| publications-1481 |
PEER REVIEWED ARTICLE |
2018 |
Afchine, A., Rolf, C., Costa, A., Spelten, N., Riese, M., Buchholz, B., Ebert, V., Heller, R., Kaufmann, S., Minikin, A., Voigt, C., Zöger, M., Smith |
Ice particle sampling from aircraft – influence of the probing position on the ice water content |
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10.5194/amt-11-4015-2018 |
Uncategorized |
Natural Water Bodies |
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Abstract. The ice water content (IWC) of cirrus clouds is an essential parameter determining their radiative properties and thus is important for climate simulations. Therefore, for a reliable measurement of IWC on board research aircraft, it is important to carefully design the ice crystal sampling and measuring devices. During the ML-CIRRUS field campaign in 2014 with the German Gulfstream GV HALO (High Altitude and Long Range Research Aircraft), IWC was recorded by three closed-path total water together with one gas-phase water instrument. The hygrometers were supplied by inlets mounted on the roof of the aircraft fuselage. Simultaneously, the IWC is determined by a cloud particle spectrometer attached under an aircraft wing. Two more examples of simultaneous IWC measurements by hygrometers and cloud spectrometers are presented, but the inlets of the hygrometers were mounted at the fuselage side (M-55 Geophysica, StratoClim campaign 2017) and bottom (NASA WB57, MacPex campaign 2011). This combination of instruments and inlet positions provides the opportunity to experimentally study the influence of the ice particle sampling position on the IWC with the approach of comparative measurements. As expected from theory and shown by computational fluid dynamics (CFD) calculations, we found that the IWCs provided by the roof inlets deviate from those measured under the aircraft wing. As a result of the inlet position in the shadow zone behind the aircraft cockpit, ice particle populations with mean mass sizes larger than about 25 µm radius are subject to losses, which lead to strongly underestimated IWCs. On the other hand, cloud populations with mean mass sizes smaller than about 12 µm are dominated by particle enrichment and thus overestimated IWCs. In the range of mean mass sizes between 12 and 25 µm, both enrichment and losses of ice crystals can occur, depending on whether the ice crystal mass peak of the size distribution – in these cases bimodal – is on the smaller or larger mass mode. The resulting deviations of the IWC reach factors of up to 10 or even more for losses as well as for enrichment. Since the mean mass size of ice crystals increases with temperature, losses are more pronounced at higher temperatures, while at lower temperatures IWC is more affected by enrichment. In contrast, in the cases where the hygrometer inlets were mounted at the fuselage side or bottom, the agreement of IWCs is most frequently within a factor of 2.5 or better – due to less disturbed ice particle sampling, as expected from theory – independently of the mean ice crystal sizes. The rather large scatter between IWC measurements reflects, for example, cirrus cloud inhomogeneities and instrument uncertainties as well as slight sampling biases which might also occur on the side or bottom of the fuselage and under the wing. However, this scatter is in the range of other studies and represent the current best possible IWC recording on fast-flying aircraft. |
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| publications-1482 |
PEER REVIEWED ARTICLE |
2018 |
Emma Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David |
Evaluation of stratospheric age of air from CF4, C2F6, C3F8, CHF3, HFC-125, HFC-227ea and SF6; implications for the calculations of halocarbon lifetimes, fractional release factors and ozone depletion potentials |
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10.5194/acp-18-3369-2018 |
Uncategorized |
Natural Water Bodies |
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Abstract. In a changing climate, potential stratospheric circulation changes require long-term monitoring. Stratospheric trace gas measurements are often used as a proxy for stratospheric circulation changes via the mean age of air values derived from them. In this study, we investigated five potential age of air tracers – the perfluorocarbons CF4, C2F6 and C3F8 and the hydrofluorocarbons CHF3 (HFC-23) and HFC-125 – and compare them to the traditional tracer SF6 and a (relatively) shorter-lived species, HFC-227ea. A detailed uncertainty analysis was performed on mean ages derived from these new tracers to allow us to confidently compare their efficacy as age tracers to the existing tracer, SF6. Our results showed that uncertainties associated with the mean age derived from these new age tracers are similar to those derived from SF6, suggesting that these alternative compounds are suitable in this respect for use as age tracers. Independent verification of the suitability of these age tracers is provided by a comparison between samples analysed at the University of East Anglia and the Scripps Institution of Oceanography. All five tracers give younger mean ages than SF6, a discrepancy that increases with increasing mean age. Our findings qualitatively support recent work that suggests that the stratospheric lifetime of SF6 is significantly less than the previous estimate of 3200 years. The impact of these younger mean ages on three policy-relevant parameters – stratospheric lifetimes, fractional release factors (FRFs) and ozone depletion potentials – is investigated in combination with a recently improved methodology to calculate FRFs. Updates to previous estimations for these parameters are provided. |
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| publications-1483 |
PEER REVIEWED ARTICLE |
2018 |
Adcock, K. E., Reeves, C. E., Gooch, L. J., Leedham Elvidge, E. C., Ashfold, M. J., Brenninkmeijer, C. A. M., Chou, C., Fraser, P. J., Langenfelds, R. |
Continued increase of CFC-113a (CCl3CF3) mixing ratios in the global atmosphere: emissions, occurrence and potential sources |
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10.5194/acp-18-4737-2018 |
Data Management & Analytics |
Natural Water Bodies |
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Abstract. Atmospheric measurements of the ozone-depleting substance CFC-113a (CCl3CF3) are reported from ground-based stations in Australia, Taiwan, Malaysia and the United Kingdom, together with aircraft-based data for the upper troposphere and lower stratosphere. Building on previous work, we find that, since the gas first appeared in the atmosphere in the 1960s, global CFC-113a mixing ratios have been increasing monotonically to the present day. Mixing ratios of CFC-113a have increased by 40 % from 0.50 to 0.70 ppt in the Southern Hemisphere between the end of the previously published record in December 2012 and February 2017. We derive updated global emissions of 1.7 Gg yr−1 on average between 2012 and 2016 using a two-dimensional model. We compare the long-term trends and emissions of CFC-113a to those of its structural isomer, CFC-113 (CClF2CCl2F), which still has much higher mixing ratios than CFC-113a, despite its mixing ratios and emissions decreasing since the 1990s. The continued presence of northern hemispheric emissions of CFC-113a is confirmed by our measurements of a persistent interhemispheric gradient in its mixing ratios, with higher mixing ratios in the Northern Hemisphere. The sources of CFC-113a are still unclear, but we present evidence that indicates large emissions in East Asia, most likely due to its use as a chemical involved in the production of hydrofluorocarbons. Our aircraft data confirm the interhemispheric gradient as well as showing mixing ratios consistent with ground-based observations and the relatively long atmospheric lifetime of CFC-113a. CFC-113a is the only known CFC for which abundances are still increasing substantially in the atmosphere. |
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| publications-1484 |
PEER REVIEWED ARTICLE |
2018 |
Brunamonti, S., Jorge, T., Oelsner, P., Hanumanthu, S., Singh, B. B., Kumar, K. R., Sonbawne, S., Meier, S., Singh, D., Wienhold, F. G., Luo, B. P., B |
Balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter at the southern slopes of the Himalayas during StratoClim 2016-2017 |
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10.5194/acp-18-15937-2018 |
Simulation & Modeling |
Precipitation & Ecological Systems |
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Abstract. The Asian summer monsoon anticyclone (ASMA) is a major meteorological system of the upper troposphere–lower stratosphere (UTLS) during boreal summer. It is known to contain enhanced tropospheric trace gases and aerosols, due to rapid lifting from the boundary layer by deep convection and subsequent horizontal confinement. Given its dynamical structure, the ASMA represents an efficient pathway for the transport of pollutants to the global stratosphere. A detailed understanding of the thermal structure and processes in the ASMA requires accurate in situ measurements. Within the StratoClim project we performed state-of-the-art balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter from two stations on the southern slopes of the Himalayas. In total, 63 balloon soundings were conducted during two extensive monsoon-season campaigns, in August 2016 in Nainital, India (29.4∘ N, 79.5∘ E), and in July–August 2017 in Dhulikhel, Nepal (27.6∘ N, 85.5∘ E); one shorter post-monsoon campaign was also carried out in November 2016 in Nainital. These measurements provide unprecedented insights into the UTLS thermal structure, the vertical distributions of water vapor, ozone and aerosols, cirrus cloud properties and interannual variability in the ASMA. Here we provide an overview of all of the data collected during the three campaign periods, with focus on the UTLS region and the monsoon season. We analyze the vertical structure of the ASMA in terms of significant levels and layers, identified from the temperature and potential temperature lapse rates and Lagrangian backward trajectories, which provides a framework for relating the measurements to local thermodynamic properties and the large-scale anticyclonic flow. Both the monsoon-season campaigns show evidence of deep convection and confinement extending up to 1.5–2 km above the cold-point tropopause (CPT), yielding a body of air with high water vapor and low ozone which is prone to being lifted further and mixed into the free stratosphere. Enhanced aerosol backscatter also reveals the signature of the Asian tropopause aerosol layer (ATAL) over the same region of altitudes. The Dhulikhel 2017 campaign was characterized by a 5 K colder CPT on average than in Nainital 2016 and a local water vapor maximum in the confined lower stratosphere, about 1 km above the CPT. Data assessment and modeling studies are currently ongoing with the aim of fully exploring this dataset and its implications with respect to stratospheric moistening via the ASMA system and related processes. |
603557 |
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| publications-1485 |
PEER REVIEWED ARTICLE |
2018 |
A. Mannan Zafar , Rolf Müller , Jens-Uwe Grooss , Sabine Robrecht , Bärbel Vogel , Ralph Lehmann |
The relevance of reactions of the methyl peroxy radical (CH 3 O 2 ) and methylhypochlorite (CH 3 OCl) for Antarctic chlorine activation and ozone loss |
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10.1080/16000889.2018.1507391 |
Simulation & Modeling |
Natural Water Bodies |
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No abstract available |
603557 |
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| publications-1486 |
PEER REVIEWED ARTICLE |
2018 |
Dan Li , Bärbel Vogel , Rolf Müller , Jianchun Bian , Gebhard Günther , Qian Li , Jinqiang Zhang , Zhixuan Bai , Holger Vömel , Martin Riese |
High tropospheric ozone in Lhasa within the Asian summer monsoon anticyclone in 2013: influence of convective transport and stratospheric intrusions |
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10.5194/acp-18-17979-2018 |
Simulation & Modeling |
Natural Water Bodies |
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Abstract. Balloon-borne measurements of ozone in Lhasa (29.66∘ N, 91.14∘ E; 3650 m above sea level) in August 2013 are investigated using backward trajectory calculations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). Measurements show three time periods characterized by high ozone mixing ratios (OMRs) in the troposphere on 8, 11, and 18–20 August 2013 during the Asian summer monsoon (ASM) season. Here, we verified two different sources for the enhanced ozone values in the troposphere. First, transport of polluted air from the boundary layer, and second downward transport from the stratosphere by stratospheric intrusions. Air pollution from South Asia through convective and long-range transport plays a key role in enhancing middle tropospheric OMRs up to 90 % on 8 August and up to 125 % on 11 August 2013 compared to monthly mean ozone of August 2013. Stratospheric air intruded from the northern high-latitudes to the southeastern flank of the ASM anticyclone to the troposphere and is identified as the source of enhanced ozone according to backward trajectory calculation and satellite measurements by the Ozone Monitoring Instrument (OMI) and the Atmospheric Infrared Sounder (AIRS). Air parcels with high ozone moved from the high-latitude lower stratosphere to the middle and upper troposphere. These air parcels are then transported to Lhasa over long distances and enhanced upper and middle tropospheric ozone over Lhasa during 18–20 August 2013. Our findings demonstrate that the strong variability of ozone within the ASM anticyclone in the free troposphere is caused by transport from very different regions of the atmosphere. |
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| publications-1487 |
PEER REVIEWED ARTICLE |
2017 |
Norbert Glatthor , Michael Höpfner , Adrian Leyser , Gabriele P. Stiller , Thomas von Clarmann , Udo Grabowski , Sylvia Kellmann , Andrea Linden , Bj |
Global carbonyl sulfide (OCS) measured by MIPAS/Envisat during 2002–2012 |
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10.5194/acp-17-2631-2017 |
Simulation & Modeling |
Natural Water Bodies |
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Abstract. We present a global carbonyl sulfide (OCS) data set covering the period June 2002 to April 2012, derived from FTIR (Fourier transform infrared) limb emission spectra measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the ENVISAT satellite. The vertical resolution is 4–5 km in the height region 6–15 km and 15 at 40 km altitude. The total estimated error amounts to 40–50 pptv between 10 and 20 km and to 120 pptv at 40 km altitude. MIPAS OCS data show no systematic bias with respect to balloon observations, with deviations mostly below ±50 pptv. However, they are systematically higher than the OCS volume mixing ratios of the ACE-FTS instrument on SCISAT, with maximum deviations of up to 100 pptv in the altitude region 13–16 km. The data set of MIPAS OCS exhibits only moderate interannual variations and low interhemispheric differences. Average concentrations at 10 km altitude range from 480 pptv at high latitudes to 500–510 pptv in the tropics and at northern mid-latitudes. Seasonal variations at 10 km altitude amount to up to 35 pptv in the Northern and up to 15 pptv in the Southern Hemisphere. Northern hemispheric OCS abundances at 10 km altitude peak in June in the tropics and around October at high latitudes, while the respective southern hemispheric maxima were observed in July and in November. Global OCS distributions at 250 hPa (∼ 10–11 km) show enhanced values at low latitudes, peaking during boreal summer above the western Pacific and the Indian Ocean, which indicates oceanic release. Further, a region of depleted OCS amounts extending from Brazil to central and southern Africa was detected at this altitude, which is most pronounced in austral summer. This depletion is related to seasonally varying vegetative uptake by the tropical forests. Typical signatures of biomass burning like the southern hemispheric biomass burning plume are not visible in MIPAS data, indicating that this process is only a minor source of upper tropospheric OCS. At the 150 hPa level (∼ 13–14 km) enhanced amounts of OCS were also observed inside the Asian monsoon anticyclone, but this enhancement is not especially outstanding compared to other low latitude regions at the same altitude. At the 80 hPa level (∼ 17–18 km), equatorward transport of mid-latitude air masses containing lower OCS amounts around the summertime anticyclones was observed. A significant trend could not be detected in upper tropospheric MIPAS OCS amounts, which points to globally balanced sources and sinks. Simulations with the ECHAM-MESSy model reproduce the observed latitudinal cross sections fairly well. |
603557 |
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| publications-1488 |
PEER REVIEWED ARTICLE |
2018 |
Sandip S. Dhomse, et al. |
Estimates of ozone return dates from Chemistry-Climate Model Initiative simulations |
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10.5194/acp-18-8409-2018 |
Simulation & Modeling |
Uncategorized |
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Abstract. >We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models. |
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| publications-1489 |
PEER REVIEWED ARTICLE |
2016 |
Patrick Jöckel , Holger Tost , Andrea Pozzer , Markus Kunze , Oliver Kirner , Carl A. M. Brenninkmeijer , Sabine Brinkop , Duy S. Cai , Christoph Dyr |
Earth System Chemistry integrated Modelling (ESCiMo) with the Modular Earth Submodel System (MESSy) version 2.51 |
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10.5194/gmd-9-1153-2016 |
AI & Machine Learning |
Uncategorized |
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Abstract. Three types of reference simulations, as recommended by the Chemistry–Climate Model Initiative (CCMI), have been performed with version 2.51 of the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model: hindcast simulations (1950–2011), hindcast simulations with specified dynamics (1979–2013), i.e. nudged towards ERA-Interim reanalysis data, and combined hindcast and projection simulations (1950–2100). The manuscript summarizes the updates of the model system and details the different model set-ups used, including the on-line calculated diagnostics. Simulations have been performed with two different nudging set-ups, with and without interactive tropospheric aerosol, and with and without a coupled ocean model. Two different vertical resolutions have been applied. The on-line calculated sources and sinks of reactive species are quantified and a first evaluation of the simulation results from a global perspective is provided as a quality check of the data. The focus is on the intercomparison of the different model set-ups. The simulation data will become publicly available via CCMI and the Climate and Environmental Retrieval and Archive (CERA) database of the German Climate Computing Centre (DKRZ). This manuscript is intended to serve as an extensive reference for further analyses of the Earth System Chemistry integrated Modelling (ESCiMo) simulations. |
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| publications-1490 |
PEER REVIEWED ARTICLE |
2016 |
Pasquale Sellitto , Alcide di Sarra , Stefano Corradini , Marie Boichu , Hervé Herbin , Philippe Dubuisson , Geneviève Sèze , Daniela Meloni , Fran |
Synergistic use of Lagrangian dispersion and radiative transfer modelling with satellite and surface remote sensing measurements for the investigation of volcanic plumes: the Mount Etna eruption of 25–27 October 2013 |
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10.5194/acp-16-6841-2016 |
Uncategorized |
Uncategorized |
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Abstract. In this paper we combine SO2 and ash plume dispersion modelling with satellite and surface remote sensing observations to study the regional influence of a relatively weak volcanic eruption from Mount Etna on the optical and micro-physical properties of Mediterranean aerosols. We analyse the Mount Etna eruption episode of 25–27 October 2013. The evolution of the plume along the trajectory is investigated by means of the FLEXible PARTicle Lagrangian dispersion (FLEXPART) model. The satellite data set includes true colour images, retrieved values of volcanic SO2 and ash, estimates of SO2 and ash emission rates derived from MODIS (MODerate resolution Imaging Spectroradiometer) observations and estimates of cloud top pressure from SEVIRI (Spinning Enhanced Visible and InfraRed Imager). Surface remote sensing measurements of aerosol and SO2 made at the ENEA Station for Climate Observations (35.52° N, 12.63° E; 50 m a.s.l.) on the island of Lampedusa are used in the analysis. The combination of these different data sets suggests that SO2 and ash, despite the initial injection at about 7.0 km altitude, reached altitudes around 10–12 km and influenced the column average aerosol particle size distribution at a distance of more than 350 km downwind. This study indicates that even a relatively weak volcanic eruption may produce an observable effect on the aerosol properties at the regional scale. The impact of secondary sulfate particles on the aerosol size distribution at Lampedusa is discussed and estimates of the clear-sky direct aerosol radiative forcing are derived. Daily shortwave radiative forcing efficiencies, i.e. radiative forcing per unit AOD (aerosol optical depth), are calculated with the LibRadtran model. They are estimated between −39 and −48 W m−2 AOD−1 at the top of the atmosphere and between −66 and −49 W m−2 AOD−1 at the surface, with the variability in the estimates mainly depending on the aerosol single scattering albedo. These results suggest that sulfate particles played a large role in the transported plume composition and radiative forcing, while the contribution by ash particles was small in the volcanic plume arriving at Lampedusa during this event. |
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