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Cloud optical thickness and liquid water path – does the k coefficient vary with droplet concentration?

Cloud radiative transfer calculations in general circulation models involve a link between cloud microphysical and optical properties. Indeed, the liquid water content expresses as a function of the mean volume droplet radius, while the light extinction is a function of their mean surface radius. There is a small difference between these two parameters because of the droplet spectrum width. This issue has been addressed by introducing an empirical multiplying correction factor to the droplet concentration. Analysis of in situ sampled data, however, revealed that the correction factor decreases when the concentration increases, hence partially mitigating the aerosol indirect effect. Five field experiments are reanalyzed here, in which standard and upgraded versions of the droplet spectrometer were used to document shallow cumulus and stratocumulus topped boundary layers. They suggest that the standard probe noticeably underestimates the correction factor compared to the upgraded versions. The analysis is further refined to demonstrate that the value of the correction factor derived by averaging values calculated locally along the flight path overestimates the value derived from liquid water path and optical thickness of a cloudy column, and that there is no detectable relationship between the correction factor and the droplet concentration. It is also shown that the droplet concentration dilution by entrainment-mixing after CCN activation is significantly stronger in shallow cumuli than in stratocumulus layers. These various effects are finally combined to produce the today best estimate of the correction factor to use in general circulation models.
Seasonal features of ultrafine particle volatility in the coastal Antarctic troposphere

The size distribution and volatility of ultrafine aerosol particles were measured using scanning mobility particle sizer and thermodenuder at Syowa Station during the 46–47 Japanese Antarctic Research Expeditions (2005–2007). The relative abundance of non-volatile particles in a 240 °C scan was approximately 20% during the summer, whereas the abundance of non-volatile particles increased by >90% during the winter–spring. Most ultrafine particles were volatilized at temperature of 150–210 °C. This volatility was consistent well to major aerosol constituents (NH4+, SO42− and CH3SO3−) during the summer. In contrast, major constituents of ultrafine particles were sea-salts (Na+ and Cl−) in winter–spring. Therefore, the seasonal feature of volatility of ultrafine particles at Syowa was associated with seasonal variations of the major aerosol constituents. Although the relative abundance of non-volatile particles was usually higher during the winter–spring, the abundance dropped occasionally to <30%. The lower abundance of non-volatile ultrafine particles during winter–spring corresponded to the lower number concentration of ultrafine particles and transport from the free troposphere over Antarctica.
Snow optical properties at Dome C (Concordia), Antarctica; implications for snow emissions and snow chemistry of reactive nitrogen

Measurements of e-folding depth, nadir reflectivity and stratigraphy of the snowpack around Concordia station (Dome C, 75.10° S, 123.31° E) were undertaken to determine wavelength dependent coefficients (350 nm to 550 nm) for light scattering and absorption and to calculate potential fluxes (depth-integrated production rates) of nitrogen dioxide (NO2) from the snowpack due to nitrate photolysis within the snowpack. The stratigraphy of the top 80 cm of Dome C snowpack generally consists of three main layers:- a surface of soft windpack (not ubiquitous), a hard windpack, and a hoar-like layer beneath the windpack(s). The e-folding depths are ~10 cm for the two windpack layers and ~20 cm for the hoar-like layer for solar radiation at a wavelength of 400 nm; about a factor 2–4 larger than previous model estimates for South Pole. The absorption cross-section due to impurities in each snowpack layer are consistent with a combination of absorption due to black carbon and HULIS (HUmic LIke Substances), with amounts of 1–2 ng g−1 of black carbon for the surface snow layers. Depth-integrated photochemical production rates of NO2 in the Dome C snowpack were calculated as 5.3 × 1012 molecules m−2 s−1, 2.3 × 1012 molecules m−2 s−1 and 8 × 1011 molecules m−2 s−1 for clear skies and solar zenith angles of 60°, 70° and 80° respectively using the TUV-snow radiative-transfer model. Depending upon the snowpack stratigraphy, a minimum of 85% of the NO2 may originate from the top 20 cm of the Dome C snowpack. It is found that on a multi-annual time-scale photolysis can remove up to 80% of nitrate from surface snow, confirming independent isotopic evidence that photolysis is an important driver of nitrate loss occurring in the EAIS (East Antarctic Ice Sheet) snowpack. However, the model cannot completely account for the total observed nitrate loss of 90–95 % or the shape of the observed nitrate concentration depth profile. A more complete model will need to include also physical processes such as evaporation, re-deposition or diffusion between the quasi-liquid layer on snow grains and firn air to account for the discrepancies.
Characteristics of water-vapour inversions observed over the Arctic by Atmospheric Infrared Sounder (AIRS) and radiosondes

An accurate characterization of the vertical structure of the Arctic atmosphere is useful in climate change and attribution studies as well as for the climate modelling community to improve projections of future climate over this highly sensitive region. Here, we investigate one of the dominant features of the vertical structure of the Arctic atmosphere, i.e. water-vapour inversions, using eight years of Atmospheric Infrared Sounder data (2002–2010) and radiosounding profiles released from the two Arctic locations (North Slope of Alaska at Barrow and during SHEBA). We quantify the characteristics of clear-sky water vapour inversions in terms of their frequency of occurrence, strength and height covering the entire Arctic for the first time. We found that the frequency of occurrence of water-vapour inversions is highest during winter and lowest during summer. The inversion strength is, however, higher during summer. The observed peaks in the median inversion-layer heights are higher during the winter half of the year, at around 850 hPa over most of the Arctic Ocean, Siberia and the Canadian Archipelago, while being around 925 hPa during most of the summer half of the year over the Arctic Ocean. The radiosounding profiles agree with the frequency, location and strength of water-vapour inversions in the Pacific sector of the Arctic. In addition, the radiosoundings indicate that multiple inversions are the norm with relatively few cases without inversions. The amount of precipitable water within the water-vapour inversion structures is estimated and we find a distinct, two-mode contribution to the total column precipitable water. These results suggest that water-vapour inversions are a significant source to the column thermodynamics, especially during the colder winter and spring seasons. We argue that these inversions are a robust metric to test the reproducibility of thermodynamics within climate models. An accurate statistical representation of water-vapour inversions in models would mean that the large-scale coupling of moisture transport, precipitation, temperature and water-vapour vertical structure and radiation are essentially captured well in such models.
Photochemical production of ozone in Beijing during the 2008 Olympic Games

As a part of the CAREBeijing-2008 campaign, observations of O3, oxides of nitrogen (NOx and NOy), CO, and hydrocarbons (NMHCs) were carried out at the air quality observatory of the Peking University in Beijing, China during August 2008, including the period of the 29th Summer Olympic Games. The measurements were compared with those of the CAREBeijing-2006 campaign to evaluate the effectiveness of the air pollution control measures, which were conducted for improving the air quality in Beijing during the Olympics. The results indicate that significant reduction in the emissions of primary air pollutants had been achieved; the monthly averaged mixing ratios of NOx, NOy, CO, and NMHCs decreased by 42.2, 56.5, 27.8, and 49.7 %, respectively. In contrast to the primary pollutants, the averaged mixing ratio of O3 increased by 42.2 %. Nevertheless, it was revealed that the ambient levels of total oxidant (Ox = O3+NO2+1.5 NOz) and NOz were reduced by 21.3 and 77.4 %, respectively. The contradictions between O3 and Ox were further examined in two case studies. Ozone production rates of 30–70 ppbv h−1 and OPEx of ~8 mole mole−1 were observed on a clear-sky day in spite of the reduced levels of precursors. In that case, it was found that the mixing ratio of O3 increased with the increasing NO2/NO ratio, whereas the NOz mixing ratio leveled off when NO2/NO>8. Consequently, the ratio of O3 to NOz increased to above 10, indicating the shift from VOC-sensitive regime to NOx-sensitive regime. However, in the other case, it was found that the O3 production was inhibited significantly due to substantial reduction in the NMHCs. According to the observations, it was suggested that the O3 and/or Ox production rates in Beijing should have been reduced as a result of the reduction in the emissions of precursors during the Olympic period. However, the nighttime O3 levels increased due to a decline in the NO-O3 titration, and the midday O3 peak levels were elevated because of the shift in the photochemical regime and the inhibition of NOz formation.
Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996–2010

China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996–2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %–17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be −16 %–17 %, −43 %–93 %, and −43 %–80 % for China, and −15 %–16 %, −41 %–87 %, and −44 %–92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and the actual FGD removal efficiency are the main contributors to the uncertainties of SO2 emissions. Biofuel combustion related parameters (i.e., technology divisions, fuel use, and emission factor determinants) are the largest source of OC uncertainties, whereas BC emissions are also sensitive to the parameters of coal combustion in the residential and industrial sectors and the coke-making process. Comparing our results with satellite observations, we find that the trends of estimated emissions in both China and India are in good agreement with the trends of aerosol optical depth (AOD) and SO2 retrievals obtained from different satellites.
Zonal asymmetries in middle atmospheric ozone and water vapour derived from Odin satellite data 2001–2010

Stationary wave patterns in middle atmospheric ozone (O3) and water vapour (H2O) are an important factor in the atmospheric circulation, but there is a strong gap in diagnosing and understanding their configuration and origin. Based on Odin satellite data from 2001 to 2010 we investigate the stationary wave patterns in O3 and H2O as indicated by the seasonal long-term means of the zonally asymmetric components O3* = O3-[O3] and H2O* = H2O-[H2O] ([O3], [H2O]: zonal means). At mid- and polar latitudes we find a pronounced wave one pattern in both constituents. In the Northern Hemisphere, the wave patterns increase during autumn, maintain their strength during winter and decay during spring, with maximum amplitudes of about 10–20 % of the zonal mean values. During winter, the wave one in O3* shows a maximum over the North Pacific/Aleutians and a minimum over the North Atlantic/Northern Europe and a double-peak structure with enhanced amplitude in the lower and in the upper stratosphere. The wave one in H2O* extends from the lower stratosphere to the upper mesosphere with a westward shift in phase with increasing height including a jump in phase at upper stratosphere altitudes. In the Southern Hemisphere, similar wave patterns occur mainly during southern spring. By comparing the observed wave patterns in O3* and H2O* with a linear solution of a steady-state transport equation for a zonally asymmetric tracer component we find that these wave patterns are primarily due to zonally asymmetric transport by geostrophically balanced winds, which are derived from observed temperature profiles. In addition temperature-dependent photochemistry contributes substantially to the spatial structure of the wave pattern in O3* . Further influences, e.g., zonal asymmetries in eddy mixing processes, are discussed.
Inversion of long-lived trace gas emissions using combined Eulerian and Lagrangian chemical transport models

We present a method for estimating emissions of long-lived trace gases from a sparse global network of high-frequency observatories, using both a global Eulerian chemical transport model and Lagrangian particle dispersion model. Emissions are derived in a single step after determining sensitivities of the observations to initial conditions, the high-resolution emissions field close to observation points, and larger regions further from the measurements. This method has the several advantages over inversions using one type of model alone, in that: high-resolution simulations can be carried out in limited domains close to the measurement sites, with lower resolution being used further from them; the influence of errors due to aggregation of emissions close to the measurement sites can be minimized; assumptions about boundary conditions to the Lagrangian model do not need to be made, since the entire emissions field is estimated; any combination of appropriate models can be used, with no code modification. Because the sensitivity to the entire emissions field is derived, the estimation can be carried out using traditional statistical methods without the need for multiple steps in the inversion. We demonstrate the utility of this approach by determining global SF6 emissions using measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) between 2007 and 2009. The global total and large-scale patterns of the derived emissions agree well with previous studies, whilst allowing emissions to be determined at higher resolution than has previously been possible, and improving the agreement between the modeled and observed mole fractions at some sites.
Global precipitation response to changing forcings since 1870

Predicting and adapting to changes in the hydrological cycle is one of the major challenges for the 21st century. To better estimate how it will respond to future changes in climate forcings, it is crucial to understand how the hydrological cycle has evolved in the past and why. In our study, we use an atmospheric global climate model with prescribed sea surface temperatures (SSTs) to investigate how, in the period 1870–2005, changing climate forcings have affected the global land temperature and precipitation. We show that between 1870 and 2005, prescribed SSTs (encapsulating other forcings and internal variability) determine the decadal and interannual variabilities of the global land temperature and precipitation, mostly via their influence in the tropics (25° S–25° N). In addition, using simulations with prescribed SSTs and considering the atmospheric response alone, we find that between 1930 and 2005 increasing aerosol emissions have reduced the global land temperature and precipitation by up to 0.4 °C and 30 mm yr−1, respectively, and that between about 1950 and 2005 increasing greenhouse gas concentrations have increased them by up to 0.25 °C and 10 mm yr−1, respectively. Finally, we suggest that between about 1950 and 1970, increasing aerosol emissions had a larger impact on the hydrological cycle than increasing greenhouse gas concentrations.
Ethane, ethyne and carbon monoxide concentrations in the upper troposphere and lower stratosphere from ACE and GEOS-Chem: a comparison study

Near global upper tropospheric concentrations of carbon monoxide (CO), ethane (C2H6) and ethyne (C2H2) from ACE (Atmospheric Chemistry Experiment) Fourier transform spectrometer on board the Canadian satellite SCISAT-1 are presented and compared with the output from the Chemical Transport Model (CTM) GEOS-Chem. The retrievals of ethane and ethyne from ACE have been improved for this paper by using new sets of microwindows compared with those for previous versions of ACE data. With the improved ethyne retrieval we have been able to produce a near global upper tropospheric distribution of C2H2 from space. Carbon monoxide, ethane and ethyne concentrations retrieved using ACE spectra show the expected seasonality linked to variations in the anthropogenic emissions and destruction rates as well as seasonal biomass burning activity. The GEOS-Chem model was run using the dicarbonyl chemistry suite, an extended chemical mechanism in which ethyne is treated explicitly. Seasonal cycles observed from satellite data are well reproduced by the model output, however the simulated CO concentrations are found to be systematically biased low over the Northern Hemisphere. An average negative global mean bias of 12% and 7% of the model relative to the satellite observations has been found for CO and C2H6 respectively and a positive global mean bias of 1% has been found for C2H2. ACE data are compared for validation purposes with MkIV spectrometer data and Global Tropospheric Experiment (GTE) TRACE-A campaign data showing good agreement with all of them.