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Simulation of the diurnal variations of the oxygen isotope anomaly (Δ17O) of reactive atmospheric species

The isotope anomaly (Δ17O) of secondary atmospheric species such as nitrate (NO3−) or hydrogen peroxide (H2O2) has potential to provide useful constrains on their formation pathways. Indeed, the Δ17O of their precursors (NOx, HOx etc.) differs and depends on their interactions with ozone, which is the main source of non-zero Δ17O in the atmosphere. Interpreting variations of Δ17O in secondary species requires an in-depth understanding of the Δ17O of their precursors taking into account non-linear chemical regimes operating under various environmental settings. This article reviews and illustrates a series of basic concepts relevant to the propagation of the Δ17O of ozone to other reactive or secondary atmospheric species within a photochemical box model. We present results from numerical simulations carried out using the atmospheric chemistry box model CAABA/MECCA to explicitly compute the diurnal variations of the isotope anomaly of short-lived species such as NOx and HOx. Using a simplified but realistic tropospheric gas-phase chemistry mechanism, Δ17O was propagated from ozone to other species (NO, NO2, OH, HO2, RO2, NO3, N2O5, HONO, HNO3, HNO4, H2O2) according to the mass-balance equations, through the implementation of various sets of hypotheses pertaining to the transfer of Δ17O during chemical reactions. The model results confirm that diurnal variations in Δ17O of NOx predicted by the photochemical steady-state relationship during the day match those from the explicit treatment, but not at night. Indeed, the Δ17O of NOx is "frozen" at night as soon as the photolytical lifetime of NOx drops below ca. 10 min. We introduce and quantify the diurnally-integrated isotopic signature (DIIS) of sources of atmospheric nitrate and H2O2, which is of particular relevance to larger-scale simulations of Δ17O where high computational costs cannot be afforded.
Episodes of cross-polar transport in the Arctic troposphere during July 2008 as seen from models, satellite, and aircraft observations

During the POLARCAT summer campaign in 2008, two episodes (2–5 July and 7–10 July 2008) occurred where low-pressure systems traveled from Siberia across the Arctic Ocean towards the North Pole. The two cyclones had extensive smoke plumes from Siberian forest fires and anthropogenic sources in East Asia embedded in their associated air masses, creating an excellent opportunity to use satellite and aircraft observations to validate the performance of atmospheric transport models in the Arctic, which is a challenging model domain due to numerical and other complications. Here we compare transport simulations of carbon monoxide (CO) from the Lagrangian transport model FLEXPART and the Eulerian chemical transport model TOMCAT with retrievals of total column CO from the IASI passive infrared sensor onboard the MetOp-A satellite. The main aspect of the comparison is how realistic horizontal and vertical structures are represented in the model simulations. Analysis of CALIPSO lidar curtains and in situ aircraft measurements provide further independent reference points to assess how reliable the model simulations are and what the main limitations are. The horizontal structure of mid-latitude pollution plumes agrees well between the IASI total column CO and the model simulations. However, finer-scale structures are too quickly diffused in the Eulerian model. Applying the IASI averaging kernels to the model data is essential for a meaningful comparison. Using aircraft data as a reference suggests that the satellite data are biased high, while TOMCAT is biased low. FLEXPART fits the aircraft data rather well, but due to added background concentrations the simulation is not independent from observations. The multi-data, multi-model approach allows separating the influences of meteorological fields, model realisation, and grid type on the plume structure. In addition to the very good agreement between simulated and observed total column CO fields, the results also highlight the difficulty to identify a data set that most realistically represents the actual pollution state of the Arctic atmosphere.
Source attribution of the changes in atmospheric methane for 2006–2008

The recent increase of atmospheric methane is investigated by using two atmospheric inversions to quantify the distribution of sources and sinks for the 2006–2008 period, and a process-based model of methane emissions by natural wetland ecosystems. Methane emissions derived from the two inversions are consistent at a global scale: emissions are decreased in 2006 (−7 Tg) and increased in 2007 (+21 Tg) and 2008 (+18 Tg), as compared to the 1999–2006 period. The agreement on the latitudinal partition of the flux anomalies for the two inversions is fair in 2006, good in 2007, and not good in 2008. In 2007, a positive anomaly of tropical emissions is found to be the main contributor to the global emission anomalies (~60–80%) for both inversions, with a dominant share attributed to natural wetlands (~2/3), and a significant contribution from high latitudes (~25%). The wetland ecosystem model produces smaller and more balanced positive emission anomalies between the tropics and the high latitudes for 2006, 2007 and 2008, mainly due to precipitation changes during these years. At a global scale, the agreement between the ecosystem model and the inversions is good in 2008 but not satisfying in 2006 and 2007. Tropical South America and Boreal Eurasia appear to be major contributors to variations in methane emissions consistently in the inversions and the ecosystem model. Finally, changes in OH radicals during 2006–2008 are found to be less than 1% in inversions, with only a small impact on the inferred methane emissions.
The annual cycle in lower stratospheric temperatures revisited

Observed lower stratospheric temperatures show a prominent annual cycle. The cycles in the tropics and Northern Hemisphere are in phase and the cycle in the Southern Hemisphere has the opposite phase. In an elegant and influential paper, Yulaeva, Holton and Wallace (1994) explained the observed pattern as a direct consequence of hemispheric asymmetries in the dynamical forcing of the stratospheric circulation. They showed that in Microwave Sounding Unit channel 4 (weighting centered in the lower stratosphere) data the combined extratropical and the tropical temperature cycle nearly compensate and interpreted the out-of-phase temperature variations between tropics and extratropics as the temperature response to an annual cycle in the wave driven residual circulation. We show that the near-compensation of temperature variations observed by Yulaeva et al. (1994) is artefact of the weighting function of the MSU-4 channel and does not hold on individual pressure levels. We discuss in detail the conditions required that temperature variations compensate, and what insights can be obtained from analysis of tropical, extratropical and global mean temperature variations. Dynamically induced seasonal variations of lower stratospheric ozone lead to an amplification of the seasonal temperature cycle particularly in the tropics. The latitudinal structure of static stability also induces a significant deviation from compensation of tropical and combined extratropical temperature variations. In line with Yulaeva et al. (1994) we affirm that the see-saw pattern in the annual cycles of tropical and combined extratropical temperatures provides an important pointer to mechanistic models for interannual variability and trends, but additionally conclude that the feedback of dynamically induced ozone variations on temperatures and the latitudinal structure of static stability should be included as leading order processes in such models.
Toward unification of the multiscale modeling of the atmosphere

As far as the representation of deep moist convection is concerned, only two kinds of model physics are used at present: highly parameterized as in the conventional general circulation models (GCMs) and explicitly simulated as in the cloud-resolving models (CRMs). Ideally, these two kinds of model physics should be unified so that a continuous transition of model physics from one kind to the other takes place as the resolution changes. With such unification, the GCM can converge to a global CRM (GCRM) as the grid size is refined. This paper suggests two possible routes to achieve the unification. ROUTE I continues to follow the parameterization approach, but uses a unified parameterization that is applicable to any horizontal resolutions between those typically used by GCMs and CRMs. It is shown that a key to construct such a unified parameterization is to eliminate the assumption of small fractional area covered by convective clouds, which is commonly used in the conventional cumulus parameterizations either explicitly or implicitly. A preliminary design of the unified parameterization is presented, which demonstrates that such an assumption can be eliminated through a relatively minor modification of the existing mass-flux based parameterizations. Partial evaluations of the unified parameterization are also presented. ROUTE II follows the "multi-scale modeling framework (MMF)" approach, which takes advantage of explicit representation of deep moist convection and associated cloud-scale processes by CRMs. The Quasi-3-D (Q3-D) MMF is an attempt to broaden the applicability of MMF without necessarily using a fully three-dimensional CRM. This is accomplished using a network of cloud-resolving grids with large gaps. An outline of the Q3-D algorithm and highlights of preliminary results are reviewed.
Chemical composition of rainwater at Maldives Climate Observatory at Hanimaadhoo (MCOH)

Water-soluble inorganic components in rain deposited at the Maldives Climate Observatory Hanimaadhoo (MCOH) were examined to determine seasonality and possible source regions. The study, which is part of the Atmospheric Brown Cloud (ABC) project, covers the period June 2005 to December 2007. Air mass trajectories were used to separate the data into situations with transport of air from India and adjacent parts of the Asian continent during the months December and January (Indian group) and those with southerly flow from the Indian Ocean during the summer monsoon season June to September (Marine group). A third trajectory group was identified with transport from the northern parts of the Arabian Sea and adjacent land areas during the months March, April and October (Arabian Sea group). The concentrations of nss-SO42−, NH4+ and NO3− were more than a factor of 4 higher in the Indian group than in the Marine group. The average rainwater pH was significantly lower in the Indian group (4.7) than in the Marine group (6.0). This shows a pronounced influence of continental pollutants during December and January. The origin of the very high concentration of nss-Ca2+ found in the Marine group – a factor of 7 higher than in the Indian group – is unclear. We discuss various possibilities including long-range transport from the African or Australian continents, local dust from nearby islands and calcareous plankton debris and exopolymer gels emitted from the ocean surface. The occurrence of NO3− and NH4+ in the Marine group suggests emissions from the ocean surface. Part of the NO3− could also be associated with lightning over the ocean. Despite the fact that the concentrations of nss-SO42−, NO3−, and NH4+ were highest in the Indian group the wet deposition was at least as big in the Marine group reflecting the larger amount of rainfall during the monsoon season. The annual wet deposition of NO3−, NH4+ and nss-SO42− at MCOH is about a factor of three lower than observed at rural sites in India.
Dynamical states of low temperature cirrus

Low ice crystal concentration and sustained in-cloud supersaturation, commonly found in cloud observations at low temperature, challenge our understanding of cirrus formation. Heterogeneous freezing from effloresced ammonium sulfate, glassy aerosol, dust and black carbon are proposed to cause these phenomena; this requires low updrafts for cirrus characteristics to agree with observations and is at odds with the gravity wave spectrum in the upper troposphere. Background temperature fluctuations however can establish a "dynamical equilibrium" between ice production and sedimentation loss (as opposed to ice crystal formation during the first stages of cloud evolution and subsequent slow cloud decay) that explains low temperature cirrus properties. This newly-discovered state is favored at low temperatures and does not require heterogeneous nucleation to occur (the presence of ice nuclei can however facilitate its onset). Our understanding of cirrus clouds and their role in anthropogenic climate change is reshaped, as the type of dynamical forcing will set these clouds in one of two "preferred" microphysical regimes with very different susceptibility to aerosol.
The impact of temperature changes on summer time ozone and its precursors in the Eastern Mediterranean

Changes in temperature due to variability in meteorology and climate change are expected to significantly impact atmospheric composition. The Mediterranean is a climate sensitive region and includes megacities like Istanbul and large urban agglomerations such as Athens. The effect of temperature changes on gaseous air pollutant levels and the atmospheric processes that are controlling them in the Eastern Mediterranean are here investigated. The WRF/CMAQ mesoscale modeling system is used, coupled with the MEGAN model for the processing of biogenic volatile organic compound emissions. A set of temperature perturbations (spanning from 1 to 5 K) is applied on a base case simulation corresponding to July 2004. The results indicate that the Eastern Mediterranean basin acts as a reservoir of pollutants and their precursor emissions from large urban agglomerations. During summer, chemistry is a major sink at these urban areas near the surface, and a minor contributor at downwind areas. On average, the atmospheric processes are more effective within the first 1000 m above ground. Temperature increases lead to increases in biogenic emissions by 9±3% K−1. Ozone mixing ratios increase almost linearly with the increases in ambient temperatures by 1±0.1 ppb O3 K−1 for all studied urban and receptor stations except for Istanbul, where a 0.4±0.1 ppb O3 K−1 increase is calculated, which is about half of the domain-averaged increase of 0.9±0.1 ppb O3 K−1. The computed changes in atmospheric processes are also linearly related with temperature changes.
Size-resolved and bulk activation properties of aerosols in the North China Plain

Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (NCCN) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. The observed CCN number concentration (NCCN-obs) are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. The calculated CCN number concentrations (NCCN-calc) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN at each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.
The role of tropical deep convective clouds on temperature, water vapor, and dehydration in the tropical tropopause layer (TTL)

Temperature and water vapor variations due to clouds in the tropical tropopause layer (TTL) are investigated using co-located MLS, CALIPSO, and CloudSat data. Convective cooling occurs only up to the cloud tops, with warming above these heights in the TTL. Water vapor and ozone anomalies above the cloud tops are consistent with the warming being due to downward motion. Thicker clouds are associated with larger anomalies. Environmental water vapor below cloud tops can be either higher or lower than when clouds are absent, depending on the cloud top height. The critical factor determining the sign of this change appears to be the relative humidity. In general cloud-forming processes hydrate the environment below 16 km, where the air after mixing between cloud and the environmental air does not reach saturation, but clouds dehydrate above 16 km, as the larger temperature drop and the high initial relative humidity cause supersaturation to occur. Negative water vapor anomalies above cloud tops compared to clear skies suggest another dehydration mechanism operating above the detected cloud layers.