bluuebunny/crossref_metadata_2025 huggingface dataset:
On the transitions in marine boundary layer cloudiness
Authors: Sandu I. , Stevens B. , Pincus R.
Published: April 2010

Abstract. Satellite observations and meteorological reanalysis are used to examine the transition from unbroken sheets of stratocumulus to fields of scattered cumulus, and the processes controlling them, in four subtropical ocean basins. A Lagrangian analysis suggests that both the transition, defined as the temporal evolution in cloudiness, and the processes driving the transition, are quite similar among the oceanic basins. The transitions in marine boundary layer cloudiness are an extremely persistent feature of the subtropical ocean's environment, so that the transitions' characteristics obtained by documenting the flow of thousands of individual air masses are well reproduced by the mean (or climatological) fields of the different data sets. This opens new opportunities for future observations and modeling studies of these transitions.
Optimal estimation retrieval of aerosol microphysical properties from SAGE II satellite observations in the lower stratosphere
Authors: Wurl D. , Grainger R. G. , McDonald A. J. , Deshler T.
Published: April 2010

Abstract. A new retrieval algorithm is presented, which is based on the Optimal Estimation (OE) approach and aimed to improve current estimates of aerosol microphysical properties under non-volcanic conditions. The new OE algorithm retrieves log-normal particle size distribution parameters and associated uncertainties from multi-wavelength aerosol extinction data at visible to near infrared wavelengths. The algorithm was tested on synthetic data and then applied to SAGE (Stratospheric Aerosol and Gas Experiment) II data measured in 1999 in the lower stratosphere between 10 and 35 km. Model validation based on synthetic data shows that the new algorithm is able to retrieve the particle size of typical background aerosols accurately and that the retrieved uncertainties are a good estimate of the true errors. Aerosol properties retrieved from measured SAGE II extinction data (recorded in 1999) using the OE approach were compared to Principal Component Analysis (PCA) results retrieved from the same SAGE II data set. The OE surface area and volume densities are observed to be larger than the PCA values by 20–50% and 10–40% whereas the OE effective radii tend to be smaller by about 10–40%. An examination of the OE algorithm biases with in situ data indicates that the new OE estimates are likely to be more realistic than the PCA results. Based on the results of this study we suggest that the new OE retrieval algorithm provides improved estimates of aerosol properties in the lower stratosphere under low aerosol loading conditions.
Alkyl nitrate production and persistence in the Mexico City Plume
Authors: Perring A. E. , Bertram T. H. , Farmer D. K. , Wooldridge P. J. , Dibb J. , Blake N. J. , Blake D. R. , Singh H. B. , Fuelberg H. , Diskin G. , Sachse G. , Cohen R. C.
Published: April 2010

Abstract. Alkyl and multifunctional nitrates (ΣANs) have been observed to be a significant fraction of NOy in a number of different chemical regimes. Their formation is an important free radical chain termination step ending production of ozone and possibly affecting formation of secondary organic aerosol. ΣANs also represent a potentially large, unmeasured contribution to OH reactivity and are a major pathway for the removal of nitrogen oxides from the atmosphere. Numerous studies have investigated the role of nitrate formation from biogenic compounds. Less attention has been paid to the role ΣANs may play in the complex mixtures of hydrocarbons typical of urban settings. Measurements of ΣANs, NO2, total peroxy nitrates (ΣPNs), HNO3 and a wide suite of hydrocarbons were obtained from the NASA DC-8 aircraft during spring of 2006 in and around Mexico City and the Gulf of Mexico. ΣANs were observed to be 10–20% of NOy in the Mexico City plume and to increase in importance with increased photochemical age. We describe three conclusions: 1) Correlations of ΣANs with odd-oxygen (Ox) indicate a stronger role for ΣANs in the photochemistry of Mexico City than is expected based on currently accepted photochemical mechanisms, 2) ΣAN formation suppresses peak ozone production rates by as much as 30% in the near-field of Mexico City and 3) ΣANs play a comparable role to ΣPNs in the export of NOy to the Gulf Region.
Temporal variation of elemental carbon in Guangzhou, China, in summer 2006
Authors: Verma R. L. , Sahu L. K. , Kondo Y. , Takegawa N. , Han S. , Jung J. S. , Kim Y. J. , Fan S. , Sugimoto N. , Shammaa M. H. , Zhang Y. H. , Zhao Y.
Published: April 2010

Abstract. In situ measurements of the mass concentration of elemental carbon (EC) and mixing ratios of carbon monoxide (CO) and carbon dioxide (CO2) were made at Guangzhou, an urban measurement site in the Pearl River Delta (PRD), China, in July 2006. The average±standard deviation (SD) concentrations of EC, CO, and CO2 were 4.7±2.3 μg C m−3, 798±459 ppbv and 400±13 ppmv, respectively. The trends of these species were mainly controlled by synoptic-scale changes in meteorology during the campaign. Based on back trajectories, data are analyzed separately for two different air mass types representing northerly and southerly flows. Northerly air masses, constituting about 25% of the campaign, were mainly impacted by stagnant conditions, resulting in elevated levels of pollutants. On the other hand, southerly air masses measured during most of the campaign were mostly influenced by clean marine air. The diurnal patterns of EC, CO, and CO2 exhibited peak concentrations during the morning and evening hours coinciding with rush-hour traffic. The diurnal variations of EC and ΔEC/ΔCO closely followed the traffic pattern of heavy-duty vehicles (HDV) in Guangzhou, similar to that observed in Beijing. The level of EC in this campaign was similar to values reported during previous studies at other sites surrounding Guangzhou. The average slopes of ΔEC/ΔCO, ΔEC/ΔCO2, and ΔCO/ΔCO2 were 0.0054 μg C m−3/ppbv, 0.15 μg C m−3/ppmv, and 46.4 ppbv/ppmv, respectively, agreeing reasonably well with their respective emission ratios derived from regional emission inventories.
Surfactants in cloud droplet activation: mixed organic-inorganic particles
Authors: Prisle N. L. , Raatikainen T. , Laaksonen A. , Bilde M.
Published: April 2010

Abstract. Organic compounds with surfactant properties are commonly found in atmospheric aerosol particles. Surface activity can significantly influence the cloud droplet forming ability of these particles. We have studied the cloud droplet formation by two-component particles comprising one of the organic surfactants sodium octanoate, sodium decanoate, sodium dodecanoate, and sodium dodecyl sulfate, mixed with sodium chloride. Critical supersaturations were measured with a static diffusion cloud condensation nucleus counter (Wyoming CCNC-100B). Results were modeled from Köhler theory applying three different representations of surfactant properties: (1) using concentration-dependent surface tension reduction during droplet growth and explicitly accounting for surfactant surface partitioning in both solute suppression (Raoult effect) and curvature enhancement (Kelvin effect) contributions to the droplet equilibrium water vapor supersaturation, (2) disregarding surfactant partitioning and using a concentration-dependent surface tension for the droplets corresponding to a macroscopic (bulk) aqueous solution of the same overall composition, and (3) disregarding surfactant properties and assuming the constant surface tension of pure water throughout droplet activation. We confirm previous results for single-component organic surfactant particles, that experimental critical supersaturations are greatly underpredicted, if reduced surface tension is applied in Köhler theory while ignoring the effects of surface partitioning in droplets. We further show that assuming the constant surface tension of pure water can also lead to significant underpredictions of experimental critical supersaturations. The full account for surfactant partitioning in activating droplets generally predicts experimental critical supersaturations well. In addition, for mixed particles comprising less than 50% by mass of surfactant, ignoring surfactant properties and simply using the constant surface tension of pure water also provides a good first-order approximation of the observed activation.
Analysis of global and regional CO burdens measured from space between 2000 and 2009 and validated by ground-based solar tracking spectrometers
Authors: Yurganov L. N. , McMillan W. , Grechko E. , Dzhola A.
Published: April 2010

Abstract. CO total column (TC) retrievals from MOPITT version 3 and AIRS version 5 are validated through comparisons with archived TC data from the Network for Detection of Atmospheric Composition Change (NDACC) ground-based Fourier Transform Spectrometers (FTS) between March 2000 and December 2007. MOPITT retrievals exhibit an increasing temporal bias with a rate of 1.4–1.8% per year; thus far, AIRS retrievals appear to be more stable. For the lowest CO values in the Southern Hemisphere (SH), AIRS TC retrievals overestimate FTS TC by 20%. MOPITT's bias and standard deviation do not depend on CO TC absolute values. Empirical corrections are derived for AIRS and MOPITT retrievals based on the observed annually averaged bias versus the FTS TC. With these corrections, CO burdens from AIRS and MOPITT come into good agreement in the mid-latitudes of the Northern Hemisphere (NH) and in the tropical belt. In the SH, agreement between AIRS and MOPITT CO burdens is better for the larger CO TC in austral winter and worse in austral summer when CO TC are smaller. Interannual variations in AIRS and MOPITT retrieved CO burdens are compared with CO emissions from wild fires from the Global Fire Emission Dataset (GFED2) inventory. Before July 2008, all variations in retrieved CO burden can be explained by changes in fire emissions. After July 2008, global and tropical CO burdens decreased until October before recovering by the beginning of 2009. The NH CO burden also decreased but reached a minimum in January 2009 before starting to recover. The decrease in tropical CO burdens is explained by lower than usual fire emissions in South America and Indonesia. This decrease in topical emissions also accounts for most of the change in global CO burden. However, no such diminution of NH biomass burning is indicated by GFED2. Thus, the CO burden decrease in the NH could result from a combination of lower fossil fuel emissions during the global economic recession and transport of less CO from the tropics. More extensive modeling will be required to fully resolve this issue.
Heavy ozone enrichments from MIPAS limb emission spectra
Authors: Piccolo C. , Dudhia A. , Payne V. H.
Published: April 2010

Abstract. Vertical enrichment profiles of stratospheric heavy ozone (asymmetric and symmetric 50O3 isotopomers) have been derived from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). As a continuously operating satellite instrument, MIPAS has an advantage over previous measurements in providing global coverage over an extended time period, allowing the variations in enrichment to be determined. However, since the spectral features of the isotopomers are comparable with the magnitude of the instrument noise, a sequential estimation retrieval scheme has been used to average the measurements zonally. The magnitude of observed enrichments is ~10% in stratosphere, a value consistent with previous observations and lab measurements. The data indicate that asymmetric heavy ozone is significantly more enriched than the symmetric isotopomer and show latitudinal and vertical variations in both the asymmetric and symmetric 50O3 enrichments. Enrichments decrease with decreasing temperature, as previously noted, at midlatidudes and polar regions, while they increase with decreasing temperature in equatorial regions. MIPAS measurements contain also information on the asymmetric and symmetric 49O3 isotopomers. The enrichments of 49O3, obtained with the same sequential estimator approach, are much larger than the enrichments of 50O3, in contraddictions with previous results which predict larger enrichments for heavier isotopomers.
Isotope effect in the formation of H2 from H2CO studied at the atmospheric simulation chamber SAPHIR
Authors: Röckmann T. , Walter S. , Bohn B. , Wegener R. , Spahn H. , Brauers T. , Tillmann R. , Schlosser E. , Koppmann R. , Rohrer F.
Published: April 2010

Abstract. Formaldehyde of known, near-natural isotopic composition was photolyzed in a large photochemical reactor under ambient conditions. The isotopic composition of the product H2 was used to determine the isotope effects in formaldehyde photolysis. The experiments are sensitive to the molecular photolysis channel, and the radical channel has only a second order effect and can thus not be derived with high precision. The molecular channel kinetic isotope effect (KIEmol), the ratio of photolysis frequencies j(HCHO→CO+H2)/j(HCDO→CO+HD) under tropospheric conditions is determined to be KIEmol=1.63±0.03. Combining this result with the total KIE from a recent relative rate experiment, it is likely that KIEmol and KIErad are not as different as described previously in the literature.
Subseasonal variability of low cloud radiative properties over the southeast Pacific Ocean
Authors: George R. C. , Wood R.
Published: April 2010

Abstract. Subseasonal variability of cloud radiative properties in the persistent southeast Pacific stratocumulus deck is investigated using MODIS satellite observations and NCEP reanalysis data. A once-daily albedo proxy is derived based on the fractional coverage of low cloud (a macrophysical field) and the cloud albedo, with the latter broken down into contributions from microphysics (cloud droplet concentration) and macrophysics (liquid water path). Subseasonal albedo variability is dominated by the contribution of low cloud fraction variability, except within 10–15° of the South American coast, where cloud albedo variability contributes significantly. Covariance between cloud fraction and cloud albedo also contributes significantly and positively to the variance in albedo, which highlights how complex and inseparable the factors controlling albedo are. Droplet concentration variability contributes only weakly to the subseasonal variability of albedo, which emphasizes that attributing albedo variability to the indirect effects of aerosols against the backdrop of natural meteorological variability is extremely challenging. The dominant large scale meteorological variability is associated with the subtropical high pressure system. Two indices representing changes in the subtropical high strength and extent explain 80–90% of this variability, and significantly modulate the cloud microphysical, macrophysical, and radiative cloud properties. Variations in droplet concentration of up to 50% of the mean are associated with the meteorological driving. We hypothesize that these fluctuations in droplet concentration are a result of the large scale meteorology and their correlation with cloud macrophysical properties should not be used as evidence of aerosol effects. Mechanisms by which large scale meteorology affects cloud properties are explored. Our results support existing hypotheses linking cloud cover variability to changes in cold advection, subsidence, and lower tropospheric stability. Within 10° of the coast interactions between variability in the surface high pressure system and the orography appear to modulate both cloud macrophysical properties and aerosol transport through suppression of the marine boundary layer depth near the coast. This suggests one possible way in which cloud macrophysical properties and droplet concentration may be correlated independently of the second aerosol indirect effect. The results provide variability constraints for models that strive to represent both meteorological and aerosol impacts on stratocumulus clouds.
Secondary Organic Aerosol from biogenic VOCs over West Africa during AMMA
Authors: Capes G. , Murphy J. G. , Reeves C. E. , McQuaid J. B. , Hamilton J. F. , Hopkins J. R. , Crosier J. , Williams P. I. , Coe H.
Published: April 2010

Abstract. This paper presents measurements of organic aerosols above subtropical West Africa during the wet season using data from the UK Facility for Airborne Atmospheric Measurements (FAAM) aircraft. Measurements of biogenic volatile organic compounds (BVOC) at low altitudes over these subtropical forests were made during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment during July and August 2006 mainly above Benin, Nigeria and Niger. Data from an Aerodyne Quadrupole Aerosol Mass Spectrometer show a median organic aerosol loading of 1.08 μg m−3 over tropical West Africa, which represents the first regionally averaged assessment of organic aerosol mass (OM) in this region during the wet season. This is in good agreement with predictions based on aerosol yields from isoprene and monoterpenes during chamber studies and model predictions based on partitioning schemes, contrasting markedly with the large under representations of OM in similar models when compared with data from mid latitudes.
Chemical composition of PM10 and PM1 at the high-altitude Himalayan station Nepal Climate Observatory-Pyramid (NCO-P) (5079 m a.s.l.)
Authors: Decesari S. , Facchini M. C. , Carbone C. , Giulianelli L. , Rinaldi M. , Finessi E. , Fuzzi S. , Marinoni A. , Cristofanelli P. , Duchi R. , Bonasoni P. , Vuillermoz E. , Cozic J. , Jaffrezo J. L. , Laj P.
Published: April 2010

Abstract. We report chemical composition data for PM10 and PM1 from the Nepal Climate Observatory-Pyramid (NCO-P), the world's highest aerosol observatory, located at 5079 m a.s.l. at the foothills of Mt. Everest. Despite its high altitude, the average PM10 mass apportioned by the chemical analyses is of the order of 6 μg m−3 (i.e., 10 μg/scm), with almost a half of this mass accounted for by organic matter, elemental carbon (EC) and inorganic ions, the rest being mineral dust. Organic matter, in particular, accounted for by 2.0 μg m−3 (i.e., 3.6 μg/scm) on a yearly basis, and it is by far the major PM10 component beside mineral oxides. Non-negligible concentrations of EC were also observed (0.36 μg/scm), confirming that optically-active aerosol produced from combustion sources can be efficiently transported up the altitudes of Himalayan glaciers. The concentrations of carbonaceous and ionic aerosols follow a common time trend with a maximum in the premonsoon season, a minimum during the monsoon and a slow "ramp-up" period in the postmonsoon and dry seasons, which is the same phenomenology observed for other Nepalese Himalayan sites in previous studies. Such seasonal cycle can be explained by the seasonal variations of dry and moist convection and of wet scavenging processes characterizing the climate of north Indian subcontinent. We document the effect of orographic transport of carbonaceous and sulphate particles upslope the Himalayas, showing that the valley breeze circulation, which is almost permanently active during the out-of-monsoon season, greatly impacts the chemical composition of PM10 and PM1 in the high Himalayas and provides an efficient mechanism for bringing anthropogenic optically-active aerosols into the Asian upper troposphere (>5000 m a.s.l.). The concentrations of mineral dust are impacted to a smaller extent by valley breezes and follow a unique seasonal cycle which suggest multiple source areas in central and south-west Asia. Our findings, based on two years of observations of the aerosol chemical composition, provide clear evidence that the southern side of the high Himalayas are impacted by transport of anthropogenic aerosols which constitute the Asian brown cloud.
The radiative forcing potential of different climate geoengineering options
Authors: Lenton T. M. , Vaughan N. E.
Published: April 2010

Abstract. Climate geoengineering proposals seek to rectify the Earth's current radiative imbalance, either by reducing the absorption of incoming solar (shortwave) radiation, or by removing CO2 from the atmosphere and transferring it to long-lived reservoirs, thus increasing outgoing longwave radiation. A fundamental criterion for evaluating geoengineering options is their climate cooling effectiveness, which we quantify here in terms of radiative forcing potential. We use a simple analytical approach, based on the global energy balance and pulse response functions for the decay of CO2 perturbations. This aids transparency compared to calculations with complex numerical models, but is not intended to be definitive. Already it reveals some significant errors in existing calculations, and it allows us to compare the relative effectiveness of a range of proposals. By 2050, only stratospheric aerosol injections or sunshades in space have the potential to cool the climate back toward its pre-industrial state, but some land carbon cycle geoengineering options are of comparable magnitude to mitigation "wedges". Strong mitigation, i.e. large reductions in CO2 emissions, combined with global-scale air capture and storage, afforestation, and bio-char production, i.e. enhanced CO2 sinks, might be able to bring CO2 back to its pre-industrial level by 2100, thus removing the need for other geoengineering. Alternatively, strong mitigation stabilising CO2 at 500 ppm, combined with geoengineered increases in the albedo of marine stratiform clouds, grasslands, croplands and human settlements might achieve a patchy cancellation of radiative forcing. Ocean fertilisation options are only worthwhile if sustained on a millennial timescale and phosphorus addition probably has greater long-term potential than iron or nitrogen fertilisation. Enhancing ocean upwelling or downwelling have trivial effects on any meaningful timescale. Our approach provides a common framework for the evaluation of climate geoengineering proposals, and our results should help inform the prioritisation of further research into them.
Technical Note: Variance-covariance matrix and averaging kernels for the Levenberg-Marquardt solution of the retrieval of atmospheric vertical profiles
Authors: Ceccherini S. , Ridolfi M.
Published: April 2010

Abstract. The variance-covariance matrix (VCM) and the averaging kernel matrix (AKM) are widely used tools to characterize atmospheric vertical profiles retrieved from remote sensing measurements. Accurate estimation of these quantities is essential for both the evaluation of the quality of the retrieved profiles and for the correct use of the profiles themselves in subsequent applications such as data comparison, data assimilation and data fusion. We propose a new method to estimate the VCM and AKM of vertical profiles retrieved using the Levenberg-Marquardt iterative technique. We apply the new method to the inversion of simulated limb emission measurements. Then we compare the obtained VCM and AKM with those resulting from other methods already published in the literature and with accurate estimates derived using statistical and numerical estimators. The proposed method accounts for all the iterations done in the inversion and provides the most accurate VCM and AKM. The method can be easily implemented in any Levenberg-Marquardt iterative retrieval scheme, either constrained or unconstrained, without significant computational overhead.
Factors influencing the contribution of ion-induced nucleation in a boreal forest, Finland
Authors: Gagné S. , Nieminen T. , Kurtén T. , Manninen H. E. , Petäjä T. , Laakso L. , Kerminen V.-M. , Boy M. , Kulmala M.
Published: April 2010

Abstract. We present the longest series of measurements so far (2 years and 7 months) made with an Ion-DMPS at the SMEAR II measurement station in Hyytiälä, Southern Finland. We show that the classification of overcharged (implying some participation of ion-induced nucleation) and undercharged (implying no or very little participation of ion-induced nucleation) days based on Ion-DMPS measurements agrees with the fraction of ion-induced nucleation based on NAIS measurements. We analyzed the influence of different parameters on the contribution of ion-induced nucleation to the total particle formation rate. We found that the fraction of ion-induced nucleation is typically higher on warmer, drier and sunnier days compared to colder days with less solar radiation and a higher relative humidity. Also, we observed that bigger concentrations of new particles were produced on days with a smaller fraction of ion-induced nucleation. Moreover, sulfuric acid concentrations were smaller for days with a bigger fraction of ion-induced nucleation. Finally, we propose tentative explanations on how these different parameters influence the different nucleation mechanisms, and show that the different mechanisms seem to take place at the same time during an event. The relative contribution of the different mechanisms seems to vary depending on the surrounding conditions.
Solar cycle signals in sea level pressure and sea surface temperature
Authors: Roy I. , Haigh J. D.
Published: April 2010

Abstract. We identify solar cycle signals in 155 years of global sea level pressure (SLP) and sea surface temperature (SST) data using a multiple linear regression approach. In SLP we find in the North Pacific a statistically significant weakening of the Aleutian Low and a northward shift of the Hawaiian High in response to higher solar activity, confirming the results of previous authors. We also find a weak but broad reduction in pressure across the equatorial Pacific. In SST we identify a weak El Niño-like pattern in the tropics, unlike the strong La Niña-like signal found recently by some other authors. We show that the latter have been influenced by the technique of compositing data from peak years of the sunspot cycle as these years have often coincided with the negative phase of the ENSO cycle. Furthermore, the date of peak annual sunspot number generally falls a year or more in advance of the broader maximum of the 11-year solar cycle so that analyses which incorporate data from all years represent more coherently the difference between periods of high and low solar activity on these timescales.
Marine boundary layer over the subtropical southeast Pacific during VOCALS-REx – Part 1: Mean structure and diurnal cycle
Authors: Rahn D. A. , Garreaud R. D.
Published: April 2010

Abstract. Atmospheric subsidence over the subtropical southeast Pacific (SEP) leads to a low-level anticyclonic circulation, a cool sea surface and a cloud-topped marine boundary layer (MBL). Observations in this region from a major field campaign during October and November 2008, the VOCALS Regional Experiment, provide ample data to characterize the lower atmospheric features over the SEP. The observations are also useful to test the ability of an area-limited, high-resolution atmospheric model to simulate the SEP conditions. Observations and model-results (where appropriate) improve the characterization of the mean state (Part 1) and variability (Part 2) of the lower troposphere including circulation, MBL characteristics and the upsidence wave. Along 20° S the MBL is generally deeper offshore (1600 m at 85° W) but there is also considerable variability. MBL depth and variability decrease towards the coast and maximum inversion strength is detected between 74–76° W. Southeasterly trades prevail within the MBL although the wind speed decreases toward the coast. Above the MBL along the coast of Chile, flow is northerly, has a maximum at 3 km, and extends westward to ~74° W, apparently due to the mechanical blocking exerted by the Andes upon the westerly flow aloft. Mean MBL features along northern Chile (18–25° S) are remarkably similar (e.g., MBL depth just below 1 km) in spite of different SST. Observed diurnal cycles of the temperature at the coast and further offshore exhibit a number of conspicuous features that are consistent with the southwestward propagation of an upsidence wave initiated during late evening along the south Peru coast. Furthermore, the passage of the vertical motion results in either constructive or deconstructive interference with the radiatively-forced diurnal cycle of MBL depth.
Atmospheric transport of persistent semi-volatile organic chemicals to the Arctic and cold condensation at the mid-troposphere – Part 2: 3-D modeling of episodic atmospheric transport
Authors:   Lisheng Zhang,   Jianmin Ma,   Chongguo Tian,   Yifan Li
Published: April 2010

Abstract. Two 3-dimensional global atmospheric transport models for persistent organic pollutants (POPs) have been employed to investigate the association between the large-scale atmospheric motions and poleward transports of persistent semi-volatile organic chemicals (SVOCs). We examine the modeled daily air concentration of α- and γ-hexachlorocyclohexane (HCH) over a period from 1997–1999 during which a number of episodic atmospheric transport events were detected in this modeling study. These events provide modeling evidence for improving the interpretation on the cold condensation effect and poleward atmospheric transport of SVOCs at the mid-troposphere. Two episodic transport events of γ-HCH (lindane) to the high Arctic (80–90° N), one from Asian and another from Eurasian sources, are reported in this paper. The both events suggest that the episodic atmospheric transports occurring at the mid-troposphere (e.g. from 3000–5500 m height) are driven by atmospheric horizontal and vertical motions. The association of the transport events with atmospheric circulation is briefly discussed. Strong southerly winds, forced by the evolution of two semi-permanent high pressure systems over mid-high latitudes in the Northern Hemisphere, play an important role in the long-range transport (LRT) of HCHs to the high latitudes from its sources. Being consistent with the cold condensation effect and poleward atmospheric transport in a mean meridional atmospheric circulation simulated by a 2-D atmospheric transport model, as reported by the first part of this study, this modeling study indicates that cold condensation is likely occurring more intensively at the mid-troposphere where rapid declining air temperature results in condensed phase of the chemical over and near its source regions and where stronger winds convey the chemical more rapidly to the polar region during the episodic poleward atmospheric transport events.
Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview
Authors: Dall'Osto M. , Ceburnis D. , Martucci G. , Bialek J. , Dupuy R. , Jennings S. G. , Berresheim H. , Wenger J. C. , Sodeau J. R. , Healy R. M. , Facchini M. C. , Rinaldi M. , Giulianelli L. , Finessi E. , Worsnop D. , O'Dowd C. D.
Published: April 2010

Abstract. As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the NE Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm−3, while background marine air aerosol concentrations were between 400–600 cm−3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm−3, was observed and attributed to open ocean particle formation. Black carbon concentrations in polluted air were between 300–400 ng m−3, and in clean marine air were less than 50 ng m−3. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40–50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were highest in marine tropical air – even higher than in continental air. MSA was present at twice the concentrations of previously-reported concentrations at the same location and the same season. Both continental and marine air exhibited aerosol GFs significantly less than ammonium sulphate and even less in terms of sea salt aerosol pointing to a significant organic contribution to all air mass aerosol properties.
Spectroscopic studies of molecular iodine emitted into the gas phase by seaweed
Authors: Ball S. M. , Hollingsworth A. M. , Humbles J. , Leblanc C. , Potin P. , McFiggans G.
Published: April 2010

Abstract. Time profiles of molecular iodine emissions from seven species of seaweed have been measured at high time resolution (7.5 s) by direct spectroscopic quantification of the gas phase I2 using broadband cavity enhanced absorption spectroscopy. Substantial differences were found between species, both in the amounts of I2 emitted when the plants were exposed to air and in the shapes of their emission time profiles. Two species of kelp, Laminaria digitata and Laminaria hyperborea, were found to be the most potent emitters, producing an intense burst of I2 when first exposed to air. I2 was also observed from Saccharina latissima and Ascophyllum nodosum but in lower amounts and with broader time profiles. I2 mixing ratios from two Fucus species and Dictyopteris membranacea were at or below the detection limit of the present instrument (25 pptv). A further set of experiments investigated the time dependence of I2 emissions and aerosol particle formation when fragments of L. digitata were exposed to desiccation in air, to ozone and to oligoguluronate stress factors. Particle formation occurred in all L. digitata stress experiments where ozone and light were present, subject to the I2 mixing ratios being above certain threshold amounts. Moreover, the particle number concentrations closely tracked variations in the I2 mixing ratios, confirming the results of previous studies that the condensable particle-forming gases derive from the photochemical oxidation of the plant's I2 emissions. This work also supports the theory that particle nucleation in the coastal atmosphere occurs in "hot-spot" regions of locally elevated concentrations of condensable gases: the greatest atmospheric concentrations of I2 and hence of condensable iodine oxides are likely to be above plants of the most efficiently emitting kelp species and localised in time to shortly after these seaweeds are uncovered by a receding tide.
Chemically-resolved aerosol volatility measurements from two megacity field studies
Authors: Huffman J. A. , Docherty K. S. , Aiken A. C. , Cubison M. J. , Ulbrich I. M. , DeCarlo P. F. , Sueper D. , Jayne J. T. , Worsnop D. R. , Ziemann P. J. , Jimenez J. L.
Published: April 2010

Abstract. The volatilities of different chemical species in ambient aerosols are important but remain poorly characterized. The coupling of a recently developed rapid temperature-stepping thermodenuder (TD, operated in the range 54–230°C) with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during field studies in two polluted megacities has enabled the first direct characterization of chemically-resolved urban particle volatility. Measurements in Riverside, CA and Mexico City are generally consistent and show ambient nitrate as having the highest volatility of any AMS aerosol species while sulfate showed the lowest volatility. Total organic aerosol (OA) showed volatility intermediate between nitrate and sulfate, with an evaporation rate of 0.6% K−1 near ambient temperature, although OA dominates the residual species at the highest temperatures. Different types of OA were characterized with marker ions, diurnal cycles, and positive matrix factorization (PMF) and show significant differences in volatility. Reduced hydrocarbon-like OA (HOA, a surrogate for primary OA, POA), oxygenated OA (OOA, a surrogate for secondary OA, SOA), and biomass-burning OA (BBOA) separated with PMF were all determined to be semi-volatile. The most aged OOA-1 and its dominant ion, CO2+, consistently exhibited the lowest volatility, with HOA, BBOA, and associated ions for each among the highest. The similar or higher volatility of HOA/POA compared to OOA/SOA contradicts the current representations of OA volatility in most atmospheric models and has important implications for aerosol growth and lifetime. Our results strongly imply that all OA types should be considered semivolatile in models. The study in Riverside identified organosulfur species (e.g. CH3HSO3+ ion, likely from methanesulfonic acid), while both studies identified ions indicative of amines (e.g. C5H12N+) with very different volatility behaviors than inorganic-dominated ions. The oxygen-to-carbon ratio of OA in each ambient study was shown to increase both with TD temperature and from morning to afternoon, while the hydrogen-to-carbon ratio showed the opposite trend.
Black carbon aerosols and the third polar ice cap
Authors: Menon S. , Koch D. , Beig G. , Sahu S. , Fasullo J. , Orlikowski D.
Published: April 2010

Abstract. Recent thinning of glaciers over the Himalayas (sometimes referred to as the third polar region) have raised concern on future water supplies since these glaciers supply water to large river systems that support millions of people inhabiting the surrounding areas. Black carbon (BC) aerosols, released from incomplete combustion, have been increasingly implicated as causing large changes in the hydrology and radiative forcing over Asia and its deposition on snow is thought to increase snow melt. In India BC from biofuel combustion is highly prevalent and compared to other regions, BC aerosol amounts are high. Here, we quantify the impact of BC aerosols on snow cover and precipitation from 1990 to 2010 over the Indian subcontinental region using two different BC emission inventories. New estimates indicate that Indian BC from coal and biofuel are large and transport is expected to expand rapidly in coming years. We show that over the Himalayas, from 1990 to 2000, simulated snow/ice cover decreases by ~0.9% due to aerosols. The contribution of the enhanced Indian BC to this decline is ~30%, similar to that simulated for 2000 to 2010. Spatial patterns of modeled changes in snow cover and precipitation are similar to observations (from 1990 to 2000), and are mainly obtained with the newer BC estimates.
A comparison of dry and wet season aerosol number fluxes over the Amazon rain forest
Authors: Ahlm L. , Nilsson E. D. , Krejci R. , Mårtensson E. M. , Vogt M. , Artaxo P.
Published: April 2010

Abstract. Vertical number fluxes of aerosol particles and vertical fluxes of CO2 were measured with the eddy covariance method at the top of a 53 m high tower in the Amazon rain forest as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) experiment. The observed aerosol number fluxes included particles with sizes down to 10 nm in diameter. The measurements were carried out during the wet and dry season in 2008. In this study focus is on the dry season aerosol fluxes, with significant influence from biomass burning, and these are compared with aerosol fluxes measured during the wet season. The primary goal is to quantify the dry deposition sink and to investigate whether particle deposition velocities change when going from the clean wet season into the more polluted dry season. Furthermore, it is tested whether the rain forest is always a net sink of particles in terms of number concentrations, or if particle emission from the surface under certain circumstances may dominate over the dry deposition sink. The particle deposition velocity vd increased linearly with increasing friction velocity in both seasons and the relations are described by vdd=(2.7 u* −0.2)×10−3 (dry season) and vdw=2.5 u*×10−3 (wet season), where u* is the friction velocity. The fact that the two relations are very similar to each other indicates that the seasonal change in aerosol number size distribution is not enough for causing any significant change in deposition velocity. In general, particle deposition velocities in this study are low compared to studies over boreal forests. The reason is probably domination of accumulation mode particles in the Amazon boundary layer, both in the dry and wet season, and low wind speeds in the tropics compared to the midlatitudes. Net particle deposition fluxes prevailed in daytime in both seasons and the deposition flux was considerably larger in the dry season due to the much higher dry season particle concentration. In the dry season, nocturnal particle fluxes behaved very similar to the nocturnal CO2 fluxes. Throughout the night, the measured particle flux at the top of the tower was close to zero, but early in the morning there was an upward particle flux peak that is not likely a result of entrainment or local pollution. It is possible that these morning upward particle fluxes are associated with emission of natural biogenic particles from the rain forest. Emitted particles may be stored within the canopy during stable conditions at nighttime, similarly to CO2, and being released from the canopy when conditions become more turbulent in the morning.
Nitrogen oxide chemistry in an urban plume: investigation of the chemistry of peroxy and multifunctional organic nitrates with a Lagrangian model
Authors: Pérez I. M. , LaFranchi B. W. , Cohen R. C.
Published: April 2010

Abstract. Air quality in the outflow from urban centers affects millions of people, as well as, natural and managed ecosystems downwind. In locations where there are large sources of biogenic VOCs downwind of urban centers, the outflow is characterized by a high VOC reactivity due to biogenic emissions and low NOx. However most field and chamber studies have focused on limiting cases of high NOx or of near zero NOx. Recent measurements of a wide suite of VOCs, O3 and meteorological parameters at several locations within the Sacramento urban plume have provided a detailed benchmark for testing our understanding of chemistry in a plume transitioning from high NOx to low NOx and high VOC reactivity. As an additional simplification, the strong mountain valley circulation in the region makes this urban plume a physical realization of a nearly idealized Lagrangian plume. Here, we describe a model of this plume. We use a Lagrangian model representing chemistry based on the Master Chemical Mechanism (MCM) v3.1 along with mixing and deposition. We discuss the effects of entrainment of background air, the branching ratio for the production of isoprene nitrates and the effects of soil NOx emissions on the composition of the evolving plume. The model predicts that after 2–3 h of chemical processing only 45% of the peroxynitrates (ΣPNs) are PAN and that most (69%) RONO2 are secondary alkyl nitrate products of the reaction of OH with RONO2. We find the model is more consistent with the observations if: a) the yield of ΣPNs from large and multi-functional aldehydes is close to zero; and b) the reaction between OH and RONO2 produces multifunctional nitrates as opposed to either HNO3 or NO2 as is typical in most currently adopted reaction mechanisms. Model results also show that adding NOx emissions throughout the transect increases the available NOx in the downwind regions, but modeled ozone concentrations were little affected by the increased NOx.
Effects of temperature and other atmospheric conditions on long-term gaseous mercury observations in the Arctic
Authors: Cole A. S. , Steffen A.
Published: April 2010

Abstract. Gaseous elemental mercury (GEM) measurements at Alert, Canada, from 1995 to 2007 were analyzed for statistical time trends and for correlations with meteorological and climate data. A significant decreasing trend in annual GEM concentration is reported at Alert, with an estimated slope of −0.0086 ng m−3 yr−1 (−0.6% yr−1) over this 13-year period. It is shown that there has been a shift in the month of minimum mean GEM concentration from May to April due to a change in the timing of springtime atmospheric mercury depletion events (AMDEs). These AMDEs are found to decrease with increasing local temperature within each month, both at Alert and at Amderma, Russia. These results agree with the temperature dependence suggested by previous experimental results and theoretical kinetic calculations and highlight the potential for changes in Arctic mercury chemistry with climate. A correlation between total monthly AMDEs at Alert and the Polar/Eurasian Teleconnection Index was observed only in March, perhaps due to higher GEM inputs in early spring in those years with a weak polar vortex. A correlation of AMDEs at Alert with wind direction supports the origin of mercury depletion events over the Arctic Ocean, in agreement with a previous trajectory study of ozone depletion events. Interannual variability in total monthly depletion event frequency at Alert does not appear to correlate significantly with total or first-year northern hemispheric sea ice area or with other major teleconnection patterns. Nor do AMDEs at either Alert or Amderma correlate with local wind speed, as might be expected if depletion events are sustained by stable, low-turbulence atmospheric conditions. The data presented here – both the change in timing of depletion events and their relationship with temperature – can be used as additional constraints to improve the ability of global models to predict the cycling and deposition of mercury in the Arctic.