Items

Advanced search

Dehydration in the tropical tropopause layer estimated from the water vapor match

We apply the match technique, whereby the same air mass is observed more than once and such cases are termed a "match", to study the dehydration process associated with horizontal advection in the tropical tropopause layer (TTL) over the western Pacific. The matches are obtained from profile data taken by the Soundings of Ozone and Water in the Equatorial Region (SOWER) campaign network observations using isentropic trajectories calculated from European Centre for Medium-Range Weather Forecasts (ECMWF) operational analyses. For the matches identified, extensive screening procedures are performed to verify the representativeness of the air parcel and the validity of the isentropic treatment, and to check for possible water injection by deep convection, consistency between the sonde data and analysis field referring to the ozone conservation. Among the matches that passed the screening tests, we identified some cases corresponding to the first quantitative value of dehydration associated with horizontal advection in the TTL. The statistical features of dehydration for the air parcels advected in the lower TTL are derived from the matches. The threshold of nucleation is estimated to be 146 ± 1% (1σ) in relative humidity with respect to ice (RHice), while dehydration seems to continue until RHice reaches about 75 ± 23% (1σ) in the altitude region from 350 to 360 K. The efficiency of dehydration expressed by the relaxation time required for the supersaturated air parcel to approach saturation is empirically determined from the matches. A relaxation time of approximately one hour reproduces the second water vapor observation reasonably well, given the first observed water vapor amount and the history of the saturation mixing ratio during advection in the lower TTL.
Brown carbon: a significant atmospheric absorber of solar radiation?

Several recent observational studies have shown organic carbon aerosols to be a significant source of absorption of solar radiation. The absorbing part of organic aerosols is referred to as "brown" carbon (BrC). Using a global chemical transport model and a radiative transfer model, we estimate for the first time the enhanced absorption of solar radiation due to BrC in a global model. The simulated wavelength dependence of aerosol absorption, as measured by the absorption Ångström exponent (AAE), increases from 0.9 for non-absorbing organic carbon to 1.2 (1.0) for strongly (moderately) absorbing BrC. The calculated AAE for the strongly absorbing BrC agrees with AERONET spectral observations at 440–870 nm over most regions but overpredicts for the biomass burning-dominated South America and southern Africa, in which the inclusion of moderately absorbing BrC has better agreement. The resulting aerosol absorption optical depth increases by 18% (3%) at 550 nm and 56% (38%) at 380 nm for strongly (moderately) absorbing BrC. The global simulations suggest that the strongly absorbing BrC contributes up to +0.25 W m−2 or 19% of the absorption by anthropogenic aerosols, while 72% is attributed to black carbon, and 9% is due to sulfate and non-absorbing organic aerosols coated on black carbon. Like black carbon, the absorption of BrC (moderately to strongly) inserts a warming effect at the top of the atmosphere (TOA) (0.04 to 0.11 W m−2), while the effect at the surface is a reduction (−0.06 to −0.14 W m−2). Inclusion of the strongly absorption of BrC in our model causes the direct radiative forcing (global mean) of organic carbon aerosols at the TOA to change from cooling (−0.08 W m−2) to warming (+0.025 W m−2). Over source regions and above clouds, the absorption of BrC is higher and thus can play an important role in photochemistry and the hydrologic cycle.
Observations of gas- and aerosol-phase organic nitrates at BEACHON-RoMBAS 2011

At the Rocky Mountain Biogenic Aerosol Study (BEACHON-RoMBAS) field campaign in the Colorado front range, July–August 2011, measurements of gas- and aerosol-phase organic nitrates enabled a study of the role of NOx (NOx = NO + NO2) in oxidation of forest-emitted volatile organic compounds (VOCs) and subsequent aerosol formation. Substantial formation of peroxy- and alkyl-nitrates is observed every morning, with an apparent 2.9% yield of alkyl nitrates from daytime RO2 + NO reactions. Aerosol-phase organic nitrates, however, peak in concentration during the night, with concentrations up to 140 ppt as measured by both optical spectroscopic and mass spectrometric instruments. The diurnal cycle in aerosol fraction of organic nitrates shows an equilibrium-like response to the diurnal temperature cycle, suggesting some reversible absorptive partitioning, but the full dynamic range cannot be reproduced by thermodynamic repartitioning alone. Nighttime aerosol organic nitrate is observed to be positively correlated with [NO2] × [O3] but not with [O3]. These observations support the role of nighttime NO3-initiated oxidation of monoterpenes as a significant source of nighttime aerosol. Nighttime production of organic nitrates is comparable in magnitude to daytime photochemical production at this site, which we postulate to be representative of the Colorado front range forests.
Inverting for volcanic SO2 flux at high temporal resolution using spaceborne plume imagery and chemistry-transport modelling: the 2010 Eyjafjallajökull eruption case study

Depending on the magnitude of their eruptions, volcanoes impact the atmosphere at various temporal and spatial scales. The volcanic source remains a major unknown to rigorously assess these impacts. At the scale of an eruption, the limited knowledge of source parameters, including time variations of erupted mass flux and emission profile, currently represents the greatest issue that limits the reliability of volcanic cloud forecasts. Today, a growing number of satellite and remote sensing observations of distant plumes are becoming available, bringing indirect information on these source terms. Here, we develop an inverse modelling approach combining satellite observations of the volcanic plume with an Eulerian regional chemistry-transport model (CHIMERE) to characterise the volcanic SO2 emissions during an eruptive crisis. The May 2010 eruption of Eyjafjallajökull is a perfect case study to apply this method as the volcano emitted substantial amounts of SO2 during more than a month. We take advantage of the SO2 column amounts provided by a vast set of IASI (Infrared Atmospheric Sounding Interferometer) satellite images to reconstruct retrospectively the time series of the mid-tropospheric SO2 flux emitted by the volcano with a temporal resolution of ~2 h, spanning the period from 1 to 12 May 2010. We show that no a priori knowledge on the SO2 flux is required for this reconstruction. The initialisation of chemistry-transport modelling with this reconstructed source allows for reliable simulation of the evolution of the long-lived tropospheric SO2 cloud over thousands of kilometres. Heterogeneities within the plume, which mainly result from the temporal variability of the emissions, are correctly tracked over a timescale of a week. The robustness of our approach is also demonstrated by the broad similarities between the SO2 flux history determined by this study and the ash discharge behaviour estimated by other means during the phases of high explosive activity at Eyjafjallajökull in May 2010. Finally, we show how a sequential IASI data assimilation allows for a substantial improvement in the forecasts of the location and concentration of the plume compared to an approach assuming constant flux at the source. As the SO2 flux is an important indicator of the volcanic activity, this approach is also of interest to monitor poorly instrumented volcanoes from space.
Evaluating the degree of oxygenation of organic aerosol during foggy and hazy days in Hong Kong using high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS)

The chemical characteristics of organic aerosol (OA) are still poorly constrained. Here we present observation results of the degree of oxygenation of OA based on high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) measurements made at a coastal site in Hong Kong from late April to the end of May in 2011. Two foggy periods and one hazy period were chosen for detailed analysis to compare the changes in the degree of oxygenation of OA due to different processes. Using HR-ToF-AMS measured inorganic species as input, the Extended Aerosol Inorganic Model (E-AIM) predicted a fine-particle liquid water content (LWCfp) up to 85 μg m−3 during the foggy days. Particle concentration as measured by HR-ToF-AMS was up to 60 μg m−3 during the hazy days and up to 30 μg m−3 during the foggy days. The degree of oxygenation of OA, as indicated by several parameters including the fraction of m/z 44 in organic mass spectra (f44), the elemental ratio of oxygen to carbon (O : C), and the carbon oxidation state (OSc), was evaluated against the odd oxygen (Ox) concentration, LWCfp, ionic strength (IS), and in situ pH (pHis). Observations suggest that the high concentration of OA (on average 11 μg m−3) and the high degree of oxygenation (f44 = 0.15, O : C = 0.51, and OSc = −0.31) during the hazy period were mainly due to gas-phase oxidation. During the foggy periods with low photochemical activities, the degree of oxygenation of OA was almost as high as that on the hazy days, and significantly higher than that during non-foggy/non-hazy days. However, the OA evolved quite differently in the two foggy periods. The first foggy period in late April saw a larger LWCfp and a lower Ox concentration and the OA were made up of ~ 20 % semi-volatile oxygenated organic aerosol (SVOOA) as resolved by positive matrix factorization (PMF). In the second foggy period in mid-May, higher Ox concentration and lower LWCfp were observed, and the OA were found to contain > 50 % low-volatility oxygenated organic aerosols (LVOOA). An examination of the particle characteristics (pHis, IS, and LWCfp) suggests that partitioning may have been the dominating process through which oxygenated species were incorporated into the particle phase during the first foggy period, while oxidation in the aqueous phase dominated over gas-phase processes during the second foggy period.
Burning of olive tree branches: a major organic aerosol source in the Mediterranean

Aerosol produced during the burning of olive tree branches was characterized with both direct source sampling (using a mobile smog chamber) and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8–10% black carbon (BC), 5% potassium, 3–4% sulfate, 2–3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA) consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O : C) ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034–0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O : C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs) such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF) was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%), HOA (hydrocarbon-like organic aerosol, 11.3%) and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.9 g kg−1. Assuming that half of the olive tree branches pruned is burned in Greece, 2300 ± 600 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in Mediterranean countries.
Global CO2 fluxes estimated from GOSAT retrievals of total column CO2

We present one of the first estimates of the global distribution of CO2 surface fluxes using total column CO2 measurements retrieved by the SRON-KIT RemoTeC algorithm from the Greenhouse gases Observing SATellite (GOSAT). We derive optimized fluxes from June 2009 to December 2010. We estimate fluxes from surface CO2 measurements to use as baselines for comparing GOSAT data-derived fluxes. Assimilating only GOSAT data, we can reproduce the observed CO2 time series at surface and TCCON sites in the tropics and the northern extra-tropics. In contrast, in the southern extra-tropics GOSAT XCO2 leads to enhanced seasonal cycle amplitudes compared to independent measurements, and we identify it as the result of a land–sea bias in our GOSAT XCO2 retrievals. A bias correction in the form of a global offset between GOSAT land and sea pixels in a joint inversion of satellite and surface measurements of CO2 yields plausible global flux estimates which are more tightly constrained than in an inversion using surface CO2 data alone. We show that assimilating the bias-corrected GOSAT data on top of surface CO2 data (a) reduces the estimated global land sink of CO2, and (b) shifts the terrestrial net uptake of carbon from the tropics to the extra-tropics. It is concluded that while GOSAT total column CO2 provide useful constraints for source–sink inversions, small spatiotemporal biases – beyond what can be detected using current validation techniques – have serious consequences for optimized fluxes, even aggregated over continental scales.
Gravitational separation in the stratosphere – a new indicator of atmospheric circulation

As a basic understanding of the dynamics of the atmospheric circulation, it has been believed that gravitational separation of atmospheric components is observable only in the atmosphere above the turbopause. However, we found, from our high-precision measurements of not only the isotopic ratios of N2, O2 and Ar but also the mole fraction of Ar, that gravitational separation occurs even in the stratosphere below the turbopause; their observed vertical profiles are in good agreement with those expected theoretically from molecular mass differences. The O2/N2 ratio observed in the middle stratosphere, corrected for gravitational separation, showed the same mean air age as estimated from the CO2 mole fraction. Simulations with a 2-dimensional model of the middle atmosphere indicated that a relationship between gravitational separation and the age of air in the stratosphere would be significantly affected if the Brewer–Dobson circulation was enhanced due to global warming. Therefore, gravitational separation is usable as a new indicator of changes in the atmospheric circulation in the stratosphere.
Light-absorbing carbon in Europe – measurement and modelling, with a focus on residential wood combustion emissions

The atmospheric concentration of elemental carbon (EC) in Europe during the six-year period 2005–2010 has been simulated with the EMEP MSC-W model. The model bias compared to EC measurements was less than 20% for most of the examined sites. The model results suggest that fossil fuel combustion is the dominant source of EC in most of Europe but that there are important contributions also from residential wood burning during the cold seasons and, during certain episodes, also from open biomass burning (wildfires and agricultural fires). The modelled contributions from open biomass fires to ground level concentrations of EC were small at the sites included in the present study, <3% of the long-term average of EC in PM10. The modelling of this EC source is subject to many uncertainties, and it was likely underestimated for some episodes. EC measurements and modelled EC were also compared to optical measurements of black carbon (BC). The relationships between EC and BC (as given by mass absorption cross section, MAC, values) differed widely between the sites, and the correlation between observed EC and BC is sometimes poor, making it difficult to compare results using the two techniques and limiting the comparability of BC measurements to model EC results. A new bottom-up emission inventory for carbonaceous aerosol from residential wood combustion has been applied. For some countries the new inventory has substantially different EC emissions compared to earlier estimates. For northern Europe the most significant changes are much lower emissions in Norway and higher emissions in neighbouring Sweden and Finland. For Norway and Sweden, comparisons to source-apportionment data from winter campaigns indicate that the new inventory may improve model-calculated EC from wood burning. Finally, three different model setups were tested with variable atmospheric lifetimes of EC in order to evaluate the model sensitivity to the assumptions regarding hygroscopicity and atmospheric ageing of EC. The standard ageing scheme leads to a rapid transformation of the emitted hydrophobic EC to hygroscopic particles, and generates similar results when assuming that all EC is aged at the point of emission. Assuming hydrophobic emissions and no ageing leads to higher EC concentrations. For the more remote sites, the observed EC concentration was in between the modelled EC using standard ageing and the scenario treating EC as hydrophobic. This could indicate too-rapid EC ageing in the model in relatively clean parts of the atmosphere.
Transport of aerosols into the UTLS and their impact on the Asian monsoon region as seen in a global model simulation

An eight-member ensemble of ECHAM5-HAMMOZ simulations for a boreal summer season is analysed to study the transport of aerosols in the upper troposphere and lower stratosphere (UTLS) during the Asian summer monsoon (ASM). The simulations show persistent maxima in black carbon, organic carbon, sulfate, and mineral dust aerosols within the anticyclone in the UTLS throughout the ASM (period from July to September), when convective activity over the Indian subcontinent is highest, indicating that boundary layer aerosol pollution is the source of this UTLS aerosol layer. The simulations identify deep convection and the associated heat-driven circulation over the southern flanks of the Himalayas as the dominant transport pathway of aerosols and water vapour into the tropical tropopause layer (TTL). Comparison of model simulations with and without aerosols indicates that anthropogenic aerosols are central to the formation of this transport pathway. Aerosols act to increase cloud ice, water vapour, and temperature in the model UTLS. Evidence of ASM transport of aerosols into the stratosphere is also found, in agreement with aerosol extinction measurements from the Halogen Occultation Experiment (HALOE) and Stratospheric Aerosol and Gas Experiment (SAGE) II. As suggested by the observations, aerosols are transported into the Southern Hemisphere around the tropical tropopause by large-scale mixing processes. Aerosol-induced circulation changes also include a weakening of the main branch of the Hadley circulation and a reduction of monsoon precipitation over India.