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    The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere
    (Katlenburg-Lindau : Copernicus, 2022) Dragoneas, Antonis; Molleker, Sergej; Appel, Oliver; Hünig, Andreas; Böttger, Thomas; Hermann, Markus; Drewnick, Frank; Schneider, Johannes; Weigel, Ralf; Borrmann, Stephan
    We report on the developments that enabled the field deployment of a fully automated aerosol mass spectrometer, especially designed for high-altitude measurements on unpressurized aircraft. The merits of the two main categories of real-time aerosol mass spectrometry, i.e. (a) single-particle laser desorption and ionization and (b) continuous thermal desorption and electron impact ionization of aerosols, have been integrated into one compact apparatus with the aim to perform in situ real-time analysis of aerosol chemical composition. The demonstrated instrument, named the ERICA (European Research Council Instrument for Chemical composition of Aerosols), operated successfully aboard the high-altitude research aircraft M-55 Geophysica at altitudes up to 20 km while being exposed to ambient conditions of very low atmospheric pressure and temperature. A primary goal of those field deployments was the in situ study of the Asian tropopause aerosol layer (ATAL). During 11 research flights, the instrument operated for more than 49 h and collected chemical composition information of more than 150 000 single particles combined with quantitative chemical composition analysis of aerosol particle ensembles. This paper presents in detail the technical characteristics of the main constituent parts of the instrument, as well as the design considerations for its integration into the aircraft and its autonomous operation in the upper troposphere and lower stratosphere (UTLS). Additionally, system performance data from the first field deployments of the instrument are presented and discussed, together with exemplary mass spectrometry data collected during those flights.
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    Tropospheric and stratospheric wildfire smoke profiling with lidar: mass, surface area, CCN, and INP retrieval
    (Katlenburg-Lindau : European Geosciences Union, 2021) Ansmann, Albert; Ohneiser, Kevin; Mamouri, Rodanthi-Elisavet; Knopf, Daniel A.; Veselovskii, Igor; Baars, Holger; Engelmann, Ronny; Foth, Andreas; Jimenez, Cristofer; Seifert, Patric; Barja, Boris
    We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area, and number concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations from backscatter lidar measurements on the ground and in space. Conversion factors used to convert the optical measurements into microphysical properties play a central role in the data analysis, in addition to estimates of the smoke extinction-to-backscatter ratios required to obtain smoke extinction coefficients. The set of needed conversion parameters for wildfire smoke is derived from AERONET observations of major smoke events, e.g., in western Canada in August 2017, California in September 2020, and southeastern Australia in January-February 2020 as well as from AERONET long-term observations of smoke in the Amazon region, southern Africa, and Southeast Asia. The new smoke analysis scheme is applied to CALIPSO observations of tropospheric smoke plumes over the United States in September 2020 and to ground-based lidar observation in Punta Arenas, in southern Chile, in aged Australian smoke layers in the stratosphere in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document large-scale and long-lasting wildfire smoke events in detail and thus to provide valuable information for climate, cloud, and air chemistry modeling efforts performed to investigate the role of wildfire smoke in the atmospheric system. © 2021 Albert Ansmann et al.
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    Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100
    (Katlenburg-Lindau : European Geosciences Union, 2021) Keeble, James; Hassler, Birgit; Banerjee, Antara; Checa-Garcia, Ramiro; Chiodo, Gabriel; Davis, Sean; Eyring, Veronika; Griffiths, Paul T.; Morgenstern, Olaf; Nowack, Peer; Zeng, Guang; Zhang, Jiankai; Bodeker, Greg; Burrows, Susannah; Cameron-Smith, Philip; Cugnet, David; Danek, Christopher; Deushi, Makoto; Horowitz, Larry W.; Kubin, Anne; Li, Lijuan; Lohmann, Gerrit; Michou, Martine; Mills, Michael J.; Nabat, Pierre; Olivié, Dirk; Park, Sungsu; Seland, Øyvind; Stoll, Jens; Wieners, Karl-Hermann; Wu, Tongwen
    Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer-Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions. © Author(s) 2021.
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    Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke
    (Katlenburg-Lindau : EGU, 2022) Ansmann, Albert; Ohneiser, Kevin; Chudnovsky, Alexandra; Knopf, Daniel A.; Eloranta, Edwin W.; Villanueva, Diego; Seifert, Patric; Radenz, Martin; Barja, Boris; Zamorano, Félix; Jimenez, Cristofer; Engelmann, Ronny; Baars, Holger; Griesche, Hannes; Hofer, Julian; Althausen, Dietrich; Wandinger, Ulla
    A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019-May 2020) and over Punta Arenas in southern Chile at 53.2°S (January 2020-November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10-12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10-12 km, smoke particle surface area (SA) concentrations of 5-7 μm2 cm-3 (Antarctica, spring 2021) and 6-10 μm2 cm-3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4-1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2-3.5 mPa (Arctic, 20 %-30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1-2 mPa (10 %-20 % contribution to the total ozone loss over Antarctica) was observed in the 14-23 km PSC height range in September-October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm-3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26-30 Dobson units (9 %-10 %, September 2020, 2021) and 52-57 Dobson units (17 %-20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70-80°S. Copyright:
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    Orographically induced spontaneous imbalance within the jet causing a large-scale gravity wave event
    (Katlenburg-Lindau : European Geosciences Union, 2021) Geldenhuys, Markus; Preusse, Peter; Krisch, Isabell; Zülicke, Christoph; Ungermann, Jörn; Ern, Manfred; Friedl-Vallon, Felix; Riese, Martin
    To better understand the impact of gravity waves (GWs) on the middle atmosphere in the current and future climate, it is essential to understand their excitation mechanisms and to quantify their basic properties. Here a new process for GW excitation by orography-jet interaction is discussed. In a case study, we identify the source of a GW observed over Greenland on 10 March 2016 during the POLSTRACC (POLar STRAtosphere in a Changing Climate) aircraft campaign. Measurements were taken with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) instrument deployed on the High Altitude Long Range (HALO) German research aircraft. The measured infrared limb radiances are converted into a 3D observational temperature field through the use of inverse modelling and limited-angle tomography. We observe GWs along a transect through Greenland where the GW packet covers ≈1/3 of the Greenland mainland. GLORIA observations indicate GWs between 10 and 13km of altitude with a horizontal wavelength of 330km, a vertical wavelength of 2km and a large temperature amplitude of 4.5K. Slanted phase fronts indicate intrinsic propagation against the wind, while the ground-based propagation is with the wind. The GWs are arrested below a critical layer above the tropospheric jet. Compared to its intrinsic horizontal group velocity (25-72ms-1) the GW packet has a slow vertical group velocity of 0.05-0.2ms-1. This causes the GW packet to propagate long distances while spreading over a large area and remaining constrained to a narrow vertical layer. A plausible source is not only orography, but also out-of-balance winds in a jet exit region and wind shear. To identify the GW source, 3D GLORIA observations are combined with a gravity wave ray tracer, ERA5 reanalysis and high-resolution numerical experiments. In a numerical experiment with a smoothed orography, GW activity is quite weak, indicating that the GWs in the realistic orography experiment are due to orography. However, analysis shows that these GWs are not mountain waves. A favourable area for spontaneous GW emission is identified in the jet by the cross-stream ageostrophic wind, which indicates when the flow is out of geostrophic balance. Backwards ray-tracing experiments trace into the jet and regions where the Coriolis and the pressure gradient forces are out of balance. The difference between the full and a smooth-orography experiment is investigated to reveal the missing connection between orography and the out-of-balance jet. We find that this is flow over a broad area of elevated terrain which causes compression of air above Greenland. The orography modifies the wind flow over large horizontal and vertical scales, resulting in out-of-balance geostrophic components. The out-of-balance jet then excites GWs in order to bring the flow back into balance. This is the first observational evidence of GW generation by such an orography-jet mechanism.
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    VAHCOLI, a new concept for lidars: technical setup, science applications, and first measurements
    (Katlenburg-Lindau : European Geosciences Union, 2021) Lübken, Franz-Josef; Höffner, Josef
    A new concept for a cluster of compact lidar systems named VAHCOLI (Vertical And Horizontal COverage by LIdars) is presented, which allows for the measurement of temperatures, winds, and aerosols in the middle atmosphere (10 110 km) with high temporal and vertical resolution of minutes and some tens of meters, respectively, simultaneously covering horizontal scales from a few hundred meters to several hundred kilometers ( four-dimensional coverage ). The individual lidars ( units ) being used in VAHCOLI are based on a diode-pumped alexandrite laser, which is currently designed to detect potassium (D 770 nm), and on sophisticated laser spectroscopy measuring all relevant frequencies (seeder laser, power laser, backscattered light) with high temporal resolution (2 ms) and high spectral resolution applying Doppler-free spectroscopy. The frequency of the lasers and the narrowband filter in the receiving system are stabilized to typically 10 100 kHz, which is a factor of roughly 105 smaller than the Doppler-broadened Rayleigh signal. Narrowband filtering allows for the measurement of Rayleigh and/or resonance scattering separately from the aerosol (Mie) signal during both night and day. Lidars used for VAHCOLI are compact (volume: 1m3) and multi-purpose systems which employ contemporary electronic, optical, and mechanical components. The units are designed to autonomously operate under harsh field conditions in remote locations. An error analysis with parameters of the anticipated system demonstrates that temperatures and line-of-sight winds can be measured from the lower stratosphere to the upper mesosphere with an accuracy of (0.1 5)K and (0.1 10)ms1, respectively, increasing with altitude. We demonstrate that some crucial dynamical processes in the middle atmosphere, such as gravity waves and stratified turbulence, can be covered by VAHCOLI with sufficient temporal, vertical, and horizontal sampling and resolution. The four-dimensional capabilities of VAHCOLI allow for the performance of time-dependent analysis of the flow field, for example by employing Helmholtz decomposition, and for carrying out statistical tests regarding, for example, intermittency and helicity. The first test measurements under field conditions with a prototype lidar were performed in January 2020. The lidar operated successfully during a 6-week period (night and day) without any adjustment. The observations covered a height range of 5 100 km and demonstrated the capability and applicability of this unit for the VAHCOLI concept.
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    Validation of Aeolus wind products above the Atlantic Ocean
    (Katlenburg-Lindau : Copernicus, 2020) Baars, Holger; Herzog, Alina; Heese, Birgit; Ohneiser, Kevin; Hanbuch, Karsten; Hofer, Julian; Yin, Zhenping; Engelmann, Ronny; Wandinger, Ulla
    In August 2018, the first Doppler wind lidar in space called Atmospheric Laser Doppler Instrument (ALADIN) was launched on board the satellite Aeolus by the European Space Agency (ESA). Aeolus measures profiles of one horizontal wind component (i.e., mainly the west-east direction) in the troposphere and lower stratosphere on a global basis. Furthermore, profiles of aerosol and cloud properties can be retrieved via the high spectral resolution lidar (HSRL) technique. The Aeolus mission is supposed to improve the quality of weather forecasts and the understanding of atmospheric processes. We used the opportunity to perform a unique validation of the wind products of Aeolus by utilizing the RV Polarstern cruise PS116 from Bremerhaven to Cape Town in November/December 2018. Due to concerted course modifications, six direct intersections with the Aeolus ground track could be achieved in the Atlantic Ocean west of the African continent. For the validation of the Aeolus wind products, we launched additional radiosondes and used the EARLINET/ACTRIS lidar Polly XT for atmospheric scene analysis. The six analyzed cases prove that Aeolus is able to measure horizontal wind speeds in the nearly west-east direction. Good agreements with the radiosonde observations could be achieved for both Aeolus wind products-the winds observed in clean atmospheric regions called Rayleigh winds and the winds obtained in cloud layers called Mie winds (according to the responsible scattering regime). Systematic and statistical errors of the Rayleigh winds were less than 1.5 and 3.3ms-1, respectively, when compared to radiosonde values averaged to the vertical resolution of Aeolus. For the Mie winds, a systematic and random error of about 1ms-1 was obtained from the six comparisons in different climate zones. However, it is also shown that the coarse vertical resolution of 2km in the upper troposphere, which was set in this early mission phase 2 months after launch, led to an underestimation of the maximum wind speed in the jet stream regions. In summary, promising first results of the first wind lidar space mission are shown and prove the concept of Aeolus for global wind observations. © 2020 Author(s).
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    How the extreme 2019-2020 Australian wildfires affected global circulation and adjustments
    (Katlenburg-Lindau : EGU, 2023) Senf, Fabian; Heinold, Bernd; Kubin, Anne; Müller, Jason; Schrödner, Roland; Tegen, Ina
    Wildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019-2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17ĝ€¯km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol-climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5ĝ€¯Wm-2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5ĝ€¯Wm-2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2ĝ€¯%. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.
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    Global perturbation of stratospheric water and aerosol burden by Hunga eruption
    (London : Springer Nature, 2022) Khaykin, Sergey; Podglajen, Aurelien; Ploeger, Felix; Grooß, Jens-Uwe; Tence, Florent; Bekki, Slimane; Khlopenkov, Konstantin; Bedka, Kristopher; Rieger, Landon; Baron, Alexandre; Godin-Beekmann, Sophie; Legras, Bernard; Sellitto, Pasquale; Sakai, Tetsu; Barnes, John; Uchino, Osamu; Morino, Isamu; Nagai, Tomohiro; Wing, Robin; Baumgarten, Gerd; Gerding, Michael; Duflot, Valentin; Payen, Guillaume; Jumelet, Julien; Querel, Richard; Liley, Ben; Bourassa, Adam; Clouser, Benjamin; Feofilov, Artem; Hauchecorne, Alain; Ravetta, François
    The eruption of the submarine Hunga volcano in January 2022 was associated with a powerful blast that injected volcanic material to altitudes up to 58 km. From a combination of various types of satellite and ground-based observations supported by transport modeling, we show evidence for an unprecedented increase in the global stratospheric water mass by 13% relative to climatological levels, and a 5-fold increase of stratospheric aerosol load, the highest in the last three decades. Owing to the extreme injection altitude, the volcanic plume circumnavigated the Earth in only 1 week and dispersed nearly pole-to-pole in three months. The unique nature and magnitude of the global stratospheric perturbation by the Hunga eruption ranks it among the most remarkable climatic events in the modern observation era, with a range of potential long-lasting repercussions for stratospheric composition and climate.