 March. The aerosol extinction coefficient and relative humidity have the similar trends and their maximums almost appear at the same heights, which presents a correlation between extinction coefficient and relative humidity known as aerosol hygroscopicity. The relative humidity is related with temperature, and then the temperature will affect the aerosol extinction properties by modifying the relative humidity condition. The aerosol extinction coefficient, scattering coefficient, and PM10 concentration present good linear correlations. The correlation coefficients of the aerosol scattering coefficients of 450, 520, and 700 nm and PM10 concentration, of aerosol extinction coefficient retrieved by lidar at 532 nm and PM10 concentration, and of aerosol extinction and scattering coefficient are respectively 0.98, 0.94, and 0.96.
Optimal estimation retrieval of aerosol microphysical properties from SAGE~II satellite observations in the volcanically unperturbed lower stratosphere

Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003). An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE) method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths) with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities), even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal) size distributions naturally differ from the correct bimodal values, the associated surface area (A) and volume densities (V) are, nevertheless, fairly accurately retrieved, except at values larger than 1.0 μm2 cm−3 (A) and 0.05 μm3 cm−3 (V), where they tend to underestimate the true bimodal values. Due to the limited information content in the SAGE II spectral extinction measurements this kind of forward model error cannot be avoided here. Nevertheless, the retrieved uncertainties are a good estimate of the true errors in the retrieved integrated properties, except where the surface area density exceeds the 1.0 μm2 cm−3 threshold. When applied to near-global SAGE II satellite extinction measured in 1999 the retrieved OE surface area and volume densities are observed to be larger by, respectively, 20–50% and 10–40% compared to those estimates obtained by the SAGE~II operational retrieval algorithm. An examination of the OE algorithm biases with in situ data indicates that the new OE aerosol property estimates tend to be more realistic than previous estimates obtained from remotely sensed data through other retrieval techniques. Based on the results of this study we therefore suggest that the new Optimal Estimation retrieval algorithm is able to contribute to an advancement in aerosol research by considerably improving current estimates of aerosol properties in the lower stratosphere under low aerosol loading conditions.
Observations of turbulence-induced new particle formation in the residual layer

Aerosol particle measurements in the atmospheric boundary layer performed by a helicopter-borne measurement payload and by a lidar system from a case study during the IMPACT field campaign in Cabauw (NL) are presented. Layers of increased number concentrations of ultrafine particles were observed in the residual layer, indicating relatively recent new-particle formation. These layers were characterized by a sub-critical Richardson number and concomitant increased turbulence. Turbulent mixing is likely to lead to local supersaturation of possible precursor gases which are essential for new particle formation. Observed peaks in the number concentrations of ultrafine particles at ground level are connected to the new particle formation in the residual layer by boundary layer development and vertical mixing.
Large estragole fluxes from oil palms in Borneo

During two field campaigns (OP3 and ACES), which ran in Borneo in 2008, we measured large emissions of estragole (methyl chavicol; IUPAC systematic name 1-allyl-4-methoxybenzene; CAS number 140-67-0) in ambient air above oil palm canopies (0.81 mg m−2 h−1 and 3.2 ppbv for mean midday fluxes and mixing ratios respectively) and subsequently from flower enclosures. However, we did not detect this compound at a nearby rainforest. Estragole is a known attractant of the African oil palm weevil (Elaeidobius kamerunicus), which pollinates oil palms (Elaeis guineensis). There has been recent interest in the biogenic emissions of estragole but it is normally not included in atmospheric models of biogenic emissions and atmospheric chemistry despite its relatively high potential for secondary organic aerosol formation from photooxidation and high reactivity with OH radical. We report the first direct canopy-scale measurements of estragole fluxes from tropical oil palms by the virtual disjunct eddy covariance technique and compare them with previously reported data for estragole emissions from Ponderosa pine. Flowers, rather than leaves, appear to be the main source of estragole from oil palms; we derive a global estimate of estragole emissions from oil palm plantations of ~0.5 Tg y−1. The observed ecosystem mean fluxes (0.44 mg m−2 h−1) and mean ambient volume mixing ratios (3.0 ppbv) of estragole are the highest reported so far. The value for midday mixing ratios is not much different from the total average as, unlike other VOCs (e.g. isoprene), the main peak occurred in the evening rather than in the middle of the day. Despite this, we show that the estragole flux can be parameterised using a modified G06 algorithm for emission. However, the model underestimates the afternoon peak even though a similar approach works well for isoprene. Our measurements suggest that this biogenic compound may have an impact on regional atmospheric chemistry that previously has not been accounted for in models and could become more important in the future due to expansion of the areas of oil palm plantation.
Technical Note: Fast two-dimensional GC-MS with thermal extraction for anhydro-sugars in fine aerosols

A fast two-dimensional gas chromatography (GC-MS) method that uses heart-cutting and thermal extraction (TE) and requires no chemical derivatization was developed for the determination of anhydro-sugars in fine aerosols. Evaluation of the TE-GC-GC-MS method shows high average relative accuracy (≥90%), reproducibility (≤10% relative standard deviation), detection limits of less than 3 ng/μL, and negligible carryover for levoglucosan, mannosan, and galactosan markers. TE-GC-GC-MS- and solvent extraction (SE)-GC-MS-measured levoglucosan concentrations correlate across several diverse types of biomass burning aerosols. Because the SE-GC-MS measurements were taken 8 years prior to the TE-GC-GC-MS ones, the stability of levoglucosan is established for quartz filter-collected biomass burning aerosol samples stored at ultra-low temperature (−50 °C). Levoglucosan concentrations (w/w) in aerosols collected following atmospheric dilution near open fires of varying intensity are similar to those in biomass burning aerosols produced in a laboratory enclosure. An average levoglucosan-mannosan-galactosan ratio of 15:2:1 is observed for these two aerosol sets. TE-GC-GC-MS analysis of atmospheric aerosols from the US and Africa produced levoglucosan concentrations (0.01–1.6 μg/m3) well within those reported for aerosols collected globally and examined using different analytical techniques (0.004–7.6 μg/m3). Further comparisons among techniques suggest that fast TE-GC-GC-MS is among the most sensitive, accurate, and precise methods for compound-specific quantification of anhydro-sugars. In addition, an approximately twofold increase in anhydro-sugar determination may be realized when combining TE with fast chromatography.
Analysis of snow bidirectional reflectance from ARCTAS Spring-2008 Campaign

The spring 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) experiment was one of major intensive field campaigns of the International Polar Year aimed at detailed characterization of atmospheric physical and chemical processes in the Arctic region. A part of this campaign was a unique snow bidirectional reflectance experiment on the NASA P-3B aircraft conducted on 7 and 15 April by the Cloud Absorption Radiometer (CAR) jointly with airborne Ames Airborne Tracking Sunphotometer (AATS) and ground-based Aerosol Robotic Network (AERONET) sunphotometers. The CAR data were atmospherically corrected to derive snow bidirectional reflectance at high 1° angular resolution in view zenith and azimuthal angles along with surface albedo. The derived albedo was generally in good agreement with ground albedo measurements collected on 15 April. The CAR snow bidirectional reflectance factor (BRF) was used to study the accuracy of analytical Ross-Thick Li-Sparse (RTLS), Modified Rahman-Pinty-Verstraete (MRPV) and Asymptotic Analytical Radiative Transfer (AART) BRF models. Except for the glint region (azimuthal angles φ<40°), the best fit MRPV and RTLS models fit snow BRF to within ±0.05. The plane-parallel radiative transfer (PPRT) solution was also analyzed with the models of spheres, spheroids, randomly oriented fractal crystals, and with a synthetic phase function. The latter merged the model of spheroids for the forward scattering angles with the fractal model in the backscattering direction. The PPRT solution with synthetic phase function provided the best fit to measured BRF in the full range of angles. Regardless of the snow grain shape, the PPRT model significantly over-/underestimated snow BRF in the glint/backscattering regions, respectively, which agrees with other studies. To improve agreement with experiment, we introduced a model of macroscopic snow surface roughness by averaging the PPRT solution over the slope distribution function and by adding a simple model of shadows. With macroscopic roughness described by two parameters, the AART model achieved an accuracy of about ±0.05 with a possible bias of ±0.03 in the spectral range 0.4–2.2 μm. This high accuracy holds at view zenith angles below 55–60° covering the practically important range for remote sensing applications, and includes both glint and backscattering directions.
Process analysis and sensitivity study of regional ozone formation over the Pearl River Delta, China, during the PRIDE-PRD2004 campaign using the Community Multiscale Air Quality modeling system

In this study, the Community Multiscale Air Quality (CMAQ) modeling system is used to simulate the ozone (O3) episodes during the Program of Regional Integrated Experiments of Air Quality over the Pearl River Delta, China, in October 2004 (PRIDE-PRD2004). The simulation suggests that O3 pollution is a regional phenomenon in the Pearl River Delta (PRD). Elevated O3 levels often occurred in the southwestern inland PRD, Pearl River estuary (PRE), and southern coastal areas during the 1-month field campaign. Three evolution patterns of simulated surface O3 are summarized based on different near-ground flow conditions. More than 75% of days featured interactions between weak synoptic forcing and local sea-land circulation. Integrated process rate (IPR) analysis shows that photochemical production is a dominant contributor to O3 enhancement from 09:00 to 15:00 local standard time in the atmospheric boundary layer over most areas with elevated O3 occurrence in the mid-afternoon. The simulated ozone production efficiency is 2–8 O3 molecules per NOx molecule oxidized in areas with high O3 chemical production. Precursors of O3 originating from different source regions in the central PRD are mixed during the course of transport to downwind rural areas during nighttime and early morning, where they then contribute to the daytime O3 photochemical production. The sea-land circulation plays an important role on the regional O3 formation and distribution over PRD. Sensitivity studies suggest that O3 formation is volatile-organic-compound-limited in the central inland PRD, PRE, and surrounding coastal areas with less chemical aging (NOx/NOy>0.6), but is NOx-limited in the rural southwestern PRD with aged air (NOx/NOy<0.3).
Observed and simulated global distribution and budget of atmospheric C2-C5 alkanes

The primary sources and atmospheric chemistry of C2-C5 alkanes were incorporated into the atmospheric chemistry general circulation model EMAC. Model output is compared with new observations from the NOAA/ESRL GMD Cooperative Air Sampling Network. Based on the global coverage of the data, two different anthropogenic emission datasets for C4-C5 alkanes, widely used in the modelling community, are evaluated. We show that the model reproduces the main atmospheric features of the C2-C5 alkanes (e.g., seasonality). While the simulated values for ethane and propane are within a 20% range of the measurements, larger deviations are found for the other tracers. According to the analysis, an oceanic source of butanes and pentanes larger than the current estimates would be necessary to match the observations at some coastal stations. Finally the effect of C2-C5 alkanes on the concentration of acetone and acetaldehyde are assessed. Their chemical sources are largely controlled by the reaction with OH, while the reactions with NO3 and Cl contribute only to a little extent. The total amount of acetone produced by propane, i-butane and i-pentane oxidation is 11.2 Tg/yr, 4.3 Tg/yr, and 5.8 Tg/yr, respectively. Moreover, 18.1, 3.1, 3.4, 1.4 and 4.8 Tg/yr of acetaldehyde are formed by the oxidation of ethane, propane, n-butane, n-pentane and i-pentane, respectively.