bluuebunny/crossref_metadata_2025 huggingface dataset:
Three years of greenhouse gas column-averaged dry air mole fractions retrieved from satellite – Part 2: Methane
Authors: Schneising O. , Buchwitz M. , Burrows J. P. , Bovensmann H. , Bergamaschi P. , Peters W.
Published: April 2010

Abstract. Carbon dioxide (CO2) and methane (CH4) are the two most important anthropogenic greenhouse gases. SCIAMACHY on ENVISAT is the first satellite instrument whose measurements are sensitive to concentration changes of the two gases at all altitude levels down to the Earth's surface where the source/sink signals are largest. We have processed three years (2003–2005) of SCIAMACHY near-infrared nadir measurements to simultaneously retrieve vertical columns of CO2 (from the 1.58 μm absorption band), CH4 (1.66 μm) and oxygen (O2 A-band at 0.76 μm) using the scientific retrieval algorithm WFM-DOAS. We show that the latest version of WFM-DOAS, version 1.0, which is used for this study, has been significantly improved with respect to its accuracy compared to the previous versions while essentially maintaining its high processing speed (~1 min per orbit, corresponding to ~6000 single measurements, and per gas on a standard PC). The greenhouse gas columns are converted to dry air column-averaged mole fractions, denoted XCO2 (in ppm) and XCH4 (in ppb), by dividing the greenhouse gas columns by simultaneously retrieved dry air columns. For XCO2 dry air columns are obtained from the retrieved O2 columns. For XCH4 dry air columns are obtained from the retrieved CO2 columns because of better cancellation of light path related errors compared to using O2 columns retrieved from the spectrally distant O2 A-band. Here we focus on a discussion of the XCH4 data set. The XCO2 data set is discussed in a separate paper (Part 1). For 2003 we present detailed comparisons with the TM5 model which has been optimally matched to highly accurate but sparse methane surface observations. After accounting for a systematic low bias of ~2% agreement with TM5 is typically within 1–2%. We investigated to what extent the SCIAMACHY XCH4 is influenced by the variability of atmospheric CO2 using global CO2 fields from NOAA's CO2 assimilation system CarbonTracker. We show that the CO2 corrected and uncorrected XCH4 spatio-temporal pattern are very similar but that agreement with TM5 is better for the CarbonTracker CO2 corrected XCH4. In line with previous studies (e.g., Frankenberg et al., 2005b) we find higher methane over the tropics compared to the model. We show that tropical methane is also higher when normalizing the CH4 columns with retrieved O2 columns instead of CO2. In consistency with recent results of Frankenberg et al. (2008b) it is shown that the magnitude of the retrieved tropical methane is sensitive to the choice of the spectroscopic line parameters of water vapour. Concerning inter-annual variability we find similar methane spatio-temporal pattern for 2003 and 2004. For 2005 the retrieved methane shows significantly higher variability compared to the two previous years, most likely due to somewhat larger noise of the spectral measurements.
Spatio-temporal observations of the tertiary ozone maximum
Authors: Sofieva V. F. , Kyrölä E. , Verronen P. T. , Seppälä A. , Tamminen J. , Marsh D. R. , Smith A. K. , Bertaux J.-L. , Hauchecorne A. , Dalaudier F. , Fussen D. , Vanhellemont F. , Fanton d'Andon O. , Barrot G. , Guirlet M. , Fehr T. , Saavedra L.
Published: April 2010

Abstract. We present spatio-temporal distributions of the tertiary ozone maximum (TOM), based on GOMOS (Global Ozone Monitoring by Occultation of Stars) ozone measurements in 2002–2006. The tertiary ozone maximum is typically observed in the high-latitude winter mesosphere at an altitude of ~72 km. Although the explanation for this phenomenon has been found recently – low concentrations of odd-hydrogen cause the subsequent decrease in odd-oxygen losses – models have had significant deviations from existing observations until recently. Good coverage of polar night regions by GOMOS data has allowed for the first time to obtain spatial and temporal observational distributions of night-time ozone mixing ratio in the mesosphere. The distributions obtained from GOMOS data have specific features, which are variable from year to year. In particular, due to a long lifetime of ozone in polar night conditions, the downward transport of polar air by the meridional circulation is clearly observed in the tertiary ozone maximum time series. Although the maximum tertiary ozone mixing ratio is achieved close to the polar night terminator (as predicted by the theory), TOM can be observed also at very high latitudes, not only in the beginning and at the end, but also in the middle of winter. We have compared the observational spatio-temporal distributions of the tertiary ozone maximum with that obtained using WACCM (Whole Atmosphere Community Climate Model) and found that the specific features are reproduced satisfactorily by the model. Since ozone in the mesosphere is very sensitive to HOx concentrations, energetic particle precipitation can significantly modify the shape of the ozone profiles. In particular, GOMOS observations have shown that the tertiary ozone maximum was temporarily destroyed during the January 2005 and December 2006 solar proton events as a result of the HOx enhancement from the increased ionization.
Exploring atmospheric boundary layer characteristics in a severe SO2 episode in the north-eastern Adriatic
Authors: Prtenjak M. T. , Jeričević A. , Kraljević L. , Bulić I. H. , Nitis T. , Klaić Z. B.
Published: April 2010

Abstract. Stable atmospheric conditions are often connected with the occurrence of high pollution episodes especially in urban or industrial areas. In this work we investigate a severe SO2 episode observed on 3–5 February 2002 in a coastal industrial town of Rijeka, Croatia, where very high daily mean concentrations (up to 353.5 μg m−3) were measured. The episode occurred under high air pressure conditions, which were accompanied with a fog and low wind speeds. Three air quality models (50-km EMEP model, 10-km EMEP4HR model and 1-km CAMx model) were used to simulate SO2 concentrations fields and to evaluate the relative contribution of distant and local pollution sources to observed concentrations. Results suggest that the episode was caused predominately by local sources. Furthermore, using three-dimensional, higher-order turbulence closure mesoscale meteorological model (WRF), the wind regimes and thermo-dynamical structure of the lower troposphere above the greater Rijeka area (GRA) were examined in detail. Modelled atmospheric fields suggest several factors whose simultaneous acting was responsible for elevated SO2 concentrations. Established small scale wind directions supported the transport of air from nearby industrial areas with major pollution sources towards Rijeka. This transport was associated with strong, ground-based temperature inversion and correspondingly, very low mixing layer (at most up to about 140 m). Additionally, the surface winds in Rijeka were light or almost calm thus, preventing ventilation of polluted air. Finally, a vertical circulation cell formed between the mainland and a nearby island, supported the air subsidence and the increase of static stability.
Relationships between size-fractionated indoor and outdoor trace elements at four retirement communities in southern California
Authors: Polidori A. , Cheung K. L. , Arhami M. , Delfino R. J. , Schauer J. J. , Sioutas C.
Published: April 2010

Abstract. Indoor and outdoor water soluble trace elements (TEs) were analyzed on quasi-ultrafine (UF), accumulation, and coarse PM filter samples collected at four retirement communities, three located in the San Gabriel Valley and one in Riverside, CA. Our analysis indicates that a complex mix of vehicular, industrial, and soil-related emissions was responsible for the elemental concentrations measured at the three San Gabriel sites, while regional transport, soil re-suspension and, to a lower degree, local traffic contributed to TE levels observed in Riverside. In the quasi-UF mode, the magnitude of indoor/outdoor concentration ratios (I/O) for elements of anthropogenic origin was highly variable, reflecting the spatial heterogeneity of combustion sources in the study area. Indoor/outdoor ratios in accumulation mode PM were closer to 1, and more homogeneous across sites, indicating that elements associated with this size fraction penetrate indoors with high efficiencies. The lowest overall I/O ratios were obtained for elements found in coarse particles, consistent with the fact that only a small portion of coarse outdoor PM infiltrates indoors. The potential of S and other TEs to serve as tracers of indoor-penetrated particles of outdoor origin was also examined. Our results suggest that using the I/O ratio of S (I/OS) as a surrogate of the infiltration factor for PM2.5 [Finf(PM2.5)] might lead to an overestimation of the indoor PM2.5 originating outdoors. This is in contrast with what was reported in previous studies conducted in the Eastern US, where S has been consistently used as a reliable tracer of outdoor PM2.5 infiltrating indoors. Our differences may be due to the fact that in the Los Angeles basin (and in general in the Western US) PM2.5 includes a number of semi-volatile labile species, such as ammonium nitrate and several organic compounds, which volatilize either entirely or to a substantial degree upon building entry.
Ozone in the boundary layer air over the Arctic Ocean: measurements during the TARA transpolar drift 2006–2008
Authors: Bottenheim J. W. , Netcheva S. , Morin S. , Nghiem S. V.
Published: April 2010

Abstract. A full year of measurements of surface ozone over the Arctic Ocean far removed from land is presented (81° N–88° N latitude). The data were obtained during the drift of the French schooner TARA between September 2006 and January 2008, while frozen in the Arctic Ocean. The data confirm that long periods of virtually total absence of ozone occur in the spring (mid March to mid June) after Polar sunrise. At other times of the year, ozone concentrations are comparable to other oceanic observations with winter mole fractions of ca. 30–40 nmol mol−1 and summer minima of ca. 20 nmol mol−1. Contrary to earlier observations from ozone sonde data obtained at Arctic coastal observatories, the ambient temperature was well above −20°C during most ODEs (ozone depletion episodes). Backwards trajectory calculations suggest that during these ODEs the air had previously been in contact with the frozen ocean surface for several days and originated largely from the Siberian coast where several large open flaw leads and polynyas developed in the spring of 2007.
Modelling multi-phase halogen chemistry in the remote marine boundary layer: investigation of the influence of aerosol size resolution on predicted gas- and condensed-phase chemistry
Authors: Lowe D. , Topping D. , McFiggans G.
Published: April 2010

Abstract. A coupled box model of photochemistry and aerosol microphysics which explicitly accounts for size-dependent chemical properties of the condensed-phase has been developed to simulate the multi-phase chemistry of chlorine, bromine and iodine in the marine boundary layer (MBL). The model contains separate seasalt and non-seasalt modes, each of which may be composed of 1–16 size-bins. By comparison of gaseous and aerosol compositions predicted using different size-resolutions with both fixed and size-dependent aerosol turnover rates, it was found that, for halogen-activation processes, the physical property initialisation of the aerosol-mode has a significant influence on gas-phase chemistry. Failure to adequately represent the appropriate physical properties can lead to substantial errors in gas-phase chemistry. The size-resolution of condensed-phase composition has a less significant influence on gas-phase chemistry.
Spatial and temporal UV irradiance and aerosol variability within the area of an OMI satellite pixel
Authors: Kazadzis S. , Bais A. , Balis D. , Kouremeti N. , Zempila M. , Arola A. , Giannakaki E. , Amiridis V. , Kazantzidis A.
Published: April 2010

Abstract. Results of an experimental campaign that took place in the greater Thessaloniki area were used to investigate temporal and spatial UV variability within an OMI satellite pixel. UV irradiance and aerosol optical depth measurements were performed for a one month period at three sites characterized as urban, rural and industrial, depending on their location and possible local aerosol sources. OMI showed a general UV irradiance overestimation compared to all three sites and for all atmospheric conditions. During the campaign the standard deviation calculated from the three sites for UV irradiance at 324 nm was of the order of 26%. For cloudless days with high spatial aerosol variability, UV differences reached ±20% within the OMI pixel. For cloudy days UV differences up to 100% were found at the three sites, a percentage that depends on the ground-based data integration time used for the comparison. Here we tried to focus on the limitations when trying to interpret results of UV irradiance comparisons between OMI satellite and ground based stations, taking into account the UV variability within an OMI pixel, due to such small scale spatial cloud and aerosol inhomogeneities.
Measurements of Volatile Organic Compounds Using Proton Transfer Reaction – Mass Spectrometry during the MILAGRO 2006 Campaign
Authors: Fortner E. C. , Zheng J. , Zhang R. , Berk Knighton W. , Volkamer R. M. , Sheehy P. , Molina L. , André M.
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 the MCMA, their diurnal patterns, and their origins. Diurnal profiles of weekday and weekend/holiday aromatic VOC concentrations showed the influence of vehicular traffic during the morning rush hours and during the afternoon hours. Plumes including 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 possibility 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.
Technical Note: In-situ quantification of aerosol sources and sinks over regional geographical scales
Authors: Buzorius G.
Published: April 2010

Abstract. In order to obtain the source/sink functions for atmospheric particulates located on the planetary surface or elevated in the atmosphere; direct aerosol emission measurements are required. For this purpose, the performance of an airborne aerosol flux measurement system with an improved 3-kilometer (km) spatial resolution is evaluated in this study. Eddy covariance method was used in flux calculations. A footprint for airborne flux sampling with the increased resolution becomes comparable in area to the footprint for tower sampling (with the footprint length being 2 to 10 km). The improvement in spatial resolution allows the quantification of emission rates from individual sources located several kilometers apart such as highway segments, city blocks, and remote and industrial areas. The advantage is a moving platform that allows scanning of aerosol emissions or depositions over regional geographic scales. Airborne flux measurements with the improved spatial resolution were conducted in various environments ranging from clean to partly polluted marine to polluted continental environment with low (<500 m) mixed boundary layer heights. The upward and downward fluxes from the clean marine environment were smaller than 0.5×106 particles m−2 s−1 in absolute value. The effective emissions measured from a ship plume ranged from 2×108 to 3×108 m−2 s−1, and effective fluxes measured crossing cities plumes with populations of 10 000 to 12 000 inhabitants were in the range of 2×108 to 3×108 m−2 s−1. Correlations between heat and aerosol fluxes are evaluated.
A review of Secondary Organic Aerosol (SOA) formation from isoprene
Authors: Carlton A. G. , Wiedinmyer C. , Kroll J. H.
Published: April 2010

Abstract. Recent field and laboratory evidence indicates that the oxidation of isoprene, (2-methyl-1,3-butadiene, C5H8) forms secondary organic aerosol (SOA). Global biogenic emissions of isoprene (600 Tg yr−1) are sufficiently large that the formation of SOA in even small yields results in substantial production of atmospheric particulate matter, likely having implications for air quality and climate. Here we present a review of field measurements, experimental work, and modeling studies aimed at understanding the mechanisms, yield, and atmospheric importance of isoprene-derived SOA. SOA yields depend on a number of factors, including organic aerosol loading (Mo), NOx level (RO2 chemistry), and, because of the importance of multigenerational chemistry, the degree of oxidation. These dependences are not always included in SOA modules used in atmospheric transport models, and instead most yield parameterizations rely on a single set of chamber experiments (carried out over a limited range of conditions); this may lead to very different estimates of the atmospheric importance of isoprene SOA. New yield parameterizations, based on all available laboratory data (Mo=0–50 μg m−3), are presented here, so that SOA formation may be computed as a function of Mo, NOx level, and temperature. Current research needs and future research directions are identified.
First steps towards the assimilation of IASI ozone data into the MOCAGE-PALM system
Authors: Massart S. , Clerbaux C. , Cariolle D. , Piacentini A. , Turquety S. , Hadji-Lazaro J.
Published: April 2010

Abstract. With the use of data assimilation, we study the quality of the Infrared Atmospheric Sounding Interferometer (IASI) total ozone column measurements. The IASI data are provided by the inversion of IASI radiances performed at the Laboratoire ATmosphères, Milieux, Observations Spatiales (LATMOS). This data set is initially compared on a five-month period to a three-dimensional time varying ozone field that we take as a reference. This reference field results from the combined assimilation of ozone profiles from the Microwave Limb Sounder (MLS) instrument and of total ozone columns from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument. It has low systematic and random errors when compared to ozonesondes and Ozone Monitoring Instrument (OMI) data. The comparison shows that on average, the LATMOS-IASI data tends to overestimate the total ozone columns by 2% to 8%. The random observation error of the LATMOS-IASI data is estimated to about 7%, except over polar regions and deserts where it is higher. The daytime data have generally lower biases but higher random error than the nighttime data. Using this information, the LATMOS-IASI data are then assimilated, combined with the MLS data. This first LATMOS-IASI data assimilation experiment shows that the resulting analysis is quite similar to the one obtained from the combined MLS and SCIAMACHY data assimilation. The differences are mainly due to the lack of SCIAMACHY measurements during polar night, and to the higher LATMOS-IASI random errors especially over the southern polar region.
In-cloud processes of methacrolein under simulated conditions – Part 3: Hygroscopic and volatility properties of the formed secondary organic aerosol
Authors: Michaud V. , El Haddad I. ,   Yao Liu, Sellegri K. , Laj P. , Villani P. , Picard D. , Marchand N. , Monod A.
Published: April 2010

Abstract. The hygroscopic and volatility properties of secondary organic aerosol (SOA) produced from the nebulization of solutions after aqueous phase photooxidation of methacrolein was experimentally studied in a laboratory, using a Volatility-Hygroscopicity Tandem DMA (VHTDMA). The obtained SOA were 80% 100°C-volatile after 5 h of reaction and only 20% 100°C-volatile after 22 h of reaction. The Hygroscopic Growth Factor (HGF) of the SOA produced from the nebulization of solutions after aqueous-phase photooxidation of methacrolein is 1.34–1.43, which is significantly higher than the HGF of SOA formed by gas-phase photooxidation of terpenes, usually found almost hydrophobic. These hygroscopic properties were confirmed for SOA formed by the nebulization of the same solutions where NaCl was added. The hygroscopic properties of the cloud droplet residuals decrease with the reaction time, in parallel with the formation of more refractory compounds. This decrease was mainly attributed to the 250°C-refractive fraction (presumably representative of the highest molecular weight compounds), which evolved from moderately hygroscopic (HGF of 1.52) to less hygroscopic (HGF of 1.36). Oligomerization is suggested as a process responsible for the decrease of both volatility and hygroscopicity with time. The NaCl seeded experiments enabled us to show that 19±4 mg L−1 of SOA was produced after 9.5 h of reaction and 41±9 mg L−1 after 22 h of in-cloud reaction. Because more and more SOA is formed as the reaction time increases, our results show that the reaction products formed during the aqueous-phase OH-oxidation of methacrolein may play a major role in the properties of residual particles upon the droplet's evaporation. Therefore, the specific physical properties of SOA produced during cloud processes should be taken into account for a global estimation of SOA and their atmospheric impacts.
Meridional transport and deposition of atmospheric 10Be
Authors: Heikkilä U. , Beer J. , Feichter J.
Published: April 2010

Abstract. 10Be concentrations measured in ice cores exhibit larger temporal variability than expected based on theoretical production calculations. To investigate whether this is due to atmospheric transport a general circulation model study is performed with the 10Be production divided into stratospheric, tropospheric tropical, tropospheric subtropical and tropospheric polar sources. A control run with present day 10Be production rate is compared with a run during a geomagnetic minimum. The present 10Be production rate is 4–5 times higher at high latitudes than in the tropics whereas during a period of no geomagnetic dipole field it is constant at all latitudes. The 10Be deposition fluxes, however, show a very similar latitudinal distribution in both the present day and the geomagnetic minimum run indicating that 10Be is well mixed in the atmosphere before its deposition. This is also confirmed by the fact that the contribution of 10Be produced in the stratosphere is dominant (55%–70%) and relatively constant at all latitudes. The contribution of stratospheric 10Be is approximately 70% in Greenland and 60% in Antarctica reflecting the weaker stratosphere-troposphere air exchange in the Southern Hemisphere.
Exposure-plant response of ambient ozone over the tropical Indian region
Authors: Deb Roy S. , Beig G. , Ghude Sachin D.
Published: April 2010

Abstract. A high resolution regional chemistry-transport model has been used to study the distribution of exposure-plant response index (AOT40, Accumulated exposure Over a Threshold of 40 ppb, expressed as ppb h) over the Indian geographical region for the year 2003 as case study. The directives on ozone pollution in ambient air provided by United Nations Economic Commission for Europe (UNECE) and World Health Organization (WHO) for vegetation protection (AOT40) have been used to assess the air quality. A substantial temporal and spatial variation in AOT40 values has been observed across the Indian region. Large areas of India show ozone values above the AOT40 threshold limit (3000 ppb h for 3 months). Simulated AOT40 values are found to be substantially higher throughout the year over the most fertile Indo-Gangetic plains than the other regions of India, which can have an adverse effect on plants and vegetation in this region. The observed monthly AOT40 values reported from an Indian station, agree reasonably well with model simulated results. There is an underestimation of AOT40 in the model results during the periods of highest ozone concentration from December to March. We find that the simulated AOT40 target values for protection of vegetation is exceeded even in individual months, especially during November to April. Necessary and effective emission reduction strategies are therefore required to be developed in order to curb the surface level ozone pollution to protect the vegetation from further damage in India whose economy is highly dependent on agricultural sector and may influence the global balance.
The impact of diurnal variability in sea surface temperature on the central Atlantic air-sea CO2 flux
Authors: Kettle H. , Merchant C. J. , Jeffery C. D. , Filipiak M. J. , Gentemann C. L.
Published: April 2010

Abstract. The effect of diurnal variations in sea surface temperature (SST) on the air-sea flux of CO2 over the central Atlantic ocean and Mediterranean Sea (60 S–60 N, 60 W–45 E) is evaluated for 2005–2006. We use high spatial resolution hourly satellite ocean skin temperature data to determine the diurnal warming (ΔSST). The CO2 flux is then computed using three different temperature fields – a foundation temperature (Tf, measured at a depth where there is no diurnal variation), Tf, plus the hourly ΔSST and Tf, plus the monthly average of the ΔSSTs. This is done in conjunction with a physically-based parameterisation for the gas transfer velocity (NOAA-COARE). The differences between the fluxes evaluated for these three different temperature fields quantify the effects of both diurnal warming and diurnal covariations. We find that including diurnal warming increases the CO2 flux out of this region of the Atlantic for 2005–2006 from 9.6 Tg C a−1 to 30.4 Tg C a−1 (hourly ΔSST) and 31.2 Tg C a−1 (monthly average of ΔSST measurements). Diurnal warming in this region, therefore, has a large impact on the annual net CO2 flux but diurnal covariations are negligible. However, in this region of the Atlantic the uptake and outgassing of CO2 is approximately balanced over the annual cycle, so although we find diurnal warming has a very large effect here, the Atlantic as a whole is a very strong carbon sink (e.g. −920 Tg C a−1 Takahashi et al., 2002) making this is a small contribution to the Atlantic carbon budget.
Technical Note: Functional sliced inverse regression to infer temperature, water vapour and ozone from IASI data
Authors: Amato U. , Antoniadis A. , De Feis I. , Masiello G. , Matricardi M. , Serio C.
Published: April 2010

Abstract. A retrieval algorithm that uses a statistical strategy based on dimension reduction is proposed. The methodology and details of the implementation of the new algorithm are presented and discussed. The algorithm has been applied to high resolution spectra measured by the Infrared Atmospheric Sounding Interferometer instrument to retrieve atmospheric profiles of temperature, water vapour and ozone. The performance of the inversion strategy has been assessed by comparing the retrieved profiles to the ones obtained by co-locating in space and time profiles from the European Centre for Medium-Range Weather Forecasts analysis.
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 order of 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 fully independently. While the observed strong empirical correlation is remarkable, it must still be noted 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 CCN abundance.
Technical Note: Evolution, current capabilities, and future advance in satellite nadir viewing ultra-spectral IR sounding of the lower atmosphere
Authors: Smith Sr. W. L. , Revercomb H. , Bingham G. , Larar A. , Huang H. , Zhou D. , Li J. , Liu X. , Kireev S.
Published: April 2010

Abstract. Infrared ultra-spectral spectrometers have brought in a new era in satellite remote atmospheric sounding capability. During the 1970s, after the implementation of the first satellite sounding instruments, it became evident that much higher vertical resolution sounding information was needed to be able to forecast life and property threatening localized severe weather. The demonstration of the ultra-spectral radiance measurement technology required to achieve higher vertical resolution began in 1985, with the aircraft flights of the High resolution Interferometer Sounder (HIS) instrument. The development of satellite instruments designed to have a HIS-like measurement capability was initiated in the late 1980's. Today, after more than a decade of development time, the Atmospheric Infrared Sounder (AIRS) and the Infrared Atmospheric Sounding Interferometer (IASI) are now operating successfully from the Aqua and MetOp polar orbiting satellites. The successful development and ground demonstration of the Geostationary Imaging Fourier Transform Spectrometer (GIFTS), during this decade, is now paving the way toward the implementation of the ultra-spectral sounding capability on the international system of geostationary environmental satellites. This note reviews the evolution of the satellite ultra-spectral sounding systems, shows examples of current polar satellite sounding capability, and discusses future advances planned for geostationary orbit.
Physical and chemical properties of the regional mixed layer of Mexico's Megapolis
Authors: Baumgardner D. , Grutter M. , Allan J. , Ochoa C. , Rappenglueck B. , Russell L. M. , Arnott P.
Published: April 2010

Abstract. The concentration of gases and aerosol particles have been measured at the mountain site of Altzomoni, 4010 m in altitude, located 60 km southeast of Mexico City, 50 km east of Puebla and 70 km northeast of Cuernavaca. The objective of this study was to evaluate the properties of gases and particles in the Regional Mixed Layer (RML) of Mexico's Megapolis. Altzomoni is generally above the RML from late evening until late morning at which time the arrival of the RML is marked by increasing concentrations of CO and aerosol particles that reach their maxima in mid-afternoon. The average diurnal cycles for fourteen days in March, 2006 were evaluated during which time the synoptic scale circulation had three principal patterns: from the east (E), southwest (SW) and west northwest (WNW). The original hypothesis was that air arriving from the direction of Mexico City would have much higher concentrations of anthropogenic gases and particles than air from Puebla or Cuernavaca, due to the relatively large differences in populations. In fact, not only were the average, maximum concentrations of CO and O3 (0.3 and 0.1 ppmv) approximately the same for air originating from the WNW and E, but the average maximum concentrations of Peroxyacyl nitrates (PAN,PPN) and particle organic matter (POM) in air from the E exceeded those in air from the WNW. Comparisons of measurements from the mountain site with those made by aircraft during the same period, using the same type of aerosol mass spectrometer, show that the total masses of POM, NO3−, SO42− and NH4+ were approximately the same from aircraft measurements made over Mexico City and when winds were from the east at the mountain site. In contrast 75% of the total aerosol mass at the mountain site was POM whereas over Mexico City the fraction of POM was less than 60%. The measurements suggest the occasional influence of emissions from the nearby volcano, Popocatepetl, as well as possible incursions of biomass combustion; however, the large concentrations of O3, PAN and POM suggest that secondary processes are the major source for these gases and particles. The similar concentrations in gases and particles when air is coming from the E and NWN raises the possibility of recirculation of air from Mexico City and the importance of this mechanism for impacting the regional air quality.
A simple model for cloud radiative forcing
Authors: Corti T. , Peter T.
Published: April 2010

Abstract. We present a simple model for the longwave and shortwave cloud radiative forcing based on the evaluation of extensive radiative transfer calculations, covering a global range of conditions. The simplicity of the model equations fosters the understanding on how clouds affect the Earth's energy balance. In comparison with results from a comprehensive radiative transfer model, the accuracy of our parameterization is typically better than 20%. We demonstrate the usefulness of our model using the example of tropical cirrus clouds. We conclude that possible applications for the model include the convenient estimate of cloud radiative forcing for a wide range of conditions, the evaluation of the sensitivity to changes in environmental conditions, and as a tool in education. An online version of the model is available at http://www.iac.ethz.ch/url/crf.
Emissions from biomass burning in the Yucatan
Authors: Yokelson R. J. , Crounse J. D. , DeCarlo P. F. , Karl T. , Urbanski S. , Atlas E. , Campos T. , Shinozuka Y. , Kapustin V. , Clarke A. D. , Weinheimer A. , Knapp D. J. , Montzka D. D. , Holloway J. , Weibring P. , Flocke F. , Zheng W. , Toohey D. , Wennberg P. O. , Wiedinmyer C. , Mauldin L. , Fried A. , Richter D. , Walega J. , Jimenez J. L. , Adachi K. , Buseck P. R. , Hall S. R. , Shetter R.
Published: April 2010

Abstract. In March 2006 two instrumented aircraft made the first detailed field measurements of biomass burning (BB) emissions in the Northern Hemisphere tropics as part of the MILAGRO project. The aircraft were the National Center for Atmospheric Research C-130 and a University of Montana/US Forest Service Twin Otter. The initial emissions of up to 49 trace gas or particle species were measured from 20 deforestation and crop residue fires on the Yucatan peninsula. This included two trace gases useful as indicators of BB (HCN and acetonitrile) and several rarely, or never before, measured species: OH, peroxyacetic acid, propanoic acid, hydrogen peroxide, methane sulfonic acid, and sulfuric acid. Crop residue fires emitted more organic acids and ammonia than deforestation fires, but the emissions from the main fire types were otherwise fairly similar. The Yucatan fires emitted unusually high amounts of SO2 and particle chloride, likely due to a strong marine influence on this peninsula. As smoke from one fire aged, the ratio ΔO3/ΔCO increased to ~15% in 1×107 molecules/cm3) that were likely caused in part by high initial HONO (~10% of NOy). Thus, more research is needed to understand critical post emission processes for the second-largest trace gas source on Earth. It is estimated that ~44 Tg of biomass burned in the Yucatan in the spring of 2006. Mexican BB (including Yucatan BB) and urban emissions from the Mexico City area can both influence the March-May air quality in much of Mexico and the US.
A statistical analysis of the influence of deep convection on water vapor variability in the tropical upper troposphere
Authors: Wright J. S. , Fu R. , Heymsfield A. J.
Published: April 2010

Abstract. The factors that control the influence of deep convective detrainment on water vapor in the tropical upper troposphere are examined using observations from multiple satellites in conjunction with a trajectory model. Deep convection is confirmed to act primarily as a moisture source to the upper troposphere, modulated by the ambient relative humidity (RH). Convective detrainment provides strong moistening at low RH and offsets drying due to subsidence across a wide range of RH. Strong day-to-day moistening and drying takes place most frequently in relatively dry transition zones, where between 0.01% and 0.1% of Tropical Rainfall Measuring Mission Precipitation Radar observations indicate active convection. Many of these strong moistening events in the tropics can be directly attributed to detrainment from recent tropical convection, while others in the subtropics appear to be related to stratosphere-troposphere exchange. The temporal and spatial limits of the convective source are estimated to be about 36–48 h and 600–1500 km, respectively, consistent with the lifetimes of detrainment cirrus clouds. Larger amounts of detrained ice are associated with enhanced upper tropospheric moistening in both absolute and relative terms. In particular, an increase in ice water content of approximately 400% corresponds to a 10–90% increase in the likelihood of moistening and a 30–50% increase in the magnitude of moistening.
Inverse modeling and mapping US air quality influences of inorganic PM2.5 precursor emissions using the adjoint of GEOS-Chem
Authors: Henze D. K. , Seinfeld J. H. , Shindell D. T.
Published: April 2010

Abstract. Influences of specific sources of inorganic PM2.5 on peak and ambient aerosol concentrations in the US are evaluated using a combination of inverse modeling and sensitivity analysis. First, sulfate and nitrate aerosol measurements from the IMPROVE network are assimilated using the four-dimensional variational (4D-Var) method into the GEOS-Chem chemical transport model in order to constrain emissions estimates in four separate month-long inversions (one per season). Of the precursor emissions, these observations primarily constrain ammonia (NH3). While the net result is a decrease in estimated US~NH3 emissions relative to the original inventory, there is considerable variability in adjustments made to NH3 emissions in different locations, seasons and source sectors, such as focused decreases in the midwest during July, broad decreases throughout the US~in January, increases in eastern coastal areas in April, and an effective redistribution of emissions from natural to anthropogenic sources. Implementing these constrained emissions, the adjoint model is applied to quantify the influences of emissions on representative PM2.5 air quality metrics within the US. The resulting sensitivity maps display a wide range of spatial, sectoral and seasonal variability in the susceptibility of the air quality metrics to absolute emissions changes and the effectiveness of incremental emissions controls of specific source sectors. NH3 emissions near sources of sulfur oxides (SOx) are estimated to most influence peak inorganic PM2.5 levels in the East; thus, the most effective controls of NH3 emissions are often disjoint from locations of peak NH3 emissions. Controls of emissions from industrial sectors of SOx and NOx are estimated to be more effective than surface emissions, and changes to NH3 emissions in regions dominated by natural sources are disproportionately more effective than regions dominated by anthropogenic sources. NOx controls are most effective in northern states in October; in January, SOx controls may be counterproductive. When considering ambient inorganic PM2.5 concentrations, intercontinental influences are small, though transboundary influences within North America are significant, with SOx emissions from surface sources in Mexico contributing almost a fourth of the total influence from this sector.
Measurements of particle masses of inorganic salt particles for calibration of cloud condensation nuclei counters
Authors: Kuwata M. , Kondo Y.
Published: April 2010

Abstract. We measured the mobility equivalent critical dry diameter for cloud condensation nuclei (CCN) activation (dc_me) and the particle mass of size-selected (NH4)2SO4 and NaCl particles to calibrate a CCN counter (CCNC) precisely. The CCNC was operated downstream of a differential mobility analyzer (DMA) for the measurement of dc_me. The particle mass was measured using an aerosol particle mass analyzer (APM) operated downstream of the DMA. The measurement of particle mass was conducted for 50–150-nm particles. Effective densities (ρeff) of (NH4)2SO4 particles were 1.67–1.75 g cm−3, which correspond to dynamic shape factors (χ) of 1.01–1.04. This shows that (NH4)2SO4 particles are not completely spherical. In the case of NaCl particles, ρeff was 1.75–1.99 g cm−3 and χ was 1.05–1.14, demonstrating that the particle shape was non-spherical. Using these experimental data, the volume equivalent critical dry diameter (dc_ve) was calculated, and it was used as an input parameter for calculations of critical supersaturation (S). Several thermodynamics models were used for the calculation of water activity. When the Pitzer model was employed for the calculations, the critical S calculated for (NH4)2SO4 and NaCl agreed to well within the uncertainty of 2% (relative). This result demonstrates that the use of the Pitzer model for the calibration of CCNCs gives the most accurate value of S.
Recent trends in atmospheric methyl bromide: analysis of post-Montreal Protocol variability
Authors: Yvon-Lewis S. A. , Saltzman E. S. , Montzka S. A.
Published: April 2010

Abstract. The atmospheric methyl bromide (CH3Br) burden has declined in recent years, in response to the phaseout of agricultural and structural fumigation consumption under the amendments to the Montreal Protocol. The timing and magnitude of this decrease represents an opportunity to examine our current understanding of atmospheric CH3Br and its budget, response to the phaseout, and response to interannual variability in biomass burning and global OH. In this study, simulations obtained from a time-dependent global model of atmospheric CH3Br emissions and uptake are compared to observations from the NOAA flask network. The model includes a detailed gridded ocean model coupled to a time-dependant atmospheric 2-box model. The phaseout of CH3Br production for agricultural uses began in 1998, concurrent with the pulse in biomass burning associated with the 1998 El Niño. The combined effects of three factors (biomass burning, global OH, and anthropogenic phaseout) appear to explain most of the observed atmospheric methyl bromide variability over the 1997–2008 period. The global budget remains imbalanced, with a large missing source indicated. The missing source does not exhibit a systematic decline during the phaseout period, and therefore, is not the result of significantly underestimating non-QPS agricultural CH3Br emissions. The model results suggest that the oceans should be less undersaturated than before the phaseout began.
The climatic effects of the direct injection of water vapour into the stratosphere by large volcanic eruptions
Authors: Joshi M. M. , Jones G. S.
Published: April 2010

Abstract. We describe a novel mechanism that can significantly lower the amplitude of the climatic response to certain large volcanic eruptions and examine its impact with a coupled ocean-atmosphere climate model. If sufficiently large amounts of water vapour enter the stratosphere, a climatically significant amount of water vapour can be left over in the lower stratosphere after the eruption, even after sulphate aerosol formation. This excess stratospheric humidity warms the tropospheric climate, and acts to balance the climatic cooling induced by the volcanic aerosol, especially because the humidity anomaly lasts for a period that is longer than the residence time of aerosol in the stratosphere. In particular, northern hemisphere high latitude cooling is reduced in magnitude. We discuss this mechanism in the context of the discrepancy between the observed and modelled cooling following the Krakatau eruption in 1883. We hypothesize that moist coignimbrite plumes caused by pyroclastic flows travelling over ocean rather than land, resulting from an eruption close enough to the ocean, might provide the additional source of stratospheric water vapour.
An overview of two years of ozone radio soundings over Cotonou as part of AMMA
Authors: Thouret V. , Saunois M. , Minga A. , Mariscal A. , Sauvage B. , Solete A. , Agbangla D. , Nédélec P. , Mari C. , Reeves C. E. , Schlager H.
Published: April 2010

Abstract. As part of the African Monsoon Multidisciplinary Analysis (AMMA) program, a total of 98 ozone vertical profiles over Cotonou, Benin, have been measured during a 26 month period (December 2004–January 2007). These regular measurements broadly document the seasonal and interannual variability of ozone in both the troposphere and the lower stratosphere over West Africa for the first time. This data set is complementary to the MOZAIC observations made from Lagos between 0 and 12 km during the period 1998–2004. Both data sets highlight the unique way in which West Africa is impacted by two biomass burning seasons: in December–February (dry season) due to burning in the Sahelian band and in June-August (wet season) due to burning in southern Africa. High interannual variabilities between Cotonou and Lagos data sets and within each data set are observed and are found to be a major characteristic of this region. In particular, the dry and wet seasons are discussed in order to set the data of the Special Observing Periods (SOPs) into a climatological context. Compared to other dry and wet seasons, the 2006 dry and wet season campaigns took place in rather high ozone environments. During the sampled wet seasons, southern intrusions of biomass burning were particularly frequent with concentrations up to 120 ppbv of ozone in the lower troposphere. An insight into the ozone distribution in the upper troposphere and the lower stratosphere (up to 26 km) is given. The first tropospheric columns of ozone based on in-situ data over West Africa are assessed. They compare well with satellite products on seasonal and interannual time-scales, provided that the layer below 850 hPa where the remote instrument is less sensitive to ozone, is removed.