Items

Advanced search

Climatology of stratocumulus cloud morphologies: microphysical properties and radiative effects

An artificial neural network cloud classification scheme is combined with A-train observations to characterize the physical properties and radiative effects of marine low clouds based on their morphology and type of mesoscale cellular convection (MCC) on a global scale. The cloud morphological categories are (i) organized closed MCC, (ii) organized open MCC and (iii) cellular but disorganized MCC. Global distributions of the frequency of occurrence of MCC types show clear regional signatures. Organized closed and open MCCs are most frequently found in subtropical regions and in midlatitude storm tracks of both hemispheres. Cellular but disorganized MCC are the predominant type of marine low clouds in regions with warmer sea surface temperature such as in the tropics and trade wind zones. All MCC types exhibit a pronounced seasonal cycle. The physical properties of MCCs such as cloud fraction, radar reflectivity, drizzle rates and cloud top heights as well as the radiative effects of MCCs are found highly variable and a function of the type of MCC. On a global scale, the cloud fraction is largest for closed MCC with mean cloud fractions of about 90%, whereas cloud fractions of open and cellular but disorganized MCC are only about 51% and 40%, respectively. Probability density functions (PDFs) of cloud fractions are heavily skewed and exhibit modest regional variability. PDFs of column maximum radar reflectivities and inferred cloud base drizzle rates indicate fundamental differences in the cloud and precipitation characteristics of different MCC types. Similarly, the radiative effects of MCCs differ substantially from each other in terms of shortwave reflectance and transmissivity. These differences highlight the importance of low-cloud morphologies and their associated cloudiness on the shortwave cloud forcing.
African dust outbreaks over the western Mediterranean Basin: 11-year characterization of atmospheric circulation patterns and dust source areas

The occurrence of African dust outbreaks over different areas of the western Mediterranean Basin were identified on an 11-year period (2001–2011). The main atmospheric circulation patterns causing the transport of African air masses were characterized by means of an objective classification methodology of atmospheric variable fields. Next, the potential source areas of mineral dust, associated to each circulation pattern were identified by trajectory statistical methods. Finally, an impact index was calculated to estimate the incidence of the African dust outbreaks produced during each circulation pattern, in the areas of study. Four circulation types were obtained (I–IV) and three main potential source areas of African dust were identified (Western Sahara and Morocco; Algeria; northeastern Algeria and Tunisia). The circulation pattern I (24% of the total number of episodic days) produced the transport of dust mainly in summer from Western Sahara, southern Morocco and Tunisia. The circulation pattern IV (33%) brings dust mainly from areas of northern and southern Algeria in summer and autumn, respectively. The circulation pattern II (31%) favored the transport of dust predominantly from northern Algeria, both in spring and summer. Finally, the circulation type III was the less frequently observed (12%). It occurred mainly in spring and with less intensity in winter, carrying dust from Western Sahara and southern Morocco. Our findings point out that the most intense episodes over the western Mediterranean Basin were produced in the summer period by the circulation type I (over the western side of the Iberian Peninsula) and the circulation type IV (over the central and eastern sides of the Iberian Peninsula and the Balearic Islands).
Impacts of the East Asian summer monsoon on interannual variations of summertime surface-layer ozone concentrations over China

We apply a global three-dimensional Goddard Earth Observing System (GEOS) chemical transport model (GEOS-Chem) driven by the NASA/GEOS-4 assimilated meteorological fields to quantify the impacts of the East Asian summer monsoon (EASM) on interannual variations of June-July-August (JJA) surface-layer O3 concentrations over China. With anthropogenic emissions fixed at year 2005 levels, the model simulation for years 1986–2006 shows that the changes in meteorological parameters alone lead to interannual variations in JJA surface-layer O3 concentrations by 2–5% over central eastern China, 1–3% in northwestern China, and 5–10% over the Tibetan Plateau as well as the border and coastal areas of southern China, as the interannual variations are relative to the average O3 concentrations over the 21 yr period. Over the years 1986–2006, the O3 concentration averaged over all of China is found to correlate positively with the EASM index with a large correlation coefficient of +0.75, indicating that JJA O3 concentrations are lower (or higher) in weaker (or stronger) EASM years. Relative to JJA surface-layer O3 concentrations in the strongest EASM years (1990, 1994, 1997, 2002, and 2006), O3 levels in the weakest EASM years (1988, 1989, 1996, 1998, and 2003) are lower over almost all of China with a national mean lower O3 concentration by 2.0 ppbv (parts per billion by volume; or 4%). Regionally, the largest percentage differences in O3 concentration between the weakest and strongest EASM years are found to exceed 6% in northeastern China, southwestern China, and over the Tibetan Plateau. Sensitivity studies show that the difference in transboundary transport of O3 is the most dominant factor that leads to lower-O3 concentrations in the weakest EASM years than in the strongest EASM years, which, together with the enhanced vertical convections in the weakest EASM years, explain about 80% of the differences in surface-layer O3 concentrations between the weakest and strongest EASM years. We also find that the impacts the EASM strength on JJA surface-layer O3 can be particularly strong (comparable in magnitude to the impacts on O3 by changes in anthropogenic emissions over years 1986–2006) for certain years. The largest increases in O3 by anthropogenic emissions are simulated over southeastern China, whereas the largest impacts of the EASM on O3 are found over central and western China.
The climate impact of ship NOx emissions: an improved estimate accounting for plume chemistry

Nitrogen oxide (NOx) emissions from maritime shipping produce ozone (O3) and hydroxyl radicals (OH), which in turn destroy methane (CH4). The balance between this warming (due to O3) and cooling (due to CH4) determines the net effect of ship NOx on climate. Previous estimates of the chemical impact and radiative forcing (RF) of ship NOx have generally assumed that plumes of ship exhaust are instantly diluted into model grid cells spanning hundreds of kilometers, even though this is known to produce biased results. Here we improve the parametric representation of exhaust-gas chemistry developed in the GEOS-Chem chemical transport model (CTM) to provide the first estimate of RF from shipping that accounts for sub-grid-scale ship plume chemistry. The CTM now calculates O3 production and CH4 loss both within and outside the exhaust plumes and also accounts for the effect of wind speed. With the improved modeling of plumes, ship NOx perturbations are smaller than suggested by the ensemble of past global modeling studies, but if we assume instant dilution of ship NOx on the grid scale, the CTM reproduces previous model results. Our best estimates of the RF components from increasing ship NOx emissions by 1 Tg(N) yr−1 are smaller than that given in the past literature: + 3.4 ± 0.85 mW m−2 (1σ confidence interval) from the short-lived ozone increase, −5.7 ± 1.3 mW m−2 from the CH4 decrease, and −1.7 ± 0.7 mW m−2 from the long-lived O3 decrease that accompanies the CH4 change. The resulting net RF is −4.0 ± 2.0 mW m−2 for emissions of 1 Tg(N) yr−1. Due to non-linearity in O3 production as a function of background NOx, RF from large changes in ship NOx emissions, such as the increase since preindustrial times, is about 20% larger than this RF value for small marginal emission changes. Using sensitivity tests in one CTM, we quantify sources of uncertainty in the RF components and causes of the ±30% spread in past model results; the main source of uncertainty is the composition of the background atmosphere in the CTM, which is driven by model formulation (±10 to 20%) and the plausible range of anthropogenic emissions (±10%).
Effects of dust aerosols on tropospheric chemistry during a typical pre-monsoon season dust storm in northern India

This study examines the effect of a typical pre-monsoon season dust storm on tropospheric chemistry through a case study in northern India. Dust can alter photolysis rates by scattering and absorbing solar radiation and provide surface area for heterogeneous reactions. We use the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to simulate the dust storm that occurred during 17–22 April 2010 and investigate the contribution of different processes on mixing ratios of several key trace gases including ozone, nitrogen oxides, hydrogen oxides, methanol, acetic acid and formaldehyde. We revised the Fast Troposphere Ultraviolet Visible (F-TUV) photolysis scheme to include effects of dust aerosols on photolysis rates in a manner consistent with the calculations of aerosol optical properties for feedback to the meteorology radiation schemes. In addition, we added 12 heterogeneous reactions on the dust surface, for which 6 reactions have relative-humidity-dependent reactive uptake coefficients (γ). The inclusion of these processes in WRF-Chem is found to reduce the difference between observed and modeled O3 from 16 ± 9 to 2 ± 8 ppbv and that in NOy from 2129 ± 1425 to 372 ± 1225 pptv compared to measurements at the high-altitude site Nainital in the central Himalayas, and reduce biases by up to 30% in tropospheric column NO2 compared to OMI retrievals. The simulated dust storm acted as a sink for all the trace gases examined here and significantly perturbed their spatial and vertical distributions. The reductions in these gases are estimated as 5–100%, and more than 80% of this reduction was due to heterogeneous chemistry. The RH dependence of γ is also found to have substantial impact on the distribution of trace gases, with changes of up to 20–25% in O3 and HO2, 50% in H2O2 and 100% in HNO3. A set of sensitivity analyses revealed that dust aging could change H2O2 and CH3COOH levels by up to 50% but has a relatively small impact on other gases.
Deriving an atmospheric budget of total organic bromine using airborne in situ measurements from the western Pacific area during SHIVA

During the recent SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere) project an extensive data set of all halogen species relevant for the atmospheric budget of total organic bromine was collected in the western Pacific region using the Falcon aircraft operated by the German Aerospace agency DLR (Deutsches Zentrum für Luft- und Raumfahrt) covering a vertical range from the planetary boundary layer up to the ceiling altitude of the aircraft of 13 km. In total, more than 700 measurements were performed with the newly developed fully automated in situ instrument GHOST-MS (Gas chromatograph for the Observation of Tracers – coupled with a Mass Spectrometer) by the Goethe University of Frankfurt (GUF) and with the onboard whole-air sampler WASP with subsequent ground-based state-of-the-art GC / MS analysis by the University of East Anglia (UEA). Both instruments yield good agreement for all major (CHBr3 and CH2Br2) and minor (CH2BrCl, CHBrCl2 and CHBr2Cl) VSLS (very short-lived substances), at least at the level of their 2σ measurement uncertainties. In contrast to the suggestion that the western Pacific could be a region of strongly increased atmospheric VSLS abundance (Pyle et al., 2011), we found only in the upper troposphere a slightly enhanced amount of total organic bromine from VSLS relative to the levels reported in Montzka and Reimann et al. (2011) for other tropical regions. From the SHIVA observations in the upper troposphere, a budget for total organic bromine, including four halons (H-1301, H-1211, H-1202, H-2402), CH3Br and the VSLS, is derived for the level of zero radiative heating (LZRH), the input region for the tropical tropopause layer (TTL) and thus also for the stratosphere. With the exception of the two minor VSLS CHBrCl2 and CHBr2Cl, excellent agreement with the values reported in Montzka and Reimann et al. (2011) is found, while being slightly higher than previous studies from our group based on balloon-borne measurements.
Influence of heterogeneous freezing on the microphysical and radiative properties of orographic cirrus clouds

The influence of heterogeneous freezing on the microphysical and optical properties of orographic cirrus clouds has been simulated with the large eddy simulation model EULAG. Idealised simulations with different concentrations of ice nuclei (IN) in a dynamically dominated regime with high vertical velocities have been performed. Furthermore the temperature at cloud formation as well as the critical supersaturation for initiation of heterogenous freezing have been varied. The shortwave, longwave and net cloud forcing has been calculated under the assumption that the clouds form between 06:00 and 12:00 local time (LT) or between 12:00 and 18:00 LT. In general it can be seen that the onset of homogeneous freezing is shifted in time depending on the IN concentration, as part of the available water vapour is depleted before the critical threshold for homogeneous freezing is reached. Although the high vertical velocities in an orographic gravity wave lead to a strong adiabatic cooling followed by high ice supersaturations, even a small number concentration of IN of the order of 5 L−1 is able to strongly decrease the simulated ice crystal number burden (ICNB), ice water path (IWP) and optical depth of the cloud. In general, the ICNB, IWP and optical depth strongly decrease when the IN concentrations are increased from 0 to 50 L−1. The absolute values of the shortwave, longwave and net cloud forcing are also reduced with increasing IN concentrations. A cloud will produce a net warming or cooling depending on the IN concentration, the temperature and the time of day when the cloud forms. The clouds that form between 06:00 and 12:00 LT are mainly cooling, whereas the clouds with the same microphysical properties can lead to a warming when they form between 12:00 and 18:00 LT. In order to predict the radiative forcing of cirrus clouds it is therefore necessary to take the correct dynamical and thermodynamical processes as well as the possible existence and freezing threshold of heterogeneous IN into account, not only for low vertical velocities but also for dynamically dominated regimes like orographic cirrus.
Atmospheric photochemistry of aromatic hydrocarbons: OH budgets during SAPHIR chamber experiments

Current photochemical models developed to simulate the atmospheric degradation of aromatic hydrocarbons tend to underestimate OH radical concentrations. In order to analyse OH budgets, we performed experiments with benzene, toluene, p-xylene and 1,3,5-trimethylbenzene in the atmosphere simulation chamber SAPHIR. Experiments were conducted under low-NO conditions (typically 0.1–0.2 ppb) and high-NO conditions (typically 7–8 ppb), and starting concentrations of 6–250 ppb of aromatics, dependent on OH rate constants. For the OH budget analysis a steady-state approach was applied in which OH production and destruction rates (POH and DOH) have to be equal. The POH were determined from measurements of HO2, NO, HONO, and O3 concentrations, considering OH formation by photolysis and recycling from HO2. The DOH were calculated from measurements of the OH concentrations and total OH reactivities. The OH budgets were determined from DOH/POH ratios. The accuracy and reproducibility of the approach were assessed in several experiments using CO as a reference compound where an average ratio DOH/POH = 1.13 ± 0.19 was obtained. In experiments with aromatics, these ratios ranged within 1.1–1.6 under low-NO conditions and 0.9–1.2 under high-NO conditions. The results indicate that OH budgets during photo-oxidation experiments with aromatics are balanced within experimental accuracies. Inclusion of a further, recently proposed OH production via HO2 + RO2 reactions led to improvements under low-NO conditions but the differences were small and insignificant within the experimental errors.
Impacts of climate and emission changes on nitrogen deposition in Europe: a multi-model study

The impact of climate and emissions changes on the deposition of reactive nitrogen (Nr) over Europe was studied using four offline regional chemistry transport models (CTMs) driven by the same global projection of future climate over the period 2000–2050. Anthropogenic emissions for the years 2005 and 2050 were used for simulations of both present and future periods in order to isolate the impact of climate change, hemispheric boundary conditions and emissions, and to assess the robustness of the results across the different models. The results from these four CTMs clearly show that the main driver of future N-deposition changes is the specified emission change. Under the specified emission scenario for 2050, emissions of oxidised nitrogen were reduced substantially, whereas emissions of NH3 increase to some extent, and these changes are largely reflected in the modelled concentrations and depositions. The lack of sulfur and oxidised nitrogen in the future atmosphere results in a much larger fraction of NHx being present in the form of gaseous ammonia. Predictions for wet and total deposition were broadly consistent, although the three fine-scale models resolve European emission areas and changes better than the hemispheric-scale model. The biggest difference in the models is for predictions of individual N compounds. One model (EMEP) was used to explore changes in critical loads, also in conjunction with speculative climate-induced increases in NH3 emissions. These calculations suggest that the area of ecosystems that exceeds critical loads is reduced from 64% for year 2005 emissions levels to 50% for currently estimated 2050 levels. A possible climate-induced increase in NH3 emissions could worsen the situation, with areas exceeded increasing again to 57% (for a 30% NH3 emission increase).
New spectral functions of the near-ground albedo derived from aircraft diffraction spectrometer observations

The airborne spectral observations of the upward and downward irradiances are revisited to investigate the dependence of the near-ground albedo as a function of wavelength in the entire solar spectrum for different surfaces (sand, water, snow) and under different conditions (clear or cloudy sky). The radiative upward and downward fluxes were determined by a diffraction spectrometer flown on a research aircraft that was performing multiple flight paths near the ground. The results obtained show that the near-ground albedo does not generally increase with increasing wavelengths for all kinds of surfaces as is widely believed today. Particularly, in the case of water surfaces it was found that the albedo in the ultraviolet region is more or less independent of the wavelength on a long-term basis. Interestingly, in the visible and near-infrared spectra the water albedo obeys an almost constant power-law relationship with wavelength. In the case of sand surfaces it was found that the sand albedo is a quadratic function of wavelength, which becomes more accurate if the ultraviolet wavelengths are neglected. Finally, it was found that the spectral dependence of snow albedo behaves similarly to that of water, i.e. both decrease from the ultraviolet to the near-infrared wavelengths by 20–50%, despite the fact that their values differ by one order of magnitude (water albedo being lower). In addition, the snow albedo vs. ultraviolet wavelength is almost constant, while in the visible near-infrared spectrum the best simulation is achieved by a second-order polynomial, as in the case of sand, but with opposite slopes.