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A six year satellite-based assessment of the regional variations in aerosol indirect effects

Aerosols act as cloud condensation nuclei (CCN) for cloud water droplets, and changes in aerosol concentrations have significant microphysical impacts on the corresponding cloud properties. Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol and cloud properties are combined with NCEP Reanalysis data for six different regions around the globe between March 2000 and December 2005 to study the effects of different aerosol, cloud, and atmospheric conditions on the aerosol indirect effect (AIE). Emphasis is placed in examining the relative importance of aerosol concentration, type, and atmospheric conditions (mainly vertical motion) to AIE from region to region. Results show that in most regions, AIE has a distinct seasonal cycle, though the cycle varies in significance and period from region to region. In the Arabian Sea (AS), the six-year mean anthropogenic + dust AIE is −0.27 Wm−2 and is greatest during the summer months (<−2.0 Wm−2) during which aerosol concentrations (from both dust and anthropogenic sources) are greatest. Comparing AIE as a function of thin (LWP<20 gm−2) vs. thick (LWP≥20 gm−2) clouds under conditions of large scale ascent or decent at 850 hPa showed that AIE is greatest for thick clouds during periods of upward vertical motion. In the Bay of Bengal, AIE is negligible owing to less favorable atmospheric conditions, a lower concentration of aerosols, and a non-alignment of aerosol and cloud layers. In the eastern North Atlantic, AIE is weakly positive (+0.1 Wm−2) with dust aerosol concentration being much greater than the anthropogenic or sea salt components. However, elevated dust in this region exists above the maritime cloud layers and does not have a hygroscopic coating, which occurs in AS, preventing the dust from acting as CCN and limiting AIE. The Western Atlantic has a large anthropogenic aerosol concentration transported from the eastern United States producing a modest anthropogenic AIE (−0.46 Wm−2). Anthropogenic AIE is also present off the West African coast corresponding to aerosols produced from seasonal biomass burning (both natural and man-made). Interestingly, atmospheric conditions are not particularly favorable for cloud formation compared to the other regions during the times where AIE is observed; however, clouds are generally thin (LWP<20 gm−2) and concentrated very near the surface. Overall, we conclude that vertical motion, aerosol type, and aerosol layer heights do make a significant contribution to AIE and that these factors are often more important than total aerosol concentration alone and that the relative importance of each differs significantly from region to region.
Impacts of aerosol-cloud interactions on past and future changes in tropospheric composition

The development of effective emissions control policies that are beneficial to both climate and air quality requires a detailed understanding of all the feedbacks in the atmospheric composition and climate system. We perform sensitivity studies with a global atmospheric composition-climate model to assess the impact of aerosols on tropospheric chemistry through their modification on clouds, aerosol-cloud interactions (ACI). The model includes coupling between both tropospheric gas-phase and aerosol chemistry and aerosols and liquid-phase clouds. We investigate past impacts from preindustrial (PI) to present day (PD) and future impacts from PD to 2050 (for the moderate IPCC A1B scenario) that embrace a wide spectrum of precursor emission changes and consequential ACI. The aerosol indirect effect (AIE) is estimated to be −2.0 Wm−2 for PD-PI and −0.6 Wm−2 for 2050-PD, at the high end of current estimates. Inclusion of ACI substantially impacts changes in global mean methane lifetime across both time periods, enhancing the past and future increases by 10% and 30%, respectively. In regions where pollution emissions increase, inclusion of ACI leads to 20% enhancements in in-cloud sulfate production and ~10% enhancements in sulfate wet deposition that is displaced away from the immediate source regions. The enhanced in-cloud sulfate formation leads to larger increases in surface sulfate across polluted regions (~10–30%). Nitric acid wet deposition is dampened by 15–20% across the industrialized regions due to ACI allowing additional re-release of reactive nitrogen that contributes to 1–2 ppbv increases in surface ozone in outflow regions. Our model findings indicate that ACI must be considered in studies of methane trends and projections of future changes to particulate matter air quality.
The relationship between aerosol and cloud drop number concentrations in a global aerosol microphysics model

Empirical relationships that link cloud droplet number (CDN) to aerosol number or mass are commonly used to calculate global fields of CDN for climate forcing assessments. In this work we use a sectional global model of sulfate and sea-salt aerosol coupled to a mechanistic aerosol activation scheme to explore the limitations of this approach. We find that a given aerosol number concentration produces a wide range of CDN concentrations due to variations in the shape of the aerosol size distribution. On a global scale, the dependence of CDN on the size distribution results in regional biases in predicted CDN (for a given aerosol number). Empirical relationships between aerosol number and CDN are often derived from regional data but applied to the entire globe. In an analogous process, we derive regional "correlation-relations" between aerosol number and CDN and apply these regional relations to calculations of CDN on the global scale. The global mean percentage error in CDN caused by using regionally derived CDN-aerosol relations is 20 to 26%, which is about half the global mean percentage change in CDN caused by doubling the updraft velocity. However, the error is as much as 25–75% in the Southern Ocean, the Arctic and regions of persistent stratocumulus when an aerosol-CDN correlation relation from the North Atlantic is used. These regions produce much higher CDN concentrations (for a given aerosol number) than predicted by the globally uniform empirical relations. CDN-aerosol number relations from different regions also show very different sensitivity to changing aerosol. The magnitude of the rate of change of CDN with particle number, a measure of the aerosol efficacy, varies by a factor 4. CDN in cloud processed regions of persistent stratocumulus is particularly sensitive to changing aerosol number. It is therefore likely that the indirect effect will be underestimated in these important regions.
36Cl bomb peak: comparison of modeled and measured data

The extensive nuclear bomb testing of the fifties and sixties and the final tests in the seventies caused a strong 36Cl peak that has been observed in ice cores world-wide. The measured 36Cl deposition fluxes in eight ice cores (Dye3, Fiescherhorn, Grenzgletscher, Guliya, Huascarán, North GRIP, Inylchek (Tien Shan) and Berkner Island) were compared with an ECHAM5-HAM general circulation model simulation (1952–1972). We find a good agreement between the measured and the modeled 36Cl fluxes assuming that the bomb test produced global 36Cl input was ~80 kg. The model simulation indicates that the fallout of the bomb test produced 36Cl is largest in the subtropics and mid-latitudes due to the strong stratosphere-troposphere exchange. In Greenland the 36Cl bomb signal is quite large due to the relatively high precipitation rate. In Antarctica the 36Cl bomb peak is small but is visible even in the driest areas. The model suggests that the large bomb tests in the Northern Hemisphere are visible around the globe but the later (end of sixties and early seventies) smaller tests in the Southern Hemisphere are much less visible in the Northern Hemisphere. The question of how rapidly and to what extent the bomb produced 36Cl is mixed between the hemispheres depends on the season of the bomb test. The model results give an estimate of the amplitude of the bomb peak around the globe.
Analysis of atmospheric neutral and charged molecular clusters in boreal forest using pulse-height CPC

We measured the size distribution of atmospheric neutral and charged clusters and particles down to mobility diameter around 1.5 nm by applying pulse-height CPC technique at SMEAR II station in Hyytiälä, southern Finland during spring 2007 and May 2008. The concentration of molecular clusters smaller than 3 nm seems to be highly variable in boreal forest environment, the concentration varied typically between 500–50 000 cm−3. By comparing to concentrations measured with ion spectrometers, we conclude that ion clusters and neutral clusters produced by ion-ion recombination are usually not sufficient to explain all of the observed clusters; the median fraction of recombination products from all neutral clusters was 4.9%. Before and during most new particle formation events the cluster formation rate rose only slightly, or remained close to stable. Nocturnal formation of clusters was also frequently observed.
Surface ozone at the Caucasian site Kislovodsk High Mountain Station and the Swiss Alpine site Jungfraujoch: data analysis and trends (1990–2006)

Long-term ozone measurements of two background mountain sites, namely the Kislovodsk High Mountain Station in Caucasus, Russia (KHMS, 43.70° N, 42.70° E, 2070 m a.s.l.) and the Jungfraujoch in Switzerland (JFJ, 46.55° N, 7.98° E, 3580 m a.s.l.) are compared. Despite of more than 1.5 km altitude difference ozone mixing ratios are comparable at JFJ an KHMS in the beginning of measurements (1990–1993) while the annually averaged levels at JFJ are around 15 ppb higher than the ones at KHMS for the most recent years (1997–2006). The seasonal cycle of the surface ozone mixing ratios is characterized by a double spring-summer maximum at both sites with a spring one being more pronounced for the air masses with the longest contact with the upper free troposphere and stratosphere. Ozone mixing ratio increased at JFJ but decreased at KHMS for the period 1990–2006. Trends are more pronounced for the 1990s (+0.73±0.20 ppb/year at JFJ and −0.91±0.17 ppb/year at KHMS for the period 1991–2001) in comparison with the later years (+0.04±0.21 ppb/year at JFJ and −0.37±0.14 ppb/year at KHMS for the period 1997–2006). Trends show a distinct seasonality, which is different for the different periods. To investigate possible reasons for this remarkable trends difference 3-D trajectories using LAGRANTO trajectory model are used. Effects of horizontal and vertical transport on ozone trends are considered. No substantial systematic changes in the transport patterns were detected which could lead to strong changes in the trend magnitude between 1991–2001 and 1997–2006. The geographical position of the sites relative to the main topographic features and emission sources as well as distance from the coast are interpreted to be among the main reasons for the opposite surface ozone trends. During the 90s the JFJ trend reflects increase of the ozone in the upper free troposphere/lower stratosphere, while KHMS is not sensitive to this change or even showing the opposite tendency. The analysis provided evidence for a stronger influence of processes in the lower troposphere, in particular the dramatic emission decrease in the earlier 1990s in former USSR and emissions regulations in Western Europe on the surface ozone trend at KHMS.
A daytime climatological distribution of high opaque ice cloud classes over the Indian summer monsoon region observed from 25-year AVHRR data

A daytime climatological spatio-temporal distribution of high opaque ice cloud (HOIC) classes over the Indian subcontinent (0–40° N, 60° E–100° E) is presented using 25-year data from the Advanced Very High Resolution Radiometers (AVHRRs) for the summer monsoon months. The HOICs are important for regional radiative balance, precipitation and troposphere-stratosphere exchange. In this study, HOICs are sub-divided into three classes based on their cloud top brightness temperatures (BT). Class I represents very deep convection (BT<220 K). Class II represents deep convection (220 K<=BT<233 K) and Class III background convection (233 K<=BT<253 K). Apart from presenting finest spatial resolution (0.1×0.1 degrees) and long-term climatology of such cloud classes from AVHRRs to date, this study for the first time illustrates on (1) how these three cloud classes are climatologically distributed during monsoon months, and (2) how their distribution changes during active and break monsoon conditions. It is also investigated that how many deep convective clouds reach the tropopause layer during individual monsoon months. It is seen that Class I and Class II clouds dominate the Indian subcontinent during monsoon. The movement of monsoon over continent is very well reflected in these cloud classes. During monsoon breaks strong suppression of convective activity is observed over the Arabian Sea and the western coast of India. On the other hand, the presence of such convective activity is crucial for active monsoon conditions and all-India rainfall. It is found that a significant fraction of HOICs (3–5%) reach the tropopause layer over the Bay of Bengal during June and over the north and northeast India during July and August. Many cases are observed when clouds penetrate the tropopause layer and reach the lower stratosphere. Such cases mostly occur during June compared to the other months.
High temporal resolution VHF radar observations of stratospheric air intrusions in to the upper troposphere during the passage of a mesoscale convective system over Gadanki (13.5° N, 79.2° E)

A high temporal resolution VHF radar experiment, which was carried out to divulge the clear-air structure of a mesoscale convective system (MCS) at fine time scales over Gadanki, is discussed. The VHF radar was continuously operated for four hours with 11 seconds time resolution on 19 June 2006, which facilitated the study of finer details of stratospheric air intrusions into the upper troposphere during the passage of a MCS. Simultaneous GPS sonde and ground based optical rain gauge measurements are also used for the present study along with radar observations. The height-time section of range corrected signal to noise ratio (RSNR) revealed the convective cells reaching as high as 14 km altitude and the signature of the tropopause as a layered structure at around 16.5 km. The important observation from the radar RSNR is the time localized inclined echoes in the height region of 12–16 km region giving evidence for stratospheric air intrusion into the upper troposphere. Further, this observation is confirmed by the height–time section of vertical velocity, which showed the intense downdraughts in the height region of inclined radar echoes. A detailed examination of this down draft revealed an episode of high frequency gravity wave excitation, which is believed to be the consequence of intrusion of stable stratospheric air into the upper troposphere. Thus, the present study brings out for the first time, how the stratospheric intrusions will appear in the radar height-time sections and the consequences of such intrusions in the upper troposphere
Gap filling and noise reduction of unevenly sampled data by means of the Lomb-Scargle periodogram

The Lomb-Scargle periodogram is widely used for the estimation of the power spectral density of unevenly sampled data. A small extension of the algorithm of the Lomb-Scargle periodogram permits the estimation of the phases of the spectral components. The amplitude and phase information is sufficient for the construction of a complex Fourier spectrum. The inverse Fourier transform can be applied to this Fourier spectrum and provides an evenly sampled series (Scargle, 1989). We are testing the proposed reconstruction method by means of artificial time series and real observations of mesospheric ozone, having data gaps and noise. For data gap filling and noise reduction, it is necessary to modify the Fourier spectrum before the inverse Fourier transform is done. The modification can be easily performed by selection of the relevant spectral components which are above a given confidence limit or within a certain frequency range. Examples with time series of lower mesospheric ozone show that the reconstruction method can reproduce steep ozone gradients around sunrise and sunset and superposed planetary wave-like oscillations observed by a ground-based microwave radiometer at Payerne. The importance of gap filling methods for climate change studies is demonstrated by means of long-term series of temperature and water vapor pressure at the Jungfraujoch station where data gaps from another instrument have been inserted before the linear trend is calculated. The results are encouraging but the present reconstruction algorithm is far away from being reliable and robust enough for a serious application.
Flux estimates of isoprene, methanol and acetone from airborne PTR-MS measurements over the tropical rainforest during the GABRIEL 2005 campaign

Tropical forests are a strong source of biogenic volatile organic compounds (BVOCs) to the atmosphere which can potentially impact the atmospheric oxidation capacity. Here we present airborne and ground-based BVOC measurements representative for the long dry season covering a large area of the northern Amazonian rainforest (6–3° N, 50–59° W). The measurements were conducted during the October 2005 GABRIEL (Guyanas Atmosphere-Biosphere exchange and Radicals Intensive Experiment with the Learjet) campaign. The vertical (35 m to 10 km) and diurnal (09:00–16:00) profiles of isoprene, its oxidation products methacrolein and methyl vinyl ketone and methanol and acetone, measured by PTR-MS (Proton Transfer Reaction Mass Spectrometry), have been used to empirically estimate their emission fluxes from the forest canopy on a regional scale. The mixed layer isoprene emission flux, inferred from the airborne measurements above 300 m, is 5.7 mg isoprene m−2 h−1 after compensating for chemistry and ~6.9 mg isoprene m−2 h−1 taking detrainment into account. This surface flux is in general agreement with previous tropical forest studies. Inferred methanol and acetone emission fluxes are 0.5 mg methanol m−2 h−1 and 0.35 mg acetone m−2 h−1, respectively. The BVOC measurements were compared with fluxes and mixing ratios simulated with a single-column chemistry and climate model (SCM). The inferred isoprene flux is substantially smaller than that simulated with an implementation of a commonly applied BVOC emission algorithm in the SCM.