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Deriving the effect of wind speed on clean marine aerosol optical properties using the A-Train satellites

The relationship between "clean marine" aerosol optical properties and ocean surface wind speed is explored using remotely sensed data from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the CALIPSO satellite and the Advanced Microwave Scanning Radiometer (AMSR-E) on board the AQUA satellite. Detailed data analyses are carried out over 15 regions selected to be representative of different areas of the global ocean for the time period from June 2006 to April 2011. Based on remotely sensed optical properties the CALIPSO algorithm is capable of discriminating "clean marine" aerosols from other types often present over the ocean (such as urban/industrial pollution, desert dust and biomass burning). The global mean optical depth of "clean marine" aerosol at 532 nm (AOD532) is found to be 0.052 ± 0.038 (mean plus or minus standard deviation). The mean layer integrated particulate depolarization ratio of marine aerosols is 0.02 ± 0.016. Integrated attenuated backscatter and color ratio of marine aerosols at 532 nm were found to be 0.003 ± 0.002 sr−1 and 0.530 ± 0.149, respectively. A logistic regression between AOD532 and 10-m surface wind speed (U10) revealed three distinct regimes. For U10 ≤ 4 m s−1 the mean CALIPSO-derived AOD532 is found to be 0.02 ± 0.003 with little dependency on the surface wind speed. For 4 < U10 ≤ 12 m s−1, representing the dominant fraction of all available data, marine aerosol optical depth is linearly correlated with the surface wind speed values, with a slope of 0.006 s m−1. In this intermediate wind speed region, the AOD532 vs. U10 regression slope derived here is comparable to previously reported values. At very high wind speed values (U10 > 18 m s−1), the AOD532-wind speed relationship showed a tendency toward leveling off, asymptotically approaching value of 0.15. The conclusions of this study regarding the aerosol extinction vs. wind speed relationship may have been influenced by the constant lidar ratio used for CALIPSO-derived AOD532. Nevertheless, active satellite sensor used in this study that allows separation of maritime wind induced component of AOD from the total AOD over the ocean could lead to improvements in optical properties of sea spray aerosols and their production mechanisms.
Source apportionment of carbonaceous aerosol in southern Sweden

A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (14C) and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (80%), which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (32%) and fossil fuel combustion (28%) were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP MSC-W chemical transport model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 2.2 compared to the measurements.
Cloud condensation nuclei closure study on summer arctic aerosol

We present an aerosol – cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble (κorg=0.02), leading to a mean total κ, κtot, of 0.33 ± 0.13. However, several settings led to closure and κorg=0.2 is found to be an upper limit at 0.1% supersaturation. κorg≤0.2 leads to a κtot range of 0.33 ± 013 to 0.50 ± 0.11. Thus, the organic material ranges from being sparingly soluble to effectively insoluble. These results suggest that an increase in organic mass fraction in particles of a certain size would lead to a suppression of the Arctic CCN activity.
Interannual variability of ozone and carbon monoxide at the Whistler high elevation site: 2002–2006

In spring 2002, an atmospheric measurement site was established at the peak of Whistler Mountain in British Columbia, Canada to measure trace gases, particle chemistry and physics, and meteorology. This paper uses continuous measurements from March 2002 to December 2006 to investigate the influence of trans-Pacific transport and North American forest fires on both O3 and CO at Whistler. Annual mean mixing ratios of O3 and CO were 41 ppbv (monthly means of 35–48 ppbv) and 145 ppbv (monthly means of 113–177 ppbv) respectively with both species exhibiting an annual cycle of late-winter to early-spring maxima and summer minima. The absence of a broad summer O3 peak differs from previously-reported high altitude sites in the western US. The highest monthly-averaged O3 and CO mixing ratios relative to the 5-yr monthly means were seen in fall 2002 and spring 2003 with increased O3 and CO of 10 % and 25 % respectively. These increases correspond to anomalously-high values reported at other Northern Hemisphere sites and are attributed to fires in the Russian Federation. Air mass back trajectory analysis is used to associate the mean enhancements of O3 and CO with trans-Pacific transported or North American air masses relative to the Pacific background. Mean values of the enhancements for March to June in trans-Pacific air masses were 6 ppbv and 16 ppbv for O3 and CO respectively. In summers 2002–2006, higher CO and O3 mixing ratios were almost always observed in North American air masses and this relative enhancement co-varied for each year with the western US and Canada total wildfire area. The greatest enhancements in O3 and CO were seen in 2004, a record year for forest fires in Alaska and the Yukon Territory with average O3 and CO mixing ratios 13 and 43 ppbv above background values.
Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia

The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker fragments places upper limits of 7.5% for amino acids and 5.6% for carbohydrates on the contribution of primary biological aerosol particles (PBAP) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m−3. Carbohydrates and proteins (composed of amino acids) make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAP mass fraction of about 20% to the submicron organic aerosol measured in Amazonia during AMAZE-08.
The Arctic vortex in March 2011: a dynamical perspective

Despite the record ozone loss observed in March 2011, dynamical conditions in the Arctic stratosphere were unusual but not unprecedented. Weak planetary wave driving in February preceded cold anomalies in the polar lower stratosphere in March and a relatively late breakup of the Arctic vortex in April. La Niña conditions and the westerly phase of the quasi-biennial oscillation (QBO) were observed in March 2011. Though these conditions are generally associated with a stronger vortex in mid-winter, the respective cold anomalies do not persist through March. Therefore, the La Niña and QBO-westerly conditions cannot explain the observed cold anomalies in March 2011. In contrast, positive sea surface temperature anomalies in the North Pacific may have contributed to the unusually weak tropospheric wave driving and strong Arctic vortex in late winter 2011.
Aerosol optical properties and radiative effect determined from sky-radiometer over Loess Plateau of Northwest China

The aerosol optical properties and their associated radiative effects are derived from sky-radiometer and surface solar radiation data collected over the Semi-Arid Climate and Environment Observatory of Lanzhou University (SACOL) for the period of March to May (MAM) 2009. The result shows that the seasonal mean aerosol optical depth (AOD) at 500 nm in MAM is 0.40. The single scattering albedo (SSA) at 500 nm in MAM at SACOL fluctuates significantly ranging from 0.82 to 0.98. The averaged value of SSA there for background aerosol is 0.90 in MAM, while it is smaller (0.87) during the dust event outbreak period. The smaller SSA can be interpreted as the result of larger particles during dust events. The averaged asymmetry factor (ASY) at 500 nm during dust event period is 0.73, which is larger than 0.70 of background aerosols. The averaged shortwave radiative effects of the aerosols during dust event period in MAM are 0.68, −70.02 and 70.70 W m−2, respectively, at the top of the atmosphere (TOA), surface and in the atmosphere. The aerosols heat the atmosphere during dust event period by up to about 2 K day−1 (daily averaged), which is 60 % larger than the heating (1.25 K day−1) of background aerosols. The significant heating effect in the atmosphere of the aerosols during dust event is determined by larger AOD and smaller SSA.
Mass absorption efficiency of elemental carbon and water-soluble organic carbon in Beijing, China

The mass absorption efficiency (MAE) of elemental carbon (EC) in Beijing was quantified using a thermal-optical carbon analyzer. The MAE measured at 632 nm was 8.45±1.71 and 9.41±1.92 m2 g−1 during winter and summer respectively. The daily variation of MAE was found to coincide with the abundance of organic carbon (OC), especially the OC to EC ratio, perhaps due to the enhancement by coating with organic aerosol (especially secondary organic aerosol, SOA) or the artifacts resulting from the redistribution of liquid-like organic particles during the filter-based absorption measurements. Using a converting approach that accounts for the discrepancy caused by measurements methods of both light absorption and EC concentration, previously published MAE values were converted to the equivalent-MAE, which is the estimated value if using the same measurement methods as used in this study. The equivalent-MAE was found to be much lower in the regions heavily impacted by biomass burning (e.g., below 2.7 m2 g−1 for two Indian cities). Results from source samples (including diesel exhaust samples and biomass smoke samples) also demonstrated that emissions from biomass burning would decrease the MAE of EC. Moreover, optical properties of water-soluble organic carbon (WSOC) in Beijing were presented. Light absorption by WSOC exhibited strong wavelength (λ) dependence such that absorption varied approximately as λ−7, which was characteristic of the brown carbon spectra. The MAE of WSOC (measured at 365 nm) was 1.79±0.24 and 0.71±0.20 m2 g−1 during winter and summer respectively. The large discrepancy between the MAE of WSOC during winter and summer was attributed to the difference in the precursors of SOA such that anthropogenic volatile organic compounds (AVOCs) should be more important as the precursors of SOA in winter. The MAE of WSOC in Beijing was much higher than results from the southeastern United States which were obtained using the same method as used in this study, perhaps due to the stronger emissions of biomass burning in China.
Amino acids in atmospheric droplets: perturbation of surface tension and critical supersaturation predicted by computer simulations

Atmospheric amino acids constitute an important fraction of the water-soluble organic nitrogen compounds in both marine and continental aerosols, and have been confirmed as effective cloud condensation nuclei materials in laboratory tests. We here present a molecular dynamics study of amino acids representative for the remote marine atmospheric aerosol-cloud system, in order to investigate molecular distributions, orientations and induced changes in surface tension, and to evaluate their indirect effects on optical properties of clouds. These L-amino acids, including serine, glycine, alanine, valine, methionine and phenylalanine, are categorized as hydrophilic and hydrophobic according to their affinities to water. Different amino acids show distinct effects on the surface tension; even the same amino acid has different influence on the surface tension for planar and spherical interfaces. The curvature dependence of the surface tension is modelled by a quadratic polynomial function of the inverse of droplet radius, and such relationship is used to improve the Köhler equation in predicting the critical water vapour supersaturation of the droplet activation.
Absolute ozone absorption cross section in the Huggins Chappuis minimum (350–470 nm) at 296 K

We report the ozone absolute absorption cross section between 350–470 nm, the minimum between the Huggins and Chappuis bands, where the ozone cross section is less than 10−22 cm2. Ozone spectra were acquired using an incoherent broadband cavity enhanced absorption spectrometer, with three channels centered at 365, 405, and 455 nm. The accuracy of the measured cross section is 4–30%, with the greatest uncertainty near the minimum absorption at 375–390 nm. Previous measurements vary by more than an order of magnitude in this spectral region. The measurements reported here provide much greater spectral coverage than the most recent measurements. The effect of O3 concentration and water vapor partial pressure were investigated, however there were no observable changes in the absorption spectrum most likely due to the low optical density of the complex.