bluuebunny/crossref_metadata_2025 huggingface dataset:
Variability of subtropical upper tropospheric humidity
Authors: Ryoo J.-M. , Waugh D. W. , Gettelman A.
Published: April 2010

Abstract. Analysis of Atmospheric Infrared Sounder (AIRS) measurements for five years shows significant longitudinal variations in the winter subtropical upper tropospheric relative humidity (RH), not only in the climatological mean values but also in the local distributions and temporal variability. The largest climatological mean values occur over the central-eastern Pacific and Atlantic oceans, where there is also large day-to-day variability. In contrast, there are smaller mean values, and smaller variability that occurs at lower frequency, over the Indian and western Pacific oceans. These differences in the distribution and variability of subtropical RH are related to differences in the key transport processes in the different sectors. The large variability and intermittent high and low RH over the central-eastern Pacific and Atlantic oceans are due to intrusions of high potential vorticity air into the subtropics. Intrusions seldom occur over the eastern Indian and western Pacific oceans, and here the subtropical RH is more closely linked to the location and strength of subtropical anticyclones. During northern winter there are eastward propagating features in the subtropical RH in this region that are out of phase with the tropical RH, and are caused by modulation of the subtropical anticyclones by the Madden-Julian Oscillation.
Improvement of vertical and residual velocities in pressure or hybrid sigma-pressure coordinates in analysis data in the stratosphere
Authors: Wohltmann I. , Rex M.
Published: April 2010

Abstract. Stratospheric vertical winds from analysis data in pressure (p) or hybrid pressure (σ-p) coordinates, for use in e.g. chemical transport models (CTMs) or trajectory models, often suffer both from excessive noise and errors in their mean magnitude, which in turn can introduce errors in important dynamical quantities like vertical mixing or constituent transport with the residual circulation. Since vertical velocities cannot be measured directly, they are inferred from other quantities, typically from horizontal wind divergence, that is the mass continuity equation. We propose a method to calculate the vertical wind field from the thermodynamic energy equation in p or σ-p vertical coordinates that substantially reduces noise and overestimation of the residual circulation. It is completely equivalent to the approach using potential temperature (θ) as a vertical coordinate and diabatic heating rates as vertical velocities, which has already been demonstrated to give superior results to the continuity equation. It provides a quickly realizable improvement of the vertical winds, when a change of the vertical variable would cause an inadequate effort (e.g. in CTMs). The method is only applicable for stably stratified regions like the stratosphere.
Spatiotemporal variations of ambient PM10 source contributions in Beijing in 2004 using positive matrix factorization
Authors: Xie S. D. , Liu Z. , Chen T. , Hua L.
Published: April 2010

Abstract. Source contributions to ambient PM10 (particles with an aerodynamic diameter of 10 μm or less) in Beijing, China were determined with positive matrix factorization (PMF) based on ambient PM10 composition data including concentrations of organic carbon (OC), elemental carbon (EC), ions and metal elements, which were simultaneously obtained at six sites through January, April, July and October in 2004. Results from PMF indicated that seven major sources of ambient PM10 were urban fugitive dust, crustal soil, coal combustion, secondary sulfate, secondary nitrate, biomass burning with municipal incineration, and vehicle emission, respectively. In paticular, urban fugitive dust and crustal soil as two types of dust sources with similar chemical characteristics were differentiated by PMF. Urban fugitive dust contributed the most, accounting for 34.4% of total PM10 mass on an annual basis, with relatively high contributions in all four months, and even covered 50% in April. It also showed higher contributions in southwestern and southeastern areas than in central urban areas. Coal combustion was found to be the primary contributor in January, showing higher contributions in urban areas than in suburban areas with seasonal variation peaking in winter, which accounted for 15.5% of the annual average PM10 concentration. Secondary sulfate and secondary nitrate combined as the largest contributor to PM10 in July and October, with strong seasonal variation peaking in summer, accounting for 38.8% and 31.5% of the total PM10 mass in July and October, respectively. Biomass burning with municipal incineration contributions were found in all four months and accounted for 9.8% of the annual average PM10 mass concentration, with obviously higher contribution in October than in other months. Incineration sources were probably located in southwestern Beijing. Contribution from vehicle emission accounted for 5.0% and exhibited no significant seasonal variation. In sum, PM10 source contributions in Beijing showed not only significant seasonal variations but also spatial differences.
Cloud system resolving model study of the roles of deep convection for photo-chemistry in the TOGA COARE/CEPEX region
Authors: Salzmann M. , Lawrence M. G. , Phillips V. T. J. , Donner L. J.
Published: April 2010

Abstract. A cloud system resolving model including photo-chemistry (CSRMC) has been developed based on a prototype version of the Weather Research and Forecasting (WRF) model and is used to study influences of deep convection on chemistry in the TOGA COARE/CEPEX region. Lateral boundary conditions for trace gases are prescribed from global chemistry-transport simulations, and the vertical advection of trace gases by large scale dynamics, which is not reproduced in a limited area cloud system resolving model, is taken into account. The influences of deep convective transport and of lightning on NOx, O3, and HOx(=HO2+OH), in the vicinity of the deep convective systems are investigated in a 7-day 3-D 248×248 km2 horizontal domain simulation and several 2-D sensitivity runs with a 500 km horizontal domain. Mid-tropospheric entrainment is more important on average for the upward transport of O3 in the 3-D run than in the 2-D runs, but at the same time undiluted O3-poor air from the marine boundary layer reaches the upper troposphere more frequently in the 3-D run than in the 2-D runs, indicating the presence of undiluted convective cores. In all runs, in situ lightning is found to have only minor impacts on the local O3 budget. Near zero O3 volume mixing ratios due to the reaction with lightning-produced NO are only simulated in a 2-D sensitivity run with an extremely high number of NO molecules per flash, which is outside the range of current estimates. The fraction of NOx chemically lost within the domain varies between 20 and 24% in the 2-D runs, but is negligible in the 3-D run, in agreement with a lower average NOx concentration in the 3-D run despite a greater number of flashes. Stratosphere to troposphere transport of O3 is simulated to occur episodically in thin filaments in the 2-D runs, but on average net upward transport of O3 from below ~16 km is simulated in association with mean large scale ascent in the region. Ozone profiles in the TOGA COARE/CEPEX region are suggested to be strongly influenced by the intra-seasonal (Madden-Julian) oscillation.
Estimation of Asian dust aerosol effect on cloud radiation forcing using Fu-Liou radiative model and CERES measurements
Authors:   Jing Su,   Jianping Huang,   Qiang Fu, Minnis P. ,   Jinming Ge,   Jianrong Bi
Published: April 2010

Abstract. The impact of Asian dust on cloud radiative forcing during 2003–2006 is studied by using the Clouds and Earth's Radiant Energy Budget Scanner (CERES) data and the Fu-Liou radiative transfer model. Analysis of satellite data shows that the dust aerosol significantly reduced the cloud cooling effect at TOA. In dust contaminated cloudy regions, the 4-year mean values of the instantaneous shortwave, longwave and net cloud radiative forcing are −138.9, 69.1, and −69.7 Wm−2, which are 57.0, 74.2, and 46.3%, respectively, of the corresponding values in pristine cloudy regions. The satellite-retrieved cloud properties are significantly different in the dusty regions and can influence the radiative forcing indirectly. The contributions to the cloud radiation forcing by the dust direct, indirect and semi-direct effects are estimated using combined satellite observations and Fu-Liou model simulation. The 4-year mean value of combination of dust indirect and semi-direct shortwave radiative forcing (SWRF) is 82.2 Wm−2, which is 78.4% of the total dust effect. The dust direct effect is only 22.7 Wm−2, which is 21.6% of the total effect. Because both first and second indirect effects enhance cloud cooling, the aerosol-induced cloud warming is mainly the result of the semi-direct effect of dust.
SIMPOL.1: a simple group contribution method for predicting vapor pressures and enthalpies of vaporization of multifunctional organic compounds
Authors: Pankow J. F. , Asher W. E.
Published: April 2010

Abstract. The SIMPOL.1 group contribution method is developed for predicting the liquid vapor pressure poL (atm) and enthalpy of vaporization Δ Hvap (kJ mol-1) of organic compounds as functions of temperature (T). For each compound i, the method assumes log10poL,i (T)=∑kνk,ibk(T) where νk,i is the number of groups of type k, and bk (T) is the contribution to log10poL,i (T) by each group of type k. A zeroeth group is included that uses b0 (T) with ν0,i=1 for all i. A total of 30 structural groups are considered: molecular carbon, alkyl hydroxyl, aromatic hydroxyl, alkyl ether, alkyl ring ether, aromatic ether, aldehyde, ketone, carboxylic acid, ester, nitrate, nitro, alkyl amine (primary, secondary, and tertiary), aromatic amine, amide (primary, secondary, and tertiary), peroxide, hydroperoxide, peroxy acid, C=C, carbonylperoxynitrate, nitro-phenol, nitro-ester, aromatic rings, non-aromatic rings, C=C–C=O in a non-aromatic ring, and carbon on the acid-side of an amide. The T dependence in each of the bk (T) is assumed to follow b(T)=B1/T+B2+B3T+B4ln T. Values of the B coefficients are fit using an initial basis set of 272 compounds for which experimentally based functions po L,i=fi (T) are available. The range of vapor pressure considered spans fourteen orders of magnitude. The ability of the initially fitted B coefficients to predict poL values is examined using a test set of 184 compounds and a T range that is as wide as 273.15 to 393.15 K for some compounds. σFIT is defined as the average over all points of the absolute value of the difference between experimental and predicted values of log10poL,i (T). After consideration of σFIT for the test set, the initial basis set and test set compounds are combined, and the B coefficients re-optimized. For all compounds and temperatures, σFIT=0.34: on average, poL,i (T) values are predicted to within a factor of 2. Because d(log10 poL,i (T))d(1/T) is related to the enthalpy of vaporization ΔHvap,i, the fitted B provide predictions of ΔHvap,i based on structure.
Utilising shade to optimize UV exposure for vitamin D
Authors: Turnbull D. J. , Parisi A. V.
Published: April 2010

Abstract. Numerous studies have stated that humans need to utilise full sun radiation, at certain times of the day, to assist the body in synthesising the required levels of vitamin D3. The time needed to be spent in the full sun depends on a number of factors, for example, age, skin type, latitude, solar zenith angle. Current Australian guidelines suggest exposure to approximately 1/6 to 1/3 of a minimum erythemal dose (MED), depending on age, would be appropriate to provide adequate vitamin D3 levels. The aim of the study was to determine the exposure times to diffuse solar UV to receive exposures of 1/6 and 1/3 MED for a changing solar zenith angle in order to assess the possible role that diffuse UV (scattered radiation) may play in vitamin D3 effective UV exposures (UVD3). Diffuse and global erythemal UV measurements were conducted at five minute intervals over a twelve month period for a solar zenith angle range of 4° to 80° at a latitude of 27.6° S. For a diffuse UV exposure of 1/3 MED, solar zenith angles smaller than approximately 50° can be utilised for exposure times of less than 10 min. Spectral measurements showed that, for a solar zenith angle of 40°, the UVA (315–400 nm) in the diffuse component of the solar UV is reduced by approximately 62% compared to the UVA in the global UV, whereas UVD3 wavelengths are only reduced by approximately 43%. At certain latitudes, diffuse UV under shade may play an important role in providing the human body with adequate levels of UVD3 (290–315 nm) radiation without experiencing the high levels of UVA observed in full sun.
Variability of the total ozone trend over Europe for the period 1950–2004 derived from reconstructed data
Authors: Krzyścin J. W. , Borkowski J. L.
Published: April 2010

Abstract. The total ozone data over Europe are available for only few ground-based stations in the pre-satellite era disallowing examination of the spatial trend variability over the whole continent. A need of having gridded ozone data for a trend analysis and input to radiative transfer models stimulated a reconstruction of the daily ozone values since January 1950. Description of the reconstruction model and its validation were a subject of our previous paper. The data base used was built within the objectives of the COST action 726 "Long-term changes and climatology of UV radiation over Europe". Here we focus on trend analyses. The long-term variability of total ozone is discussed using results of a flexible trend model applied to the reconstructed total ozone data for the period 1950–2004. The trend pattern, which comprises both anthropogenic and "natural" component, is not a priori assumed but it comes from a smooth curve fit to the zonal monthly means and monthly grid values. The ozone long-term changes are calculated separately for cold (October–next year April) and warm (May–September) seasons. The confidence intervals for the estimated ozone changes are derived by the block bootstrapping. The statistically significant negative trends are found almost over the whole Europe only in the period 1985–1994. Negative trends up to −3% per decade appeared over small areas in earlier periods when the anthropogenic forcing on the ozone layer was weak . The statistically positive trends are found only during warm seasons 1995–2004 over Svalbard archipelago. The reduction of ozone level in 2004 relative to that before the satellite era is not dramatic, i.e., up to ~−5% and ~−3.5% in the cold and warm subperiod, respectively. Present ozone level is still depleted over many popular resorts in southern Europe and northern Africa. For high latitude regions the trend overturning could be inferred in last decade (1995–2004) as the ozone depleted areas are not found there in 2004 in spite of substantial ozone depletion in the period 1985–1994.
Quality assessment of water cycle parameters in REMO by radar-lidar synergy
Authors: Hennemuth B. , Weiss A. , Bösenberg J. , Jacob D. , Linné H. , Peters G. , Pfeifer S.
Published: April 2010

Abstract. A comparison study of water cycle parameters derived from ground-based remote-sensing instruments and from the regional model REMO is presented. Observational data sets were collected during three measuring campaigns in summer/autumn 2003 and 2004 at Richard Aßmann Observatory, Lindenberg, Germany. The remote sensing instruments which were used are differential absorption lidar, Doppler lidar, ceilometer, cloud radar, and micro rain radar for the derivation of humidity profiles, ABL height, water vapour flux profiles, cloud parameters, and rain rate. Additionally, surface latent and sensible heat flux and soil moisture were measured. Error ranges and representativity of the data are discussed. For comparisons the regional model REMO was run for all measuring periods with a horizontal resolution of 18 km and 33 vertical levels. Parameter output was every hour. The measured data were transformed to the vertical model grid and averaged in time in order to better match with gridbox model values. The comparisons show that the atmospheric boundary layer is not adequately simulated, on most days it is too shallow and too moist. This is found to be caused by a wrong partitioning of energy at the surface, particularly a too large latent heat flux. The reason is obviously an overestimation of soil moisture during drying periods by the one-layer scheme in the model. The profiles of water vapour transport within the ABL appear to be realistically simulated. The comparison of cloud cover reveals an underestimation of low-level and mid-level clouds by the model, whereas the comparison of high-level clouds is hampered by the inability of the cloud radar to see cirrus clouds above 10 km. Simulated ABL clouds apparently have a too low cloud base, and the vertical extent is underestimated. The ice water content of clouds agree in model and observation whereas the liquid water content is unsufficiently derived from cloud radar reflectivity in the present study. Rain rates are similar, but the representativeness of both observations and grid box values is low.
Measurement of the water vapour vertical profile and of the Earth's outgoing far infrared flux
Authors: Palchetti L. , Bianchini G. , Carli B. , Cortesi U. , Del Bianco S.
Published: April 2010

Abstract. Our understanding of global warming depends on the accuracy with which the atmospheric components that modulate the Earth's radiation budget are known. Many uncertainties still exist as regards the radiative effect of water in the different spectral regions, among which is the far infrared, where very few observations have been made. An assessment is shown of the atmospheric outgoing flux obtained from a balloon-borne platform with wideband spectrally-resolved nadir measurements at the top of the atmosphere over the full spectral range, from 100 to 1400 cm−1, made by a Fourier transform spectrometer with uncooled detectors. From these measurements, we retrieved 15 pieces of information regarding water vapour and temperature profiles and surface temperature, with a major improvement in our knowledge of water vapour in the upper troposphere. The retrieved atmospheric state made it possible to calculate the emitted radiance also at frequencies and zenith angles that have not been observed and to determine the outgoing spectral radiation flux. This proves that spectrally resolved observations can be used to derive accurate information on the integrated flux. While the retrieved temperature was in agreement with ECMWF analysis, the retrieved water vapour profile differed significantly; depending on the time and the location, the derived flux in the far infrared (20–600 cm−1) differed by 2–3.5 W/m2 from that calculated using ECMWF. The error with which the far infrared flux is determined by REFIR-PAD is about 0.4 W/m2 and is caused mainly by calibration uncertainties, while detector noise has a negligible effect. This proves that uncooled detectors are adequate for top-of-the-atmosphere radiometry.
An Ensemble Kalman Filter for severe dust storm data assimilation over China
Authors: Lin C. , Wang Z. , Zhu J.
Published: April 2010

Abstract. An Ensemble Kalman Filter (EnKF) data assimilation system was developed for a regional dust transport model. This paper applied the EnKF method to investigate modeling of severe dust storm episodes occurring in March 2002 over China based on surface observations of dust concentrations to explore the impact of the EnKF data assimilation systems on forecast improvement. A series of sensitivity experiments using our system demonstrates the ability of the advanced EnKF assimilation method using surface observed PM10 in North China to correct initial conditions, which leads to improved forecasts of dust storms. However, large errors in the forecast may arise from model errors (uncertainties in meteorological fields, dust emissions, dry deposition velocity, etc.). This result illustrates that the EnKF requires identification and correction model errors during the assimilation procedure in order to significantly improve forecasts. Results also show that the EnKF should use a large inflation parameter to obtain better model performance and forecast potential. Furthermore, the ensemble perturbations generated at the initial time should include enough ensemble spreads to represent the background error after several assimilation cycles.
The effects of airmass history on new particle formation in the free troposphere: case studies
Authors: Benson D. R. ,   Li-Hao Young,   Shan-Hu Lee, Campos T. L. , Rogers D. C. , Jensen J.
Published: April 2010

Abstract. Recent aircraft studies showed that new particle formation (NPF) is very active in the free troposphere. And, these observations lead to a new question: when does NPF not occur? Here, we provide case studies to show how different meteorological parameters affect NPF in the upper troposphere, using the aerosol size distributions measured at latitudes from 18° N–52° N and altitudes up to 14 km during the NSF/NCAR GV Progressive Science Missions. About 95% of the total samples showed the NPF feature with median number concentrations of particles with diameters from 4 to 9 nm (N4–9), 288±199 cm−3, and the total particle number concentrations with diameters from 4 to 2000 nm (N4–2000), 500±259 cm−3. Surface areas were in general very low in the free troposphere, 1.58±0.87 μm2 cm−3, which in part explains the high frequency of NPF measured in this region, but there was no distinctive difference in surface area for the NPF and non-NPF cases. Our case studies show that rather airmass history is more important for nucleation in this region. Weak- or non-events did not display uplifting of airmasses. On the other hand, strong NPF events were usually associated with uplifting of airmasses, although there were also NPF cases in which uplift did not occur, consistent with the previous observations (Young et al., 2007). NPF tends to easily occur in the free troposphere because of low surface areas and low temperatures (Carslaw and Kärcher, 2006), but because of the low aerosol precursors in this region, vertical motion (that can bring higher concentrations of aerosol precursors from low altitude source regions to higher altitudes) can play a critical role. Latitude dependence of new particles also shows higher particle concentrations in the midlatitude and subtropics tropopause region than in the tropics, consistent with Hermann et al. (2003).
Accounting for the effect of horizontal gradients in limb measurements of scattered sunlight
Authors: Puķīte J. , Kühl S. , Deutschmann T. , Platt U. , Wagner T.
Published: April 2010

Abstract. Limb measurements provided by the SCanning Imaging Absorption spectrometer for Atmospheric CHartographY (SCIAMACHY) on the ENVISAT satellite allow retrieving stratospheric profiles of various trace gases on a global scale, among them BrO for the first time. For limb observations in the UV/VIS spectral region the instrument measures scattered light with a complex distribution of light paths: the light is measured at different tangent heights and can be scattered or absorbed in the atmosphere or reflected by the ground. By means of spectroscopy and radiative transfer modelling these measurements can be inverted to retrieve the vertical distribution of stratospheric trace gases. The fully spherical 3-D Monte Carlo radiative transfer model "Tracy-II" is applied in this study. The Monte Carlo method benefits from conceptual simplicity and allows realizing the concept of full spherical geometry of the atmosphere and also its 3-D properties, which is important for a realistic description of the limb geometry. Furthermore it allows accounting for horizontal gradients in the distribution of trace gases. In this study the effect of horizontally inhomogeneous distributions of trace gases along flight/viewing direction on the retrieval of profiles is investigated. We introduce a tomographic method to correct for this effect by combining consecutive limb scanning sequences and utilizing the overlap in their measurement sensitivity regions. It is found that if horizontal inhomogenity is not properly accounted for, typical errors of 20% for NO2 and up to 50% for OClO around the altitude of the profile peak can arise for measurements close to the Arctic polar vortex boundary in boreal winter.
Impact of nonlinearity on changing the a priori of trace gas profile 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 maximum a posteriori (MAP) estimates of atmospheric profiles from the Tropospheric Emission Spectrometer (TES) contains a priori information that may vary geographically, which is a confounding factor in the analysis and physical interpretation of an ensemble of profiles. One mitigation strategy is to transform 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. The robustness of this assumption is tested 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. 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.
Halogenated organic species over the tropical South American rainforest
Authors: Gebhardt S. , Colomb A. , Hofmann R. , Williams J. , Lelieveld J.
Published: April 2010

Abstract. Airborne measurements of the halogenated trace gases methyl chloride, methyl bromide and chloroform were conducted over the Atlantic Ocean and about 1000 km of pristine tropical rainforest in Suriname and French Guyana (3–6° N, 51–59° W) in October 2005. In the boundary layer (0–1.4 km), maritime air masses, advected over the forest by southeasterly trade winds, were measured at various distances from the coast. Since the organohalogens presented here have relatively long atmospheric lifetimes (0.4–1.0 years) in comparison to the advection times from the coast (1–2 days), emissions will accumulate in air traversing the rainforest. The distributions of methyl chloride, methyl bromide and chloroform were analyzed as a function of time the air spent over land and the respective relationship used to determine net fluxes from the rainforest for one week within the long dry season. Net fluxes from the rainforest ecosystem have been calculated for methyl chloride and chloroform as 9.5 (±3.8 2σ) and 0.35 (±0.15 2σ)μg m-2 h−1, respectively. No significant flux was observed for methyl bromide within the limits of these measurements. The global budget of methyl chloride contains large uncertainties, in particular with regard to a possible source from tropical vegetation. Our measurements are used in a large-scale approach to determine the net flux from a tropical ecosystem to the planetary boundary layer. The obtained global net flux of 1.5 (±0.6 2σ) Tg yr-1 for methyl chloride is at the lower end of current estimates for tropical vegetation sources, which helps to constrain the range of tropical sources and sinks (0.82 to 8.2 Tg yr-1 from tropical plants, 0.03 to 2.5 Tg yr-1 from senescent/dead leaves and a sink of 0.1 to 1.6 Tg yr-1 by soil uptake). Nevertheless, these results show that the contribution of the rainforest ecosystem is the major source in the global budget of methyl chloride. For chloroform, the extrapolated global net flux from tropical ecosystems is 56 (±23 2σ) Gg yr−1, which is of minor importance compared to the total global sources and might be already contained in the soil emission term.
Technical note: Measuring tropospheric OH and HO2by laser-induced fluorescence at low pressure. A comparison of calibration techniques
Authors: Dusanter S. , Vimal D. , Stevens P. S.
Published: April 2010

Abstract. The hydroxyl radical (OH) is one of the most important oxidants in the atmosphere, as it is involved in many reactions that affect regional air quality and global climate change. Because of its high reactivity, measurements of OH radical concentrations in the atmosphere are difficult, and often require careful calibrations that rely on the production of a known concentration of OH at atmospheric pressure. The Indiana University OH instrument, based on the Fluorescence Assay by Gas Expansion technique (FAGE), has been calibrated in the laboratory using two different approaches: the production of OH from the UV-photolysis of water-vapor, and the steady-state production of OH from the reaction of ozone with alkenes. The former technique relies on two different actinometric methods to measure the product of the lamp flux at 184.9 nm and the photolysis time. This quantity derived from N2O actinometry was found to be 1.5 times higher than that derived from O2 actinometry. The water photolysis and ozone-alkene techniques are shown to agree within their experimental uncertainties (respectively 17% and 44%), although the sensitivities derived from the ozone-alkene technique were systematically lower by 40% than those derived from the water-vapor UV- photolysis technique using O2 actinometry. The agreement between the two different methods improves the confidence of the water-vapor photolysis method as an accurate calibration technique for HOx instruments. Because several aspects of the mechanism of the gas phase ozonolysis of alkenes are still uncertain, this technique should be used with caution to calibrate OH instruments.
Detection of regional scale sea-to-air oxygen emission related to spring bloom near Japan by using in-situ measurements of the atmospheric oxygen/nitrogen ratio
Authors: Yamagishi H. , Tohjima Y. , Mukai H. , Sasaoka K.
Published: April 2010

Abstract. We have been carrying out in-situ monitoring of atmospheric O2/N2 ratio at Cape Ochi-ishi (COI; 43°10' N, 145°30' E) in the northern part of Japan since March 2005 by using a modified gas chromatography/thermal conductivity detector (GC/TCD). The standard deviation of the O2/N2 ratio is estimated to be about ±14 per meg (≈3 ppm) with intervals of 10 minutes. Thus, the in-situ measurement system has a 1σ precision of ± 6 per meg (≈1.2 ppm) for one-hour mean O2/N2 ratio. Atmospheric potential oxygen (APO≈O2+1.1 CO2), which is conserved with respect to terrestrial photosynthesis and respiration but reflects changes in air-sea O2 and CO2 fluxes, shows large variabilities from April to early July 2005. Distribution of satellite-derived marine primary production indicates occurrences of strong bloom in the Japan Sea and the latitudinal band between 30° and 40° N in the western North Pacific in April and in the Okhotsk Sea and northeastern region near Hokkaido Island in the North Pacific in June. Back trajectory analysis of air masses indicates that high values of APO, which last for several hours or several days, can be attributed to the oxygen emission associated with the spring bloom of active primary production.
First retrieval of tropospheric aerosol profiles using MAX-DOAS and 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. By analyzing the measured spectra of scattered sunlight with DOAS and optimal estimation methods, we first retrieve the aerosol optical depth (τ) and the vertical profile of the aerosol extinction coefficient (k) at 476 nm in the lower troposphere. These retrieved quantities are characterized through comparisons with coincident lidar and sky radiometer measurements. The retrieved k 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 k at 0–1 km are obtained for the retrieved τ values, demonstrating that MAX-DOAS provides a new, unique aerosol dataset in the lower troposphere.
Morphology of the tropopause layer and lower stratosphere above a tropical cyclone: a case study on cyclone Davina (1999)
Authors: Cairo F. , Buontempo C. , MacKenzie A. R. , Schiller C. , Volk C. M. , Adriani A. , Mitev V. , Matthey R. , Di Donfrancesco G. , Oulanovsky A. , Ravegnani F. , Yushkov V. , Snels M. , Cagnazzo C. , Stefanutti L.
Published: April 2010

Abstract. During the APE-THESEO mission in the Indian Ocean the Myasishchev Design Bureau stratospheric research aircraft M55 Geophysica performed a flight over and within the inner core region of tropical cyclone Davina. Measurements of total water, water vapour, temperature, aerosol backscattering, ozone and tracers were made and are discussed here in comparison with the averages of those quantities acquired during the campaign time frame. Temperature anomalies in the tropical tropopause layer (TTL), warmer than average in the lower part and colder than average in the upper TTL were observed. Ozone was strongly reduced compared to its average value, and thick cirrus decks were present up to the cold point, sometimes topped by a layer of very dry air. Evidence for meridional transport of trace gases in the stratosphere above the cyclone was observed and perturbed water distribution in the TTL was documented. The paper discuss possible processes of dehydration induced by the cirrus forming above the cyclone, and change in the chemical tracer and water distribution in the lower stratosphere 400–430 K due to meridional transport from the mid-latitudes and link with Davina. Moreover it compares the data prior and after the cyclone passage to discuss its actual impact on the atmospheric chemistry and thermodynamics.
Data assimilation of dust aerosol observations for the CUACE/dust forecasting system
Authors: Niu T. , Gong S. L. , Zhu G. F. , Liu H. L. , Hu X. Q. , Zhou C. H. , Wang Y. Q.
Published: April 2010

Abstract. A data assimilation system (DAS) was developed for the Chinese Unified Atmospheric Chemistry Environment – Dust (CUACE/Dust) forecast system and applied in the operational forecasts of sand and dust storm (SDS) in spring 2006. The system is based on a three dimensional variational method (3D-Var) and uses extensively the measurements of surface visibility (phenomena) and dust loading retrieval from the Chinese geostationary satellite FY-2C. By a number of case studies, the DAS was found to provide corrections to both under- and over-estimates of SDS, presenting a major improvement to the forecasting capability of CUACE/Dust in the short-term variability in the spatial distribution and intensity of dust concentrations in both source regions and downwind areas. The seasonal mean Threat Score (TS) over the East Asia in spring 2006 increased from 0.22 to 0.31 by using the data assimilation system, a 41% enhancement. The forecast results with DAS usually agree with the dust loading retrieved from FY-2C and visibility distribution from surface meteorological stations, which indicates that the 3D-Var method is very powerful by the unification of observation and numerical model to improve the performance of forecast model.
VOC reactivity in central California: comparing an air quality model to ground-based measurements
Authors: Steiner A. L. , Cohen R. C. , Harley R. A. , Tonse S. , Millet D. B. , Schade G. W. , Goldstein A. H.
Published: April 2010

Abstract. Volatile organic compound (VOC) reactivity in central California is examined using a photochemical air quality model (the Community Multiscale Air Quality model; CMAQ) and ground-based measurements to evaluate the contribution of VOC to photochemical activity. We classify VOC into four categories: anthropogenic, biogenic, aldehyde, and other oxygenated VOC. Anthropogenic and biogenic VOC consist of primary emissions, while aldehydes and other oxygenated VOC include both primary anthropogenic emissions and secondary products from primary VOC oxidation. To evaluate the model treatment of VOC chemistry, we compare calculated and modeled OH and VOC reactivities using the following metrics: 1) cumulative distribution functions of NOx concentration and VOC reactivity (ROH,VOC), 2) the relationship between ROH,VOC and NOx, 3) total OH reactivity (ROH,total) and speciated contributions, and 4) the relationship between speciated ROH,VOC and NOx. We find that the model predicts ROH,total to within 25–40% at three sites representing urban (Sacramento), suburban (Granite Bay) and rural (Blodgett Forest) chemistry. However in the urban area of Fresno, the model under predicts NOx and VOC emissions by a factor of 2–3. At all locations the model is consistent with observations of the relative contributions of total VOC. In urban areas, anthropogenic and biogenic ROH,VOC are predicted fairly well over a range of NOx conditions. In suburban and rural locations, anthropogenic and other oxygenated ROH,VOC relationships are reproduced, but calculated biogenic and aldehyde ROH,VOC are often poorly characterized by measurements, making evaluation of the model with available data unreliable. In central California, 30–50% of the modeled urban VOC reactivity is due to aldehydes and other oxygenated species, and the total oxygenated ROH,VOC is nearly equivalent to anthropogenic VOC reactivity. In rural vegetated regions, biogenic and aldehyde reactivity dominates. This indicates that more attention needs to be paid to the accuracy of models and measurements of both primary emissions of oxygenated VOC and secondary production of oxygenates, especially formaldehyde and other aldehydes, and that a more comprehensive set of oxygenated VOC measurements is required to include all of the important contributions to atmospheric reactivity.
Boundary layer physics over snow and ice
Authors: Anderson P. S. , Neff W. D.
Published: April 2010

Abstract. Observations of the unique chemical environment over snow and ice in recent decades, particularly in the polar regions, have stimulated increasing interest in the boundary layer processes that mediate exchanges between the ice/snow interface and the atmosphere. This paper provides a review of the underlying concepts and examples from recent field studies in polar boundary layer meteorology, which will generally apply to atmospheric flow over snow and ice surfaces. It forms a companion paper to the chemistry review papers in this special issue of ACP that focus on processes linking halogens to the depletion of boundary layer ozone in coastal environments, mercury transport and deposition, snow photochemistry, and related snow physics. In this context, observational approaches, stable boundary layer behavior, the effects of a weak or absent diurnal cycle, and transport and mixing over the heterogeneous surfaces characteristic of coastal ocean environments are of particular relevance.
Impact of climate change on tropospheric ozone and its global budgets
Authors: Zeng G. , Pyle J. A. , Young P. J.
Published: April 2010

Abstract. We present the chemistry-climate model UMCAM in which a relatively detailed tropospheric chemical module has been incorporated into the UK Met Office's Unified Model version 4.5. We obtain good agreements between the modelled ozone/nitrogen species and a range of observations including surface ozone measurements, ozone sonde data, and some aircraft campaigns. Four 2100 calculations assess model responses to projected changes of anthropogenic emissions (SRES A2), climate change (due to doubling CO2), and idealised climate change-associated changes in biogenic emissions (i.e. 50% increase of isoprene emission and doubling emissions of soil-NOx). The global tropospheric ozone burden increases significantly for all the 2100 A2 simulations, with the largest response caused by the increase of anthropogenic emissions. Climate change has diverse impacts on O3 and its budgets through changes in circulation and meteorological variables. Increased water vapour causes a substantial ozone reduction especially in the tropical lower troposphere (>10 ppbv reduction over the tropical ocean). On the other hand, an enhanced stratosphere-troposphere exchange of ozone, which increases by 80% due to doubling CO2, contributes to ozone increases in the extratropical free troposphere which subsequently propagate to the surface. Projected higher temperatures favour ozone chemical production and PAN decomposition which lead to high surface ozone levels in certain regions. Enhanced convection transports ozone precursors more rapidly out of the boundary layer resulting in an increase of ozone production in the free troposphere. Lightning-produced NOx increases by about 22% in the doubled CO2 climate and contributes to ozone production. The response to the increase of isoprene emissions shows that the change of ozone is largely determined by background NOx levels: high NOx environment increases ozone production; isoprene emitting regions with low NOx levels see local ozone decreases, and increase of ozone levels in the remote region due to the influence of PAN chemistry. The calculated ozone changes in response to a 50% increase of isoprene emissions are in the range of between −8 ppbv to 6 ppbv. Doubling soil-NOx emissions will increase tropospheric ozone considerably, with up to 5 ppbv in source regions.
How small is a small cloud?
Authors: Koren I. , Oreopoulos L. , Feingold G. , Remer L. A. , Altaratz O.
Published: April 2010

Abstract. The interplay between clouds and aerosols and their contribution to the radiation budget is one of the largest uncertainties of climate change. Most work to date has separated cloudy and cloud-free areas in order to evaluate the individual radiative forcing of aerosols, clouds, and aerosol effects on clouds. Here we examine the size distribution and the optical properties of small, sparse cumulus clouds and the associated optical properties of what is considered a cloud-free atmosphere within the cloud field. We show that any separation between clouds and cloud free atmosphere will incur errors in the calculated radiative forcing. The nature of small cumulus cloud size distributions suggests that at any resolution, a significant fraction of the clouds are missed, and their optical properties are relegated to the apparent cloud-free optical properties. At the same time, the cloudy portion incorporates significant contribution from non-cloudy pixels. We show that the largest contribution to the total cloud reflectance comes from the smallest clouds and that the spatial resolution changes the apparent energy flux of a broken cloudy scene. When changing the resolution from 30 m to 1 km (Landsat to MODIS) the average "cloud-free" reflectance at 1.65 μm increases from 0.0095 to 0.0115 (>20%), the cloud reflectance decreases from 0.13 to 0.066 (~50%), and the cloud coverage doubles, resulting in an important impact on climate forcing estimations. The apparent aerosol forcing is on the order of 0.5 to 1 Wm−2 per cloud field.
N2O release from agro-biofuel production negates global warming reduction by replacing fossil fuels
Authors: Crutzen P. J. , Mosier A. R. , Smith K. A. , Winiwarter W.
Published: April 2010

Abstract. The relationship, on a global basis, between the amount of N fixed by chemical, biological or atmospheric processes entering the terrestrial biosphere, and the total emission of nitrous oxide (N2O), has been re-examined, using known global atmospheric removal rates and concentration growth of N2O as a proxy for overall emissions. For both the pre-industrial period and in recent times, after taking into account the large-scale changes in synthetic N fertiliser production, we find an overall conversion factor of 3–5% from newly fixed N to N2O-N. We assume the same factor to be valid for biofuel production systems. It is covered only in part by the default conversion factor for "direct" emissions from agricultural crop lands (1%) estimated by IPCC (2006), and the default factors for the "indirect" emissions (following volatilization/deposition and leaching/runoff of N: 0.35–0.45%) cited therein. However, as we show in the paper, when additional emissions included in the IPCC methodology, e.g. those from livestock production, are included, the total may not be inconsistent with that given by our "top-down" method. When the extra N2O emission from biofuel production is calculated in "CO2-equivalent" global warming terms, and compared with the quasi-cooling effect of "saving" emissions of fossil fuel derived CO2, the outcome is that the production of commonly used biofuels, such as biodiesel from rapeseed and bioethanol from corn (maize), depending on N fertilizer uptake efficiency by the plants, can contribute as much or more to global warming by N2O emissions than cooling by fossil fuel savings. Crops with less N demand, such as grasses and woody coppice species, have more favourable climate impacts. This analysis only considers the conversion of biomass to biofuel. It does not take into account the use of fossil fuel on the farms and for fertilizer and pesticide production, but it also neglects the production of useful co-products. Both factors partially compensate each other. This needs to be analyzed in a full life cycle assessment.
Past and future scenarios of the effect of carbon dioxide on plant growth and transpiration for three vegetation types of southwestern France
Authors: Calvet J.-C. , Gibelin A.-L. , Roujean J.-L. , Martin E. , Le Moigne P. , Douville H. , Noilhan J.
Published: April 2010

Abstract. The sensitivity of an operational CO2-responsive land surface model (the ISBA-A-gs model of Météo-France) to the atmospheric CO2 concentration, (CO2), is investigated for 3 vegetation types (winter wheat, irrigated maize, coniferous forest). Past (1960) and future (2050) scenarios of (CO2) corresponding to 320 ppm and 550 ppm, respectively, are explored. The sensitivity study is performed for 4 annual cycles presenting contrasting conditions of precipitation regime and air temperature, based on continuous measurements performed on the SMOSREX site near Toulouse, in southwestern France. A significant CO2-driven reduction of canopy conductance is simulated for the irrigated maize and the coniferous forest. The reduction is particularly large for maize, from 2000 to 2050 (−18%), and triggers a drop in optimum irrigation (−30 mm y−1). In the case of wheat, the response is more complex, with an equal occurrence of enhanced or reduced canopy conductance.
Correlation between equatorial Kelvin waves and the occurrence of extremely thin ice clouds at the tropical tropopause
Authors: Immler F. , Krüger K. , Fujiwara M. , Verver G. , Rex M. , Schrems O.
Published: April 2010

Abstract. A number of field-campaigns in the tropics have been conducted in recent years with two different LIDAR systems at Paramaribo (5.8° N, 55.2° W), Suriname. The lidars detect particles in the atmosphere with high vertical and temporal resolution and are capable of detecting extremely thin cloud layers which frequently occur in the tropical tropopause layer (TTL). Radiosonde as well as operational ECMWF analysis showed that equatorial Kelvin waves propagated in the TTL and greatly modulated its temperature structure. We found a clear correlation between the temperature anomalies introduced by these waves and the occurrence of thin cirrus in the TTL. In particular we found that extremely thin ice clouds form regularly where cold anomalies shift the tropopause to high altitudes. These findings suggest an influence of Kelvin wave activity on the dehydration in the TTL and thus on the global stratospheric water vapour concentration.