Abstract. Preliminary attempts of quantifying the stratospheric ozone contribution in the observations at the Zugspitze summit (2962 m a.s.l.) next to GarmischPartenkirchen in the German Alps had yielded an approximate doubling of the stratospheric fraction of the Zugspitze ozone during the time period 1978 to 2004. These investigations had been based on data filtering by using low relative humidity (RH) and elevated 7 Be as the criteria for selecting half-hour intervals of ozone data representative of stratospheric intrusion air. To quantify the residual stratospheric component in stratospherically influenced air masses, however, the mixing of tropospheric air into the stratospheric intrusion layers must be taken into account. In fact, the dewpoint mirror instrument at the Zugspitze summit station rarely registers RH values lower than 10 % in stratospheric air intrusions. Since 2007 a programme of routine lidar sounding of ozone, water vapour and aerosol has been conducted in the Garmisch-Partenkirchen area. The lidar results demonstrate that the intrusion layers are drier by roughly one order of magnitude than indicated in the in situ measurements. Even in thin layers RH values clearly below 1 % have frequently been observed. These thin, undiluted layers present an important challenge for atmospheric modelling. Although the ozone values never reach values typical of the lower-stratosphere it becomes, thus, obvious that, without strong wind shear or convective processes, mixing of stratospheric and tropospheric air must be very slow in most of the free troposphere. As a consequence, the analysis the Zugspitze data can be assumed to be more reliable than anticipated. Finally, the concentrations of Zugspitze carbon monoxide rarely drop inside intrusion layers and normally stay clearly above full stratospheric values. This indicates that most of the CO, and thus the intrusion air mass, originates in the shallow "mixing layer" around the thermal tropopause. The CO mixing ratio in these descending layers between 1990 and 2004 exhibits a slightly positive trend indicating some Asian influence on the lowermost stratosphere in the high-latitude source region of most intrusions reaching the station.

The eruption of the Icelandic volcano Eyjafjallajökull in April- May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April-26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org.During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5-15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area.The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events

In 1978–1980, measurements of dissolved carbon monoxide in seawater were carried out during three ship expeditions in the northern and southern Atlantic Ocean, covering an area between 53°N and 35°S. Measurements in surface water were performed by a continuously working equilibration technique that allowed for the determination of small and rapid variations of the dissolved CO. Carbon monoxide concentrations in the water body increased toward the sea surface, there reaching saturation factors of up to 50 with respect to atmospheric CO. The daily average CO saturation increased with average chlorophyll a concentration and light intensity and decreased with wind speed. The dissolved CO showed strong diurnal variations, with maximum values in the afternoon. Diurnal variations were observed within the entire euphotic zone, indicating that CO is both produced and consumed in the seawater. Carbon monoxide production in seawater was mainly due to photooxidation of dissolved organic matter. Photobiological and microbial CO production processes were of minor importance. Carbon monoxide destruction was due to a light‐independent microbial metabolism. Based on average CO saturation factors of 30±20 in the surface water of the ocean, the total source strength for atmospheric CO is calculated to 10–180 Tg yr−1.

Lidar measurements at Garmisch-Partenkirchen (Germany) have almost continually delivered backscatter coefficients of stratospheric aerosol since 1976. The time series is dominated by signals from the particles injected into or formed in the stratosphere due to major volcanic eruptions, in particular those of El Chichon (Mexico, 1982) and Mt Pinatubo (Philippines, 1991). Here, we focus more on the long-lasting background period since the late 1990s and 2006, in view of processes maintaining a residual lower-stratospheric aerosol layer in absence of major eruptions, as well as the period of moderate volcanic impact afterwards. During the long background period the stratospheric backscatter coefficients reached a level even below that observed in the late 1970s. This suggests that the predicted potential influence of the strongly growing air traffic on the stratospheric aerosol loading is very low. Some correlation may be found with single strong forest-fire events, but the average influence of biomass burning seems to be quite limited. No positive trend in background aerosol can be resolved over a period as long as that observed by lidar at Mauna Loa. We conclude that the increase of our integrated backscatter coefficients starting in 2008 is mostly due to volcanic eruptions with explosivity index 4, penetrating strongly into the stratosphere. Most of them occurred in the mid-latitudes. A key observation for judging the role of eruptions just reaching the tropopause region was that of the plume from the Icelandic volcano Eyjafjallajökull above Garmisch-Partenkirchen (April 2010) due to the proximity of that source. The top altitude of the ash above the volcano was reported just as 9.3 km, but the lidar measurements revealed enhanced stratospheric aerosol up to 14.3 km. Our analysis suggests for two or three of the four measurement days the presence of a stratospheric contribution from Iceland related to quasi-horizontal transport, differing from the strong descent of the layers entering Central Europe at low altitudes. The backscatter coefficients within the first 2 km above the tropopause exceed the stratospheric background by a factor of four to five. In addition, Asian and Saharan dust layers were identified in the free troposphere, Asian dust most likely even in the stratosphere

[1] Extreme pyrocumulonimbus (pyroCb) blowups that pollute the stratosphere have been documented on at least five occasions. However, the frequency of these events is still uncertain. One published pyroCb case study, the Chisholm Fire in May 2001, was restricted to the convective phase and its immediate aftermath. Here and in a companion paper we describe the stratospheric impact of the Chisholm pyroCb. The companion paper focuses on nadir satellite views of the plume. This paper synthesizes a broad array of space-, balloon-, and ground-based profile measurements. The Chisholm pyroCb, which we identify as the singular cause of stratospheric aerosol increase in northern spring/ summer of 2001, created a doubling of the zonal average aerosol optical depth in the lowermost stratosphere. The meridional spread of the plume was from the tropics (20°N) to the high Arctic (79°N) within the first month. The stratospheric Chisholm smoke became a hemispheric phenomenon in midlatitudes and northern tropics and persisted for at least 3 months. A size-resolved particle concentration profile over Laramie, Wyoming, indicated a lower stratospheric aerosol with a twofold to threefold increase in volume of particles with radii between 0.3 and 0.6 mm. We also find evidence of localized warming in the air masses of four of the lidar-measured smoke layers. This work contains the first reported stratospheric smoke layers measured by lidar at Ny Å lesund, Esrange, Kühlungsborn, Garmisch-Partenkirchen, Boulder, and Mauna Loa. In addition, the first detection of smoke-enhanced aerosol extinction at near IR wavelengths by the Halogen Occultation Experiment (HALOE) is introduced.