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The isotopic composition of precipitation from a winter storm – a case study with the limited-area model COSMOiso

Stable water isotopes are valuable tracers of the atmospheric water cycle, and potentially provide useful information also on weather-related processes. In order to further explore this potential, the water isotopes H218O and HDO are incorporated into the limited-area model COSMO. In a first case study, the new COSMOiso model is used for simulating a winter storm event in January 1986 over the eastern United States associated with intense frontal precipitation. The modelled isotope ratios in precipitation and water vapour are compared to spatially distributed δ18O observations. COSMOiso very accurately reproduces the statistical distribution of δ18O in precipitation, and also the synoptic-scale spatial pattern and temporal evolution agree well with the measurements. Perpendicular to the front that triggers most of the rainfall during the event, the model simulates a gradient in the isotopic composition of the precipitation, with high δ18O values in the warm air and lower values in the cold sector behind the front. This spatial pattern is created through an interplay of large scale air mass advection, removal of heavy isotopes by precipitation at the front and microphysical interactions between rain drops and water vapour beneath the cloud base. This investigation illustrates the usefulness of high resolution, event-based model simulations for understanding the complex processes that cause synoptic-scale variability of the isotopic composition of atmospheric waters. In future research, this will be particularly beneficial in combination with laser spectrometric isotope observations with high temporal resolution.
The Mineral Dust Cycle in EMAC 2.40: sensitivity to the spectral resolution and the dust emission scheme

This first detailed analysis of the mineral dust cycle in the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model system investigates the performance of two dust emission schemes, following the approach of Balkanski et al. (2004) and Tegen et al. (2002), respectively, and the influence of the horizontal model resolution. Here the spectral resolutions T42, T63, T85, and T106 are investigated. A basic sulphur chemistry, enabling the coating of insoluble dust particles to make them soluble, is employed in order to realistically describe the ageing and wet deposition of mineral dust. Independent of the dust emission scheme the five-year simulations with the horizontal resolutions T42 and T63 produce unrealistically high emissions at some grid points in the Tarim Basin in Central Asia, leading to very high dust loads in polar regions. With these coarse resolutions, dust source grid points in the basin and elevated grid points of the Himalayas with high wind speeds cannot be distinguished, causing this overestimation. In T85 and T106 these regions are well separated and considerably less dust is emitted there. With the chosen model setup, the dust emission scheme by Balkanski et al. (2004) places the global maximum of emissions in the Thar Desert in India. This is unrealistic as the Sahara Desert is known to be the largest dust source in the world. This is the main deficiency of this scheme compared to the one by Tegen et al. (2002), which, based on a qualitative comparison to AEROCOM data, produces a very reasonable distribution of emissions and dust loads in simulations with resolutions T85 and T106. For future climate simulations with EMAC focusing on mineral dust, we recommend to use the dust emission scheme by Tegen et al. (2002) and a model resolution of at least T85. Simulations of two selected episodes and comparison to observational data sets show that in this model configuration EMAC is able to realistically simulate also intense, episodic events of dust emission and long-range transport.
Impacts of changes in land use and land cover on atmospheric chemistry and air quality over the 21st century

The effects of future land use and land cover change on the chemical composition of the atmosphere and air quality are largely unknown. To investigate the potential effects associated with future changes in vegetation driven by atmospheric CO2 concentrations, climate, and anthropogenic land use over the 21st century, we performed a series of model experiments combining a general circulation model with a dynamic global vegetation model and an atmospheric chemical-transport model. Our results indicate that climate- and CO2-induced changes in vegetation composition and density between 2100 and 2000 could lead to decreases in summer afternoon surface ozone of up to 10 ppb over large areas of the northern mid-latitudes. This is largely driven by the substantial increases in ozone dry deposition associated with increases in vegetation density in a warmer climate with higher atmospheric CO2 abundance. Climate-driven vegetation changes over the period 2000–2100 lead to general increases in isoprene emissions, globally by 15% in 2050 and 36% in 2100. These increases in isoprene emissions result in decreases in surface ozone concentrations where the NOx levels are low, such as in remote tropical rainforests. However, over polluted regions, such as the northeastern United States, ozone concentrations are calculated to increase with higher isoprene emissions in the future. Increases in biogenic emissions also lead to higher concentrations of secondary organic aerosols, which increase globally by 10% in 2050 and 20% in 2100. Summertime surface concentrations of secondary organic aerosols are calculated to increase by up to 1 μg m−3 and double for large areas in Eurasia over the period of 2000–2100. When we use a scenario of future anthropogenic land use change, we find less increase in global isoprene emissions due to replacement of higher-emitting forests by lower-emitting cropland. The global atmospheric burden of secondary organic aerosols changes little by 2100 when we account for future land use change, but both secondary organic aerosols and ozone show large regional changes at the surface.
Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional air quality and atmospheric parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O:C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O:C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the markers m/z 55, 57, and 44 is developed here and allows for a first-order-estimation of COA in urban air. This study emphasizes the importance of cooking activities for ambient air quality and confirms the importance of chemical composition measurements with a high mass and time resolution.
Dust aerosol impact on North Africa climate: a GCM investigation of aerosol-cloud-radiation interactions using A-Train satellite data

The climatic effects of dust aerosols in North Africa have been investigated using the atmospheric general circulation model (AGCM) developed at the University of California, Los Angeles (UCLA). The model includes an efficient and physically based radiation parameterization scheme developed specifically for application to clouds and aerosols. Parameterization of the effective ice particle size in association with the aerosol first indirect effect based on ice cloud and aerosol data retrieved from A-Train satellite observations have been employed in climate model simulations. Offline simulations reveal that the direct solar, IR, and net forcings by dust aerosols at the top of the atmosphere (TOA) generally increase with increasing aerosol optical depth. When the dust semi-direct effect is included with the presence of ice clouds, positive IR radiative forcing is enhanced since ice clouds trap substantial IR radiation, while the positive solar forcing with dust aerosols alone has been changed to negative values due to the strong reflection of solar radiation by clouds, indicating that cloud forcing associated with aerosol semi-direct effect could exceed direct aerosol forcing. With the aerosol first indirect effect, the net cloud forcing is generally reduced in the case for an ice water path (IWP) larger than 20 g m−2. The magnitude of the reduction increases with IWP. AGCM simulations show that the reduced ice crystal mean effective size due to the aerosol first indirect effect results in less OLR and net solar flux at TOA over the cloudy area of the North Africa region because ice clouds with smaller size trap more IR radiation and reflect more solar radiation. The precipitation in the same area, however, increases due to the aerosol indirect effect on ice clouds, corresponding to the enhanced convection as indicated by reduced OLR. Adding the aerosol direct effect into the model simulation reduces the precipitation in the normal rainfall band over North Africa, where precipitation is shifted to the south and the northeast produced by the absorption of sunlight and the subsequent heating of the air column by dust particles. As a result, rainfall is drawn further inland to the northeast. This study represents the first attempt to quantify the climate impact of the aerosol indirect effect using a GCM in connection with A-Train satellite data. The parameterization for the aerosol first indirect effect developed in this study can be readily employed for application to other GCMs.
Gravity wave variances and propagation derived from AIRS radiances

As the first gravity wave (GW) climatology study using nadir-viewing infrared sounders, 50 Atmospheric Infrared Sounder (AIRS) radiance channels are selected to estimate GW variances at pressure levels between 2–100 hPa. The GW variance for each scan in the cross-track direction is derived from radiance perturbations in the scan, independently of adjacent scans along the orbit. Since the scanning swaths are perpendicular to the satellite orbits, which are inclined meridionally at most latitudes, the zonal component of GW propagation can be inferred by differencing the variances derived between the westmost and the eastmost viewing angles. Consistent with previous GW studies using various satellite instruments, monthly mean AIRS variance shows large enhancements over meridionally oriented mountain ranges as well as some islands at winter hemisphere high latitudes. Enhanced wave activities are also found above tropical deep convective regions. GWs prefer to propagate westward above mountain ranges, and eastward above deep convection. AIRS 90 field-of-views (FOVs), ranging from +48° to −48° off nadir, can detect large-amplitude GWs with a phase velocity propagating preferentially at steep angles (e.g., those from orographic and convective sources). The annual cycle dominates the GW variances and the preferred propagation directions for all latitudes. Indication of a weak two-year variation in the tropics is found, which is presumably related to the Quasi-biennial oscillation (QBO). AIRS geometry makes its out-tracks capable of detecting GWs with vertical wavelengths substantially shorter than the thickness of instrument weighting functions. The novel discovery of AIRS capability of observing shallow inertia GWs will expand the potential of satellite GW remote sensing and provide further constraints on the GW drag parameterization schemes in the general circulation models (GCMs).
Physical and optical properties of 2010 Eyjafjallajökull volcanic eruption aerosol: ground-based, Lidar and airborne measurements in France

During the Eyjafjallajökull eruption (14 April to 24 May 2010), the volcanic aerosol cloud was observed across Europe by several airborne in situ and ground-based remote-sensing instruments. On 18 and 19 May, layers of depolarizing particles (i.e. non-spherical particles) were detected in the free troposphere above the Puy de Dôme station, (PdD, France) with a Rayleigh-Mie LIDAR emitting at a wavelength of 355 nm, with parallel and crossed polarization channels. These layers in the free troposphere (FT) were also well captured by simulations with the Lagrangian particle dispersion model FLEXPART, which furthermore showed that the ash was eventually entrained into the planetary boundary layer (PBL). Indeed, the ash cloud was then detected and characterized with a comprehensive set of in situ instruments at the Puy de Dôme station (PdD). In agreement with the FLEXPART simulation, up to 65 μg m−3 of particle mass and 2.2 ppb of SO2 were measured at PdD, corresponding to concentrations higher than the 95 percentile of 2 yr of measurements at PdD. Moreover, the number concentration of particles increased to 24 000 cm−3, mainly in the submicronic mode, but a supermicronic mode was also detected with a modal diameter of 2 μm. The resulting optical properties of the ash aerosol were characterized by a low scattering Ångström exponent (0.98), showing the presence of supermicronic particles. For the first time to our knowledge, the combination of in situ optical and physical characterization of the volcanic ash allowed the calculation of the mass-to-extinction ratio (η) with no assumptions on the aerosol density. The mass-to-extinction ratio was found to be significantly different from the background boundary layer aerosol (max: 1.57 g m−2 as opposed to 0.33 ± 0.03 g m−2). Using this ratio, ash mass concentration in the volcanic plume derived from LIDAR measurements was found to be 655 ± 23 μg m−3 when the plume was located in the FT (3000 m above the sea level – a.s.l.). This ratio could also be used to retrieve an aerosol mass concentration of 579 ± 60 μg m−3 on 19 April, when LIDAR observations detected the ash cloud at 3000 m a.s.l. in correspondence with model simulations (FLEXPART). On 22 April, another ash plume entered the BL, and although it was more diluted than during the May episode, the French research aircraft ATR42 that passed over Clermont-Ferrand in the PBL confirmed the presence of particles with a supermicronic mode, again with a modal diameter at 2 μm. This data set combining airborne, ground-based and remote sensing observations with dispersion model simulations shows an overall very good coherence during the volcanic eruption period, which allows a good confidence in the characteristics of the ash particles that can be derived from this unique data set.
Impact of lightning-NO on eastern United States photochemistry during the summer of 2006 as determined using the CMAQ model

A lightning-nitrogen oxide (NO) algorithm is implemented in the Community Multiscale Air Quality Model (CMAQ) and used to evaluate the impact of lightning-NO emissions (LNOx) on tropospheric photochemistry over the United States during the summer of 2006. For a 500 mole per flash lightning-NO source, the mean summertime tropospheric NO2 column agrees with satellite-retrieved columns to within −5 to +13%. Temporal fluctuations in the column are moderately well simulated; however, the addition of LNOx does not lead to a better simulation of day-to-day variability. The contribution of lightning-NO to the model column ranges from &sim;10% in the northern US to >45% in the south-central and southeastern US. Lightning-NO adds up to 20 ppbv to upper tropospheric model ozone and 1.5–4.5 ppbv to 8-h maximum surface layer ozone, although, on average, the contribution of LNOx to model surface ozone is 1–2 ppbv less on poor air quality days. LNOx increases wet deposition of oxidized nitrogen by 43% and total deposition of nitrogen by 10%. This additional deposition reduces the mean magnitude of the CMAQ low-bias in nitrate wet deposition with respect to National Atmospheric Deposition monitors to near zero. Differences in urban/rural biases between model and satellite-retrieved NO2 columns were examined to identify possible problems in model chemistry and/or transport. CMAQ columns were too large over urban areas. Biases at other locations were minor after accounting for the impacts of lightning-NO emissions and the averaging kernel on model columns. In order to obtain an upper bound on the contribution of uncertainties in NOy chemistry to upper tropospheric NOx low biases, sensitivity calculations with updated chemistry were run for the time period of the Intercontinental Chemical Transport Experiment (INTEX-A) field campaign (summer 2004). After adjusting for possible interferences in NO2 measurements and averaging over the entire campaign, these updates reduced 7–9 km biases from 32 to 17% and 9–12 km biases from 57 to 46%. While these changes lead to better agreement, a considerable unexplained NO2 low-bias remains in the uppermost troposphere.
The climatology, propagation and excitation of ultra-fast Kelvin waves as observed by meteor radar, Aura MLS, TRMM and in the Kyushu-GCM

Wind measurements from a meteor radar on Ascension Island (8° S, 14° W) and simultaneous temperature measurements from the Aura MLS instrument are used to characterise ultra-fast Kelvin waves (UFKW) of zonal wavenumber 1 (E1) in the mesosphere and lower thermosphere (MLT) in the years 2005–2010. These observations are compared with some predictions of the Kyushu-general circulation model. Good agreement is found between observations of the UFKW in the winds and temperatures, and also with the properties of the waves in the Kyushu-GCM. UFKW are found at periods between 2.5–4.5 days with amplitudes of up to 40 m s−1 in the zonal winds and 6 K in the temperatures. The average vertical wavelength is found to be 44 km. Amplitudes vary with latitude in a Gaussian manner with the maxima centred over the equator. Dissipation of the waves results in monthly-mean eastward accelerations of 0.2–0.9 m s−1 day−1 at heights around 95 km, with 5-day mean peak values of 4 m s−1 day−1. Largest wave amplitudes and variances are observed over Indonesia and central Africa and may be a result of very strong moist convective heating over those regions. Rainfall data from TRMM are used as a proxy for latent-heat release in an investigation of the excitation of these waves. No strong correlation is found between the occurrence of large-amplitude mesospheric UFKW events and either the magnitude of the equatorial rainfall or the amplitudes of E1 signatures in the rainfall time series, indicating that either other sources or the propagation environment are more important in determining the amplitude of UFKW in the MLT. A strong semiannual variation in wave amplitudes is observed. Intraseasonal oscillations (ISOs) with periods 25–60 days are evident in the zonal background winds, zonal-mean temperature, UFKW amplitudes, UFKW accelerations and the rainfall rate. This suggests that UFKW play a role in carrying the signature of tropospheric ISOs to the MLT region.
Evaluation of cloud fraction and its radiative effect simulated by IPCC AR4 global models against ARM surface observations

Cloud Fraction (CF) is the dominant modulator of radiative fluxes. In this study, we evaluate CF simulated in the IPCC AR4 GCMs against ARM long-term ground-based measurements, with a focus on the vertical structure, total amount of cloud and its effect on cloud shortwave transmissivity. Comparisons are performed for three climate regimes as represented by the Department of Energy Atmospheric Radiation Measurement (ARM) sites: Southern Great Plains (SGP), Manus, Papua New Guinea and North Slope of Alaska (NSA). Our intercomparisons of three independent measurements of CF or sky-cover reveal that the relative differences are usually less than 10% (5%) for multi-year monthly (annual) mean values, while daily differences are quite significant. The total sky imager (TSI) produces smaller total cloud fraction (TCF) compared to a radar/lidar dataset for highly cloudy days (CF > 0.8), but produces a larger TCF value than the radar/lidar for less cloudy conditions (CF < 0.3). The compensating errors in lower and higher CF days result in small biases of TCF between the vertically pointing radar/lidar dataset and the hemispheric TSI measurements as multi-year data is averaged. The unique radar/lidar CF measurements enable us to evaluate seasonal variation of cloud vertical structures in the GCMs. Both inter-model deviation and model bias against observation are investigated in this study. Another unique aspect of this study is that we use simultaneous measurements of CF and surface radiative fluxes to diagnose potential discrepancies among the GCMs in representing other cloud optical properties than TCF. The results show that the model-observation and inter-model deviations have similar magnitudes for the TCF and the normalized cloud effect, and these deviations are larger than those in surface downward solar radiation and cloud transmissivity. This implies that other dimensions of cloud in addition to cloud amount, such as cloud optical thickness and/or cloud height, have a similar magnitude of disparity as TCF within the GCMs, and suggests that the better agreement among GCMs in solar radiative fluxes could be a result of compensating effects from errors in cloud vertical structure, overlap assumption, cloud optical depth and/or cloud fraction. The internal variability of CF simulated in ensemble runs with the same model is minimal. Similar deviation patterns between inter-model and model-measurement comparisons suggest that the climate models tend to generate larger biases against observations for those variables with larger inter-model deviation. The GCM performance in simulating the probability distribution, transmissivity and vertical profiles of cloud are comprehensively evaluated over the three ARM sites. The GCMs perform better at SGP than at the other two sites in simulating the seasonal variation and probability distribution of TCF. However, the models remarkably underpredict the TCF at SGP and cloud transmissivity is less susceptible to the change of TCF than observed. In the tropics, most of the GCMs tend to underpredict CF and fail to capture the seasonal variation of CF at middle and low levels. The high-level CF is much larger in the GCMs than the observations and the inter-model variability of CF also reaches a maximum at high levels in the tropics, indicating discrepancies in the representation of ice cloud associated with convection in the models. While the GCMs generally capture the maximum CF in the boundary layer and vertical variability, the inter-model deviation is largest near the surface over the Arctic.