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- ItemNear-global aerosol mapping in the upper troposphere and lowermost stratosphere with data from the CARIBIC project(Milton Park : Taylor & Francis, 2017) Heintzenberg, Jost; Hermann, Markus; Weigelt, Andreas; Kapustin, Vladimir; Anderson, Bruce; Thornhill, Kenneth; Van Velthoven, Peter; Zahn, Andreas; Brenninkmeijer, CarlThis study extrapolates aerosol data of the CARIBIC project from 1997 until June 2008 in along trajectories to compose large-scale maps and vertical profiles of submicrometre particle concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). The extrapolation was validated by comparing extrapolated values with CARIBIC data measured near the respective trajectory position and by comparing extrapolated CARIBIC data to measurements by other experiments near the respective trajectory positions. Best agreement between extrapolated and measured data is achieved with particle lifetimes longer than the maximum length of used trajectories. The derived maps reveal regions of strong and frequent new particle formation, namely the Tropical Central and Western Africa with the adjacent Atlantic, South America, the Caribbean and Southeast Asia. These regions of particle formation coincide with those of frequent deep convective clouds. Vertical particle concentration profiles for the troposphere and the stratosphere confirm statistically previous results indicating frequent new particle formation in the tropopause region. There was no statistically significant increase in Aitken mode particle concentration between the first period of CARIBIC operation, 1997–2002, and the second period, 2004–2009. However, a significant increase in concentration occurred within the latter period when considering it in isolation.
- ItemDiurnal variation of midlatitudinal NO3 column abundance over table mountain facility, California(Göttingen : Copernicus GmbH, 2011) Chen, C.M.; Cageao, R.P.; Lawrence, L.; Stutz, J.; Salawitch, R.J.; Jourdain, L.; Li, Q.; Sander, S.P.The column abundance of NO3 was measured over Table Mountain Facility, CA (34.4° 117.7° W) from May 2003 through September 2004, using lunar occultation near full moon with a grating spectrometer. The NO 3 column retrieval was performed with the differential optical absorption spectroscopy (DOAS) technique using both the 623 and 662 nm NO 3 absorption bands. Other spectral features such as Fraunhofer lines and absorption from water vapor and oxygen were removed using solar spectra obtained at different airmass factors. We observed a seasonal variation, with nocturnally averaged NO3 columns between 5-7 × 1013 molec cm-2 during October through March, and 5-22 × 10 13 molec cm-2 during April through September. A subset of the data, with diurnal variability vastly different from the temporal profile obtained from one-dimensional stratospheric model calculations, clearly has boundary layer contributions; this was confirmed by simultaneous long-path DOAS measurements. However, even the NO3 columns that did follow the modeled time evolution were often much larger than modeled stratospheric partial columns constrained by realistic temperatures and ozone concentrations. This discrepancy is attributed to substantial tropospheric NO3 in the free troposphere, which may have the same time dependence as stratospheric NO 3.
- ItemPolarization lidar: An extended three-signal calibration approach(Katlenburg-Lindau : Copernicus, 2019) Jimenez, Cristofer; Ansmann, Albert; Engelmann, Ronny; Haarig, Moritz; Schmidt, Jörg; Wandinger, UllaWe present a new formalism to calibrate a threesignal polarization lidar and to measure highly accurate height profiles of the volume linear depolarization ratios under realistic experimental conditions. The methodology considers elliptically polarized laser light, angular misalignment of the receiver unit with respect to the main polarization plane of the laser pulses, and cross talk among the receiver channels. A case study of a liquid-water cloud observation demonstrates the potential of the new technique. Long-term observations of the calibration parameters corroborate the robustness of the method and the long-term stability of the three-signal polarization lidar. A comparison with a second polarization lidar shows excellent agreement regarding the derived volume linear polarization ratios in different scenarios: A biomass burning smoke event throughout the troposphere and the lower stratosphere up to 16 km in height, a dust case, and also a cirrus cloud case. © Author(s) 2019.
- ItemParticulate sulfur in the upper troposphere and lowermost stratosphere - Sources and climate forcing(Katlenburg-Lindau : EGU, 2017) Martinsson, Bengt G.; Friberg, Johan; Sandvik, Oscar S.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, AndreasThis study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8-12 km altitude of the IAGOS-CARIBIC platform in the time period 1999-2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.
- ItemMercury distribution in the upper troposphere and lowermost stratosphere according to measurements by the IAGOS-CARIBIC observatory: 2014-2016(Katlenburg-Lindau : EGU, 2018) Slemr, Franz; Weigelt, Andreas; Ebinghaus, Ralf; Bieser, Johannes; Brenninkmeijer, Carl A. M.; Rauthe-Schöch, Armin; Hermann, Markus; Martinsson, Bengt G.; van Velthoven, Peter; Bönisch, Harald; Neumaier, Marco; Zahn, Andreas; Ziereis, HelmutMercury was measured onboard the IAGOS-CARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM-thinsp;GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes.
- ItemDepolarization and lidar ratios at 355, 532, and 1064 nm and microphysical properties of aged tropospheric and stratospheric Canadian wildfire smoke(Göttingen : Copernicus GmbH, 2018) Haarig, M.; Ansmann, A.; Baars, H.; Jimenez, C.; Veselovskii, I.; Engelmann, R.; Althausen, D.We present spectrally resolved optical and microphysical properties of western Canadian wildfire smoke observed in a tropospheric layer from 5-6.5 km height and in a stratospheric layer from 15-16 km height during a recordbreaking smoke event on 22 August 2017. Three polarization/ Raman lidars were run at the European Aerosol Research Lidar Network (EARLINET) station of Leipzig, Germany, after sunset on 22 August. For the first time, the linear depolarization ratio and extinction-to-backscatter ratio (lidar ratio) of aged smoke particles were measured at all three important lidar wavelengths of 355, 532, and 1064 nm. Very different particle depolarization ratios were found in the troposphere and in the stratosphere. The obviously compact and spherical tropospheric smoke particles caused almost no depolarization of backscattered laser radiation at all three wavelengths ( < 3 %), whereas the dry irregularly shaped soot particles in the stratosphere lead to high depolarization ratios of 22% at 355 nm and 18% at 532 nm and a comparably low value of 4% at 1064 nm. The lidar ratios were 40- 45 sr (355 nm), 65-80 sr (532 nm), and 80-95 sr (1064 nm) in both the tropospheric and stratospheric smoke layers indicating similar scattering and absorption properties. The strong wavelength dependence of the stratospheric depolarization ratio was probably caused by the absence of a particle coarse mode (particle mode consisting of particles with radius > 500nm). The stratospheric smoke particles formed a pronounced accumulation mode (in terms of particle volume or mass) centered at a particle radius of 350-400 nm. The effective particle radius was 0.32 μm. The tropospheric smoke particles were much smaller (effective radius of 0.17 μm). Mass concentrations were of the order of 5.5 μgm-3 (tropospheric layer) and 40 μgm-3 (stratospheric layer) in the night of 22 August 2017. The single scattering albedo of the stratospheric particles was estimated to be 0.74, 0.8, and 0.83 at 355, 532, and 1064 nm, respectively.
- ItemTropospheric forcing of the boreal polar vortex splitting in January 2003(München : European Geopyhsical Union, 2010) Peters, D.H.W.; Vargin, P.; Gabriel, A.; Tsvetkova, N.; Yushkov, V.e dynamical evolution of the relatively warm stratospheric winter season 2002–2003 in the Northern Hemisphere was studied and compared with the cold winter 2004–2005 based on NCEP-Reanalyses. Record low temperatures were observed in the lower and middle stratosphere over the Arctic region only at the beginning of the 2002–2003 winter. Six sudden stratospheric warming events, including the major warming event with a splitting of the polar vortex in mid-January 2003, have been identified. This led to a very high vacillation of the zonal mean circulation and a weakening of the stratospheric polar vortex over the whole winter season. An estimate of the mean chemical ozone destruction inside the polar vortex showed a total ozone loss of about 45 DU in winter 2002–2003; that is about 2.5 times smaller than in winter 2004–2005. Embedded in a winter with high wave activity, we found two subtropical Rossby wave trains in the troposphere before the major sudden stratospheric warming event in January 2003. These Rossby waves propagated north-eastwards and maintained two upper tropospheric anticyclones. At the same time, the amplification of an upward propagating planetary wave 2 in the upper troposphere and lower stratosphere was observed, which could be caused primarily by those two wave trains. Furthermore, two extratropical Rossby wave trains over the North Pacific Ocean and North America were identified a couple of days later, which contribute mainly to the vertical planetary wave activity flux just before and during the major warming event. It is shown that these different tropospheric forcing processes caused the major warming event and contributed to the splitting of the polar vortex.
- ItemGlobal annual methane emission rate derived from its current atmospheric mixing ratio and estimated lifetime(Göttingen : Copernicus, 2014) Sonnemann, G.R.; Grygalashvyly, M.We use the estimated lifetime of methane (CH4), the current methane concentration, and its annual growth rate to calculate the global methane emission rate. The upper and lower limits of the annual global methane emission rate, depending on loss of CH4 into the stratosphere and methane consuming bacteria, amounts to 648.0 Mt a-1 and 608.0 Mt a-1. These values are in reasonable agreement with satellite and with much more accurate in situ measurements of methane. We estimate a mean tropospheric and mass-weighted temperature related to the reaction rate and employ a mean OH-concentration to calculate a mean methane lifetime. The estimated atmospheric lifetime of methane amounts to 8.28 years and 8.84 years, respectively. In order to improve the analysis a realistic 3D-calculations should be performed.