bluuebunny/crossref_metadata_2025 huggingface dataset:
Regional aerosol optical properties and radiative impact of the extreme smoke event in the European Arctic in spring 2006
Authors: Lund Myhre C. , Toledano C. , Myhre G. , Stebel K. , Yttri K. E. , Aaltonen V. , Johnsrud M. , Frioud M. , Cachorro V. , de Frutos A. , Lihavainen H. , Campell J. R. , Chaikovsky A. P. , Shiobara M. , Welton E. J. , Tørseth K.
Published: April 2010

Abstract. In spring 2006 a special meteorological situation occurred in the European Arctic region giving record high levels of air pollution. The synoptic situation resulted in extensive transport of pollution predominantly from agricultural fires in Eastern Europe into the Arctic region and record high air-pollution levels were measured at the Zeppelin observatory at Ny-Ålesund (78°54' N, 11°53' E) in the period from 25 April to 12 May. In the present study we investigate the optical properties of the aerosols from this extreme event and we estimate the radiative forcing of this episode. We examine the aerosol optical properties from the source region and into the European Arctic and explore the evolution of the episode and the changes in the optical properties. A number of sites in Eastern Europe, Northern Scandinavia and Svalbard are included in the study. In addition to AOD measurements, we explored lidar measurements from Minsk, ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research at Andenes) and Ny-Ålesund. For the AERONET sites included (Minsk, Toravere, Hornsund) we have further studied the evolution of the aerosol size. Importantly, at Svalbard it is consistency between the AERONET measurements and calculations of single scattering albedo based on aerosol chemical composition. We have found strong agreement between the satellite daily MODIS AOD and the ground-based AOD observations. This agreement is crucial for the radiative forcing calculations. We calculate a strong negative radiative forcing for the most polluted days employing the analysed ground based data, MODIS AOD and a multi-stream model for radiative transfer of solar radiation.
Asian dust storm influence on North American ambient PM levels: observational evidence and controlling factors
Authors: Zhao T. L. , Gong S. L. , Zhang X. Y. , Jaffe D. A.
Published: April 2010

Abstract. New observational evidence of the trans-Pacific transport of Asian dust and its contribution to the ambient particulate matter (PM) levels in North America was revealed, based on the interannual variations between Asian dust storms and the ambient PM levels in western North America from year 2000 to 2006. A high correlation was found between them with an R2 value of 0.83. From analysis of the differences in the correlation between 2005 and 2006, three factors explain the variation of trans-Pacific transport and influences of Asian dust storms on PM levels in western North America. These were identified by modeling results and the re-analysis data. They were 1) Strength of frontal cyclones from Mongolia to north eastern China: The frontal cyclones in East Asia not only bring strong cold air outbreaks, generating dust storms in East Asia, but also lift Asian dust into westerly winds of the free troposphere for trans-Pacific transport; 2) Pattern of transport pathway over the North Pacific: The circulation patterns of westerlies over the North Pacific govern the trans-Pacific transport pattern. Strong zonal airflow of the westerly jet in the free troposphere over the North Pacific favor significant trans-Pacific transport of Asian dust; 3) Variation of precipitation in the North Pacific: The scavenging of Asian dust particles by precipitation is a major process of dust removal on the trans-Pacific transport pathway; therefore, variation of precipitation in the North Pacific could affect trans-Pacific transport of Asian dust.
Efficiency of immersion mode ice nucleation on surrogates of mineral dust
Authors: Marcolli C. , Gedamke S. , Peter T. , Zobrist B.
Published: April 2010

Abstract. A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in heterogeneous CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.
Impact of using different ozone cross sections on ozone profile retrievals from Global Ozone Monitoring Experiment (GOME) ultraviolet measurements
Authors: Liu X. , Chance K. , Sioris C. E. , Kurosu T. P.
Published: April 2010

Abstract. We investigate the effect of using three different cross section data sets on ozone profile retrievals from Global Ozone Monitoring Experiment (GOME) ultraviolet measurements (289–307 nm, 326–337 nm). These include Bass-Paur, Brion, and GOME flight model cross sections (references below). Using different cross sections can significantly affect the retrievals, by up to 12 Dobson Units (DU, 1 DU=2.69×1016 molecules cm−2) in total column ozone, up to 10 DU in tropospheric column ozone, and up to 100% in retrieved ozone values for individual atmospheric layers. Compared to using the Bass-Paur and GOME flight model cross sections, using the Brion cross sections not only reduces fitting residuals by 15–60% in the Huggins bands, but also improves retrievals, especially in the troposphere, as seen from validation against ozonesonde measurements. Therefore, we recommend using the Brion cross section for ozone profile retrievals from ultraviolet measurements. The total column ozone retrieved using the GOME flight model cross sections is systematically lower, by 7–10 DU, than that retrieved using the Brion and Bass-Paur cross sections and is also systematically lower than Total Ozone Mapping Spectrometer (TOMS) observations. This study demonstrates the need for improved ozone cross section measurements in the ultraviolet to improve profile retrievals of this key atmospheric constituent.
Performance of MAX-DOAS measurements of aerosols at Tsukuba, Japan: a comparison with lidar and sky radiometer measurements
Authors: Irie H. , Kanaya Y. , Akimoto H. , Iwabuchi H. , Shimizu A. , Aoki K.
Published: April 2010

Abstract. Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed at Tsukuba, Japan (36.1° N, 140.1° E), in November–December 2006. The measured spectra of scattered sunlight are analyzed by DOAS and optimal estimation methods to retrieve the aerosol optical depth (τ) and the vertical profile of the aerosol extinction coefficient (σ) at 476 nm in the lower troposphere. We characterize these retrieved quantities through comparisons with coincident lidar and sky radiometer measurements. The retrieved σ values for layers of 0–1 and 1–2 km agree with lidar data to within 30% and 60%, respectively, for most cases, including partly cloudy conditions. Results similar to σ at 0–1 km are obtained for the retrieved τ values, demonstrating that MAX-DOAS provides the new, unique aerosol dataset in the lower troposphere.
The Response of surface ozone to climate change over the Eastern United States
Authors: Racherla P. N. , Adams P. J.
Published: April 2010

Abstract. We examined the response of surface ozone to future climate change over the eastern United States by performing simulations corresponding to present (1990s) and future (2050s) climates using an integrated model of global climate, tropospheric gas-phase chemistry, and aerosols. A future climate has been imposed using ocean boundary conditions corresponding to the IPCC SRES A2 scenario for the 2050 s decade, resulting in an increase in the global annual-average surface air temperature by 1.7°C, with a 1.4°C increase over the surface layer of the eastern United States. Present-day anthropogenic emissions and CO2/CH4 mixing ratios have been used in both simulations while climate-sensitive natural emissions were allowed to vary with the simulated climate. There is practically zero change in the spatiotemporally averaged ozone mixing ratios predicted over the eastern United States. However, the severity and frequency of ozone episodes over the eastern United States increased due to future climate change, primarily as a result of increased ozone chemical production due to increased natural isoprene emissions. The 95th percentile ozone mixing ratio increased by 5 ppbv and the largest frequency increase occured in the 80–90 ppbv range. The most substantial and statistically significant (p-value <0.05) increases in episode frequency occurred over the southeast and midatlantic United States, largely as a result of 20% higher annual-average natural isoprene emissions. Increased chemical production and shorter average lifetime are consistent features of the predicted seasonal surface ozone response, with the former's magnitude for a location largely a function of increased natural isoprene emissions, and the latter largely due to faster dry deposition removal rates. Future climate change is also predicted to lengthen the ozone season over the eastern United States to include late spring and early fall. Significant interannual variability is observed in the frequency of ozone episodes and we find that it is necessary to utilize 5 years or more of simulation data in order to separate the effects of interannual variability and climate change on ozone episodes.
Methane spectroscopy in the near infrared and its implication on atmospheric retrievals
Authors: Frankenberg C. , Warneke T. , Butz A. , Aben I. , Hase F. , Spietz P. , Brown L. R.
Published: April 2010

Abstract. N2-broadened half widths and pressure shifts were obtained for transitions in the Q and R branches of the 2ν3 methane band. Laboratory measurements were done from 5985 to 6185 cm−1 using spectra recorded at 0.011 cm−1 resolution with a Bruker 120 HR Fourier transform spectrometer. A 140 cm gas cell was filled with methane at room temperature and N2 as foreign gas at pressures ranging from 125 to 900 hPa. A multispectrum nonlinear constrained least squares approach based on Optimal Estimation was applied to derive the spectroscopic parameters by simultaneously fitting laboratory spectra at different ambient pressures assuming a Voigt line-shape. At room temperature, the half widths ranged between 0.030 and 0.071 cm−1 atm−1, and the pressure shifts varied from −0.002 to −0.025 cm−1 atm−1 for transitions up to J"=10. Especially for higher rotational levels, we find systematically narrower lines than HITRAN predicts. The new set of spectroscopic parameters is further tested with ground based direct sun FTIR measurements where fit residuals reduce by about a factor of 3–4. We report the implication of those differences on atmospheric methane measurements using high-resolution ground based FTIR measurements as well as low-resolution spectra from the SCIAMACHY instrument onboard ENVISAT. We find that for SCIAMACHY, a latitudinal and seasonally varying bias of about 1% can be introduced by erroneous broadening parameters.
Estimation of the mass absorption cross section of the organic carbon component of aerosols in the Mexico City Metropolitan Area (MCMA)
Authors: Barnard J. C. , Volkamer R. , Kassianov E. I.
Published: April 2010

Abstract. Data taken from the MCMA-2003 and the 2006 MILAGRO field campaigns are used to examine the absorption of solar radiation by the organic component of aerosols. Using irradiance data from a Multi-Filter Rotating Shadowband Radiometer (MFRSR) and an actinic flux spectroradiometer (SR), we derive aerosol single scattering albedo, π0,λ, as a function of wavelength, λ. We find that in the near-UV spectral range (250 to 400 nm) π0,λ is much lower compared to π0,λ at 500 nm indicating enhanced absorption in the near-UV range. Absorption by elemental carbon, dust, or gas cannot account for this enhanced absorption leaving the organic part of the aerosol as the only possible absorber. We use data from a surface deployed Aerodyne Aerosol Mass Spectrometer (AMS) along with the inferred π0,λ to estimate the Mass Absorption Cross section (MAC) for the organic carbon. We find that the MAC is about 10.5 m2/g at 300 nm and falls close to zero at about 500 nm; values that are roughly consistent with other estimates of organic carbon MAC. These MAC values can be considered as "radiatively correct" because when used in radiative transfer calculations the calculated irradiances/actinic fluxes match those measured at the wavelengths considered here. For an illustrative case study described here, we estimate that the light absorption by the "brown" (organic) carbonaceous aerosol can add about 40% to the light absorption of black carbon in Mexico City. This contribution will vary depending on the relative abundance of organic carbon relative to black carbon. Furthermore, our analysis indicates that organic aerosol would slow down photochemistry by selectively scavenging the light reaching the ground at those wavelengths that drive photochemical reactions. Finally, satellite retrievals of trace gases that are used to infer emissions currently assume that the MAC of organic carbon is zero. For trace gases that are retrieved using wavelengths shorter then 420 nm (i.e. SO2, HCHO, halogenoxides, NO2), the assumption of non-zero MAC values will induce an upward correction to the inferred emissions. This will be particularly relevant in polluted urban atmospheres and areas of biomass burning where organic aerosols are particularly abundant.
Measurements of size-resolved hygroscopicity in the California coastal zone
Authors: Hegg D. A. , Covert D. S. , Jonsson H. H.
Published: April 2010

Abstract. Aircraft – based measurements of aerosol hygroscopicity, both in the form of size-resolved, diameter growth factors and in the dependence of particle light scattering on relative humidity, are presented for the marine boundary layer of the southern California coastal zone. The chemical composition of the aerosol is collated with the hygroscopicity data, both to examine the nature of aerosol aging and as input for receptor type modeling. The data suggest an increase in aerosol hygroscopicity with altitude, possibly associated with oxidation of organic films. The receptor modeling suggests three distinct aerosol types/sources for this venue: marine, biomass burning and pollution. Model output is used in regression analyses to derive a prognostic mixing rule for the hygroscopicity of aerosol with these three sources.
Mixing processes and exchanges in the tropical and the subtropical UT/LS
Authors: James R. , Legras B.
Published: April 2010

Abstract. Both in situ measurements and satellite observations indicate evidence of mixing in the upper troposphere (UT) and the lower-stratosphere (LS). In this study, the measurements performed during the Pre-AVE and Costa-Rica AVE campaigns are analysed with diffusive back-trajectories to assess mixing properties in the tropical and the subtropical UT/LS. A description of cross-tropopause pathways and mixing time scales is provided. In the subtropics, Troposphere-Stratosphere mixing processes are found to differ in the vicinity of the tropopause and at higher altitudes. Below 350 K, the mixing line observed during Pre-AVE is shown to result from fast and local cross-tropopause irreversible exchange, involving two initially distant air masses with distinct chemical compositions. For measurements located above 350 K, mixing of the tropospheric air in the subtropical stratosphere occurs over a period of a month, the origins of the tropospheric source being localised in the tropical UT and the tropical boundary layer. In the tropics, quantitative reconstructions of CO and O3 profiles above 360 K are obtained for one month back-trajectories calculations, pointing out that long term mixing is essential to determine the chemical composition in the tropical ascent. In particular, the existence of two-way meridional irreversible exchanges between 360 and 450 K is found to export tropical air in the subtropical stratosphere and to entrain old stratospheric air in the tropical ascent. Calculations of the Lagrangian mean age of air is shown to be in qualitative agreement with the CO2 observations and diabatic calculations.
Atmospheric chemistry of trans-CF3CH=CHF: products and mechanisms of hydroxyl radical and chlorine atom initiated oxidation
Authors: Javadi M. S. , Søndergaard R. , Nielsen O. J. , Hurley M. D. , Wallington T. J.
Published: April 2010

Abstract. Smog chamber/FTIR techniques were used to study the products and mechanisms of OH radical and Cl atom initiated oxidation of trans-CF3CH=CHF in 700 Torr of N2/O2 diluent at 295±1 K. Hydroxyl radical initiated oxidation leads to the formation of CF3CHO and HC(O)F in yields which were indistinguishable from 100% and were not dependent on the O2 partial pressure. Chlorine atom initiated oxidation gives HC(O)F, CF3CHO, CF3C(O)Cl, and CF3C(O)CHFCl. The yields of CF3C(O)Cl and CF3C(O)CHFCl increased at the expense of HC(O)F and CF3CHO as the O2 partial pressure was increased over the range 5–700 Torr. The results are discussed with respect to the atmospheric chemistry and environmental impact of trans-CF3CH=CHF.
Aerosol model selection and uncertainty modelling by adaptive MCMC technique
Authors: Laine M. , Tamminen J.
Published: April 2010

Abstract. We apply Bayesian model selection techniques on the statistical inversion problem of the GOMOS instrument. The motif is to study which type of aerosol model best fits the data and to show how the uncertainty of the aerosol model can be included in the error estimates. The competing models consist of various formulations, each having different unknown parameter vectors. We have developed an Adaptive Automatic Reversible Jump Markov chain Monte Carlo method (AARJ) for sampling values from the posterior distributions of the unknowns of the models. The algorithm is easy to implement and can readily be employed for model selection as well as for model averaging, to properly take into account the uncertainty of the modelling.
SO2 Retrieval from SCIAMACHY using the Weighting Function DOAS (WFDOAS) Technique: comparison with Standard DOAS retrieval
Authors: Lee C. , Richter A. , Weber M. , Burrows J. P.
Published: April 2010

Abstract. Atmospheric SO2 can be measured by remote sensing of scattered sunlight from space, using its unique absorption features in the ultraviolet region. However, the sensitivity of the SO2 measurement depends critically on spectral interference, surface albedo and varies with wavelength as Rayleigh scattering increases at shorter wavelengths. The Weighting Function Differential Optical Absorption Spectroscopy (WFDOAS) method was used to solve these problems. The Ring spectra included in the WFDOAS fit were determined as a function of total ozone column density, solar zenith angle, surface albedo, and effective scene altitude. The WFDOAS SO2 retrieval from SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) data onboard the ENVISAT satellite are presented here and compared to those of the Standard DOAS (SDOAS) method for cases of background conditions and volcanic eruption. The study demonstrates that the problems in the SO2 retrieval with SDOAS, such as the positive offsets over remote (clean) regions and the negative offsets at high solar zenith angles and high ozone, can be solved by the WFDOAS approach.
Concatenated non-stationary dispersive scenarios on complex terrain under summer conditions
Authors: Palau J. L. , Pérez-Landa G. , Millán M. M.
Published: April 2010

Abstract. The results and discussions presented in this paper arise from a statistically representative study of the physical processes associated with the multimodal distribution of pollutants aloft and around a 343-m-tall chimney under summer conditions in the Iberian Peninsula. The indetermination of a transversal plume to the preferred transport direction during transitional periods implies a small (or null) physical significance of the classical definition of horizontal standard deviation of the concentration distribution. By experimentation and modelling, this paper analyses the atmospheric dispersion of the SO2 emissions from a power plant on complex terrain, describing the main dispersion features as an ensemble of "stationary dispersive scenarios" and reformulating some "classical" dispersive concepts to deal with the systematically monitored summer dispersive scenarios in inland Spain.
Attribution of aerosol light absorption to black carbon, brown carbon, and dust in China – interpretations of atmospheric measurements during EAST-AIRE
Authors: Yang M. , Howell S. G. , Zhuang J. , Huebert B. J.
Published: April 2010

Abstract. Black carbon, brown carbon, and mineral dust are three of the most important light absorbing aerosols. Their optical properties differ greatly and are distinctive functions of the wavelength of light. Most optical instruments that quantify light absorption, however, are unable to distinguish one type of absorbing aerosol from another. It is thus instructive to separate total absorption from these different light absorbers to gain a better understanding of the optical characteristics of each aerosol type. During the EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) campaign near Beijing, we measured light scattering using a nephelometer, and light absorption using an aethalometer and a particulate soot absorption photometer. We also measured the total mass concentrations of carbonaceous (elemental and organic carbon) and inorganic particulates, as well as aerosol number and mass distributions. We were able to identify periods during the campaign that were dominated by dust, biomass burning, fresh (industrial) chimney plumes, other coal burning pollution, and relatively clean (background) air for Northern China. Each of these air masses possessed distinct intensive optical properties, including the single scatter albedo and Ångstrom exponents. Based on the wavelength-dependence and particle size distribution, we apportioned total light absorption to black carbon, brown carbon, and dust; their mass absorption efficiencies at 550 nm were estimated to be 9.5, 0.5, and 0.03 m2/g, respectively. While agreeing with the common consensus that BC is the most important light absorber in the mid-visible, we demonstrated that brown carbon and dust could also cause significant absorption, especially at shorter wavelengths.
Correlation between cloud condensation nuclei concentration and aerosol optical thickness in remote and polluted regions
Authors: Andreae M. O.
Published: April 2010

Abstract. A large number of published and unpublished measurements of cloud condensation nuclei (CCN) concentrations and aerosol optical thickness (AOT) measurements have been analyzed. AOT measurements were obtained mostly from the AERONET network, and selected to be collocated as closely as possible to the CCN investigations. In remote marine regions, CCN0.4 (CCN at a supersaturation of 0.4%) are around 110 cm−3 and the mean AOT500 (AOT at 500 nm) is 0.057. Over remote continental areas, CCN are almost twice as abundant, while the mean AOT500 is ca. 0.075. (Sites dominated by desert dust plumes were excluded from this analysis.) Some, or maybe even most of this difference must be because even remote continental sites are in closer proximity to pollution sources than remote marine sites. This suggests that the difference between marine and continental levels must have been smaller before the advent of anthropogenic pollution. Over polluted marine and continental regions, the CCN concentrations are about one magnitude higher than over their remote counterparts, while AOT is about five times higher over polluted than over clean regions. The average CCN concentrations from all studies show a remarkable correlation to the corresponding AOT values, which can be expressed as a power law. This can be very useful for the parameterization of CCN concentrations in modeling studies, as it provides an easily measured proxy for this variable, which is difficult to measure directly. It also implies that, at least at large scales, the radiative and microphysical effects of aerosols on cloud physics are correlated and not free to vary independently. While this strong empirical correlation is remarkable, it must still be noted that that there is about a factor-of-four range of CCN concentrations at a given AOT, and that there remains considerable room for improvement in remote sensing techniques for measuring CCN abundance.
Gas phase precursors to anthropogenic secondary organic aerosol: detailed observations of 1,3,5-trimethylbenzene photooxidation
Authors: Wyche K. P. , Monks P. S. , Ellis A. M. , Cordell R. L. , Parker A. E. , Whyte C. , Metzger A. , Dommen J. , Duplissy J. , Prevot A. S. H. , Baltensperger U. , Rickard A. R. , Wulfert F.
Published: April 2010

Abstract. A series of photooxidation experiments were conducted in an atmospheric simulation chamber in order to investigate the secondary organic aerosol (SOA) formed from the anthropogenic model gas phase precursor, 1,3,5-trimethylbenzene. Alongside specific aerosol measurements, comprehensive gas phase measurements, primarily by chemical ionisation reaction time-of-flight mass spectrometry (CIR-TOF-MS), were carried out to provide detailed insight into the composition and behaviour of the organic components of the gas phase matrix during SOA formation. An array of gas phase organic compounds was measured during the oxidation process, including several previously unmeasured primary bicyclic compounds possessing various functional groups. Analysis of results obtained during this study implies that these peroxide bicyclic species along with a series of furanones and organic acids contribute to SOA growth. The effect of varying the VOC/NOx ratio on SOA formation was explored, as was the effect of acid seeding. It was found that low NOx conditions favour more rapid aerosol formation and a higher aerosol yield, a finding that points towards a role for organic peroxides in the nucleation process and SOA growth.
Simulating mixed-phase Arctic stratus clouds: sensitivity to ice initiation mechanisms
Authors: Sednev I. , Menon S. , McFarquhar G.
Published: April 2010

Abstract. The importance of Arctic mixed-phase clouds on radiation and the Arctic climate is well known. However, the development of mixed-phase cloud parameterization for use in large scale models is limited by lack of both related observations and numerical studies using multidimensional models with advanced microphysics that provide the basis for understanding the relative importance of different microphysical processes that take place in mixed-phase clouds. To improve the representation of mixed-phase cloud processes in the GISS GCM we use the GISS single-column model coupled to a bin resolved microphysics (BRM) scheme that was specially designed to simulate mixed-phase clouds and aerosol-cloud interactions. Using this model with the microphysical measurements obtained from the DOE ARM Mixed-Phase Arctic Cloud Experiment (MPACE) campaign in October 2004 at the North Slope of Alaska, we investigate the effect of ice initiation processes and Bergeron-Findeisen process (BFP) on glaciation time and longevity of single-layer stratiform mixed-phase clouds. We focus on observations taken during 9th–10th October, which indicated the presence of a single-layer mixed-phase clouds. We performed several sets of 12-h simulations to examine model sensitivity to different ice initiation mechanisms and evaluate model output (hydrometeors' concentrations, contents, effective radii, precipitation fluxes, and radar reflectivity) against measurements from the MPACE Intensive Observing Period. Overall, the model qualitatively simulates ice crystal concentration and hydrometeors content, but it fails to predict quantitatively the effective radii of ice particles and their vertical profiles. In particular, the ice effective radii are overestimated by at least 50%. However, using the same definition as used for observations, the effective radii simulated and that observed were more comparable. We find that for the single-layer stratiform mixed-phase clouds simulated, process of ice phase initiation due to freezing of supercooled water in both saturated and undersaturated (w.r.t. water) environments is as important as primary ice crystal origination from water vapor. We also find that the BFP is a process mainly responsible for the rates of glaciation of simulated clouds. These glaciation rates cannot be adequately represented by a water-ice saturation adjustment scheme that only depends on temperature and liquid and solid hydrometeors' contents as is widely used in bulk microphysics schemes and are better represented by processes that also account for supersaturation changes as the hydrometeors grow.
Measurements of volatile organic compounds using proton transfer reaction – mass spectrometry during the MILAGRO 2006 Campaign
Authors: Fortner E. C. , Zheng J. , Zhang R. , Knighton W. B. , Molina L.
Published: April 2010

Abstract. Volatile organic compounds (VOCs) were measured by proton transfer reaction – mass spectrometry (PTR-MS) on a rooftop in the urban mixed residential and industrial area North Northeast of downtown Mexico City as part of the Megacity Initiative – Local and Global Research Observations (MILAGRO) 2006 field campaign. Thirty eight individual masses were monitored during the campaign and many species were quantified including methanol, acetaldehyde, toluene, the sum of C2 benzenes, the sum of C3 benzenes, acetone, isoprene, benzene, and ethyl acetate. The VOC measurements were analyzed to gain a better understanding of the type of VOCs present in this region of the MCMA, their diurnal patterns and their origins. Diurnal profiles of weekday and weekend/holiday aromatic VOC concentrations show the influence of vehicular traffic during the morning rush hours and during the afternoon hours. Plumes including of elevated toluene as high as 216 parts per billion (ppb) and ethyl acetate as high as 183 ppb were frequently observed during the late night and early morning hours, indicating the probability of significant industrial sources of the two compounds in the region. Wind fields during those peak episodes revealed no specific direction for the majority of the toluene plumes but the ethyl acetate plumes arrived at the site when winds were from the Southwest or West. The PTR-MS measurements combined with other VOC measuring techniques at the field site as well as VOC measurements conducted in other areas of the Mexico City Metropolitan Area (MCMA) will help to develop a better understanding of the spatial pattern of VOCs and its variability in the MCMA.
Ten years of CO2, CH4, CO and N2O fluxes over Western Europe inferred from atmospheric measurements at Mace Head, Ireland
Authors: Messager C. , Schmidt M. , Ramonet M. , Bousquet P. , Simmonds P. , Manning A. , Kazan V. , Spain G. , Jennings S. G. , Ciais P.
Published: April 2010

Abstract. We estimated CO2, CH4, CO and N2O emission fluxes over the British Isles and Western Europe using atmospheric radon observations and concentrations recorded at the Mace Head Atmospheric Research Station between 1996 and 2005. We classified hourly concentration data into either long-range European or regional sources from Ireland and UK, by using local wind speed data in conjunction with 222Rn and 212Pb threshold criteria. This leads to the selection of about 7% of the total data for both sectors. We then used continuous 222Rn measurements and assumptions on the surface emissions of 222Rn to deduce the unknown fluxes of CO2, CH4, CO and N2O. Our results have been compared to the UNFCCC, EMEP and EDGAR statistical inventories and to inversion results for CH4. For Western Europe, we found yearly mean fluxes of 4.1±1.5 106 kg CO2 km−2 yr−1 , 11.9±2.0 103 kg CH4 km−2 yr−1, 12.8±4.2 103 kg CO km−2 yr−1 and 520.2±129.2 kg N2O km−2 yr−1, respectively, for CO2, CH4, CO and N2O over the period 1996–2005. The method based upon 222Rn to infer emissions has many sources of systematic errors, in particular its poorly known and variable footprint, uncertainties in 222Rn soil fluxes and in atmospheric mixing of air masses with background air. However, these biases are likely to remain constant in the long-term, which makes the method quite efficient to detect trends in fluxes. Over the last ten years period, the decrease of the anthropogenic CH4, CO and N2O emissions in Europe estimated by inventories (respectively −30%, −35% and −23%) is confirmed by the Mace Head data within 2%. Therefore, the 222Rn method provides an independent way of verification of changes in national emissions derived from inventories. Using European-wide estimates of the CO/CO2 emission ratio, we also found that it is possible to separate the fossil fuel CO2 emissions contribution from the one of total CO2 fluxes. The fossil fuel CO2 emissions and their trends derived in that manner agree very well with inventories.
Characterizing ozone production and response under different meteorological conditions in Mexico City
Authors: Lei W. , Zavala M. , de Foy B. , Volkamer R. , Molina L. T.
Published: April 2010

Abstract. Tropospheric photochemistry, particularly the formation of ozone (O3), depends not only on pollutant emissions, but also on meteorological conditions. In this study a 3-D chemical transport model CAMx was employed to investigate the O3 formation and its response to emission reductions under three distinctively different meteorological conditions ("Cold Surge", "O3-North" and "O3-South") in the Mexico City Metropolitan Area during the MCMA-2003 field measurement campaign. The O3 formation characteristics and sensitivity to emissions changes were found to be weakly dependent on the meteorological conditions. The evolution of O3 formation and sensitivity were also examined along the photochemical plume transport pathway. The midday O3 production was found to undergo a rapid increase in a narrow range of chemical aging, while plumes in the downwind were characterized with low and constant O3 production, and plumes along their transport pathway were featured by a combination of the two. The O3 formation was more VOC sensitive near the source area, but as the plume became chemically aged, O3 formation became progressively VOC insensitive and more NOx sensitive.
Middle atmospheric water vapour and dynamics in the vicinity of the polar vortex during the Hygrosonde-2 campaign
Authors: Lossow S. , Khaplanov M. , Gumbel J. , Stegman J. , Witt G. , Dalin P. , Kirkwood S. , Schmidlin J. D. , Fricke K. H. , Blum A.
Published: April 2010

Abstract. The Hygrosonde-2 campaign took place on 16 December 2001 at Esrange/Sweden, with the aim to investigate the small scale distribution of water vapour in the middle atmosphere in the vicinity of the Arctic polar vortex. In-situ balloon and rocket-borne measurements of water vapour were performed by means of OH fluorescence hygrometry. The combined measurements yielded a high resolution water vapour profile up to an altitude of 75 km. Using water vapour as a dynamical tracer it was possible to directly relate the water data to the position of the polar vortex. The measurement probed extra-vortex air below 19 km and in the altitude range between 45 km and 60 km and vortex air elsewhere. Transitions between vortex and extra-vortex usually coincided with wind shears caused by gravity waves which advect air masses with different water vapour characteristics. From the combination of the results from the Hygrosonde-2 campaign and the first flight of the optical hygrometer in 1994 (Hygrosonde-1) a clear picture of the characteristic water vapour distribution inside and outside the polar vortex can be drawn. Systematic differences in the water vapour concentration between the inside and outside of the polar vortex can be observed all the way up into the mesosphere and are consistent with efficient downward transport of air inside the vortex. It is evident that in-situ measurements with high spatial resolution are needed to fully account for the small-scale exchange processes in the polar winter middle atmosphere.
Sensitivity of US air quality to mid-latitude cyclone frequency and implications of 1980–2006 climate change
Authors: Leibensperger E. M. , Mickley L. J. , Jacob D. J.
Published: April 2010

Abstract. We show that the frequency of summertime mid-latitude cyclones tracking across eastern North America at 40°–50° N (the southern climatological storm track) is a strong predictor of stagnation and ozone pollution episodes in the eastern United States. The NCEP/NCAR Reanalysis, going back to 1948, shows a significant long-term decline in the number of summertime mid-latitude cyclones in that track starting in 1980 (−0.15 a-1). The more recent but shorter NCEP/DOE Reanalysis (1979–2006) shows similar interannual variability in cyclone frequency but no significant long-term trend. A GISS general circulation model (GCM) simulation including historical forcing by greenhouse gases reproduces the cyclone trend seen in the NCEP/NCAR data. Such a long-term decrease in mid-latitude cyclone frequency over the 1980–2006 period would have offset by about a factor of 2 the ozone air quality gains from reductions in anthropogenic emissions in the northeastern United States. We find that if mid-latitude cyclone frequency had not declined, the northeastern US would have been largely compliant with the ozone air quality standard by 2001. Mid-latitude cyclone frequency is expected to decrease further over the coming decades in response to greenhouse warming and this trend needs to be considered in air quality management.
Evaluating local anthropogenic impact on remote Arctic monitoring stations: a case study at Summit, Greenland
Authors: Hagler G. S. W. , Bergin M. H. , Smith E. A. , Town M. , Dibb J. E.
Published: April 2010

Abstract. Summit, Greenland is a remote Arctic research station allowing for field measurements at the highest point of the Greenland Ice Sheet. Due to the current reliance on diesel generators for electricity at Summit, unavoidable local emissions are a potential contamination threat to the measurement of combustion-related species in the air and snow. The effect of fossil-fuel combustion on particulate elemental carbon (EC) is assessed by a combination of ambient measurements (~1 km from the main camp), a series of snow pits (up to 20 km from Summit Camp), and Gaussian plume modeling. Ambient measurements indicate that the air directly downwind of the research station generators experiences particulate absorption coefficient (closely related to EC) values that are up to a factor of 200 higher than the summer 2006 non-camp-impacted ambient average. Local anthropogenic influence on snow EC content is also evident. The average EC concentration in 1-m snow pits in the "clean air" sector of Summit Camp are a factor of 1.8–2.4 higher than in snow pits located 10 km and 20 km to the north ("downwind") and south ("upwind") of the research site. Gaussian plume modeling performed using meteorological data from years 2003–2006 suggests a strong angular dependence of anthropogenic impact, with highest risk to the northwest of Summit Camp and lowest to the southeast. Along a transect to the southeast (5 degree angle bin), the modeled frequency of significant camp contribution to atmospheric EC (i.e. camp-produced EC>2006 summer average EC) at a distance of 0.5 km, 10 km, and 20 km is 1%, 0.2%, and 0.05%, respectively. According to both the snow pit and model results, a distance exceeding 10 km towards the southeast is expected to minimize risk of contamination. These results also suggest that other remote Arctic monitoring stations powered by local fuel combustion may need to account for local air and snow contamination in field sampling design and data interpretation.
Polar organic tracers in PM2.5 aerosols from forests in eastern China
Authors: Wang W. , Wu M. H. , Li L. , Zhang T. , Li H. J. , Wang Y. J. , Liu X. D. , Sheng G. Y. , Claeys M. , Fu J. M.
Published: April 2010

Abstract. Photooxidation products of biogenic volatile organic compounds, mainly isoprene and monoterpenes, are significant sources of atmospheric particulate matter in forested regions. The objectives of this study were to examine time trends and diurnal variations of polar organic tracers for the photooxidation of isoprene and α-pinene to investigate whether they are linked with meteorological parameters or trace gases and to estimate their regional carbon contributions. PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) aerosol samples were collected from forests in eastern China and compared with data from forested sites in Europe and America. Aerosol sampling was conducted at four sites located along a gradient of ecological succession in four different regions of China, i.e. Changbai Mountain Nature Reserve (boreal-temperate), Chongming National Forest Park (temperate), Dinghu Mountain Nature Reserve (subtropical) and Jianfengling Nature Reserve (tropical) during summer periods when the meteorological conditions are believed to be favorable for photochemical processes. Fifty PM2.5 samples were collected; seventeen organic compounds, organic carbon (OC), elemental carbon and trace gases were measured. Results indicate that the concentration trends of the secondary organic compounds reflected those of the trace gases and meteorological parameters. The 24-h average concentrations of isoprene oxidation products, α-pinene oxidation products, sugars and sugar alcohols vary systematically along gradients of ecological succession, except malic acid which may have both biogenic and anthropogenic sources. The maximum carbon contribution of isoprene and α-pinene oxidation products to the OC was 2.4% (293 ng/m3, Changbai day-time) and 0.3% (41.3 ng/m3, Changbai night-time), respectively.
Statistical analysis of water vapour and ozone in the UT/LS observed during SPURT and MOZAIC
Authors: Kunz A. , Schiller C. , Rohrer F. , Smit H. G. J. , Nedelec P. , Spelten N.
Published: April 2010

Abstract. A statistical analysis for the comparability of water (H2O) and ozone (O3) data sets sampled during the SPURT aircraft campaigns and the MOZAIC passenger aircraft flights is presented. The Kolmogoroff–Smirnoff test reveals that the distribution functions from SPURT and MOZAIC trace gases differ from each other with a confidence of 95%. A variance analysis shows a different variability character in both trace gas data sets. While the SPURT data only contain atmospheric processes variable on a diurnal or synoptical timescale, MOZAIC data also reveal processes, which vary on inter-seasonal and seasonal timescales. The SPURT data set does not represent the full MOZAIC H2O variance in the UT/LS for climatological investigations, whereas the variance of O3 is much better represented. SPURT H2O data are better suited in the stratosphere, where the MOZAIC RH sensor looses its sensitivity.
The role of ice in N2O5 heterogeneous hydrolysis at high latitudes
Authors: Apodaca R. L. , Huff D. M. , Simpson W. R.
Published: April 2010

Abstract. We report evidence for ice catalyzing N2O5 heterogeneous hydrolysis from a study conducted near Fairbanks, AK in November 2007. Mixing ratios of N2O5, NO, NO2, and ozone are reported and are used to determine steady state N2O5 lifetimes. When air masses are sub-saturated with respect to ice, the data show longer lifetimes (≈20 min) and elevated N2O5 levels, while ice-saturated air masses show shorter lifetimes (≈6 min) and suppressed N2O5 levels. We also report estimates of aerosol surface area densities that are on the order of 50 μm2/cm3, a surface area density that is insufficient to explain the rapid losses of N2O5 observed in this study, reinforcing the importance of other reactive surfaces such as ice. Ice-saturated pollution plumes are ubiquitous in high latitudes; therefore, catalysis on these surfaces is largely responsible for nocturnal processing of N2O5 leading to nitric acid production and loss of NOx in high latitude plumes.
Technical Note: Impact of nonlinearity on changing the a priori of trace gas profiles estimates from the Tropospheric Emission Spectrometer (TES)
Authors: Kulawik S. S. , Bowman K. W. , Luo M. , Rodgers C. D. , Jourdain L.
Published: April 2010

Abstract. Non-linear optimal estimates of atmospheric profiles from the Tropospheric Emission Spectrometer (TES) may contain a priori information that varies geographically, which is a confounding factor in the analysis and physical interpretation of an ensemble of profiles. A common strategy is to transform these profile estimates to a common prior using a linear operation thereby facilitating the interpretation of profile variability. However, this operation is dependent on the assumption of not worse than moderate non-linearity near the solution of the non-linear estimate. We examines the robustness of this assumption when exchanging the prior by comparing atmospheric retrievals from the Tropospheric Emission Spectrometer processed with a uniform prior with those processed with a variable prior and converted to a uniform prior following the non-linear retrieval. We find that linearly converting the prior following a non-linear retrieval is shown to have a minor effect on the results as compared to a non-linear retrieval using a uniform prior when compared to the expected total error, with less than 10% of the change in the prior ending up as unbiased fluctuations in the profile estimate results.