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In this study ozone profiles of the differential-absorption lidar at Garmisch-Partenkirchen are compared with those of ozone sondes of the Forschungszentrum Jülich and of the Meteorological Observatory Hohenpeißenberg (German Weather Service). The lidar measurements are quality assured by the highly accurate in-situ measurements at nearby the Wank (1780 m a.s.l.) and Zugspitze (2962 m a.s.l.) summits and at the Global Atmosphere Watch station Schneefernerhaus (2670 m a.s.l.). The lidar results agree almost perfectly with those of the monitoring stations. Side-by-side sounding of the lidar and electrochemical (ECC) sonde measurements by a team of the Forschungszentrum Jülich shows just small positive offsets (≤ 3.4 ppb), almost constant within the troposphere. We conclude that the recently published uncertainties of the lidar in the final configuration since 2012 are realistic and rather small for low to moderate ozone. Comparisons with the Hohenpeißenberg routine Brewer-Mast sonde measurements are more demanding because of the distance of 38 km between both sites. These comparisons cover the three years September 2000 to August 2001, 2009 and 2018. A slight negative average offset (-3.64 ppb ± 7.5 ppb (full error)) of the sondes with respect to the lidar is found. Most sonde measurements could be improved in the troposphere by recalibration with the station data. This would not only remove the average offset, but also greatly reduce the variability of the individual offsets. The comparison for 2009 suggests a careful partial re-evaluation of the lidar measurements between 2007 and 2011 for altitudes above 6 km where an occasional negative bias occurred.

The pronounced increase of ozone observed at the Alpine station Zugspitze (2962 m a.s.l.) since the 1970s has been ascribed to an increase of stratospheric air descending to the Alps. In this paper, we present a re-analysis of the data from 1978 to 2011 for both ozone and carbon monoxide, extended until 2020 by the data from the Global Atmosphere Watch site Schneefernerhaus (UFS, 2671 m a.s.l.) just below the Zugspitze summit. The analysis is based on data filtering utilizing the isotope 7Be (measured between 1970 and 2006) and relative humidity (1970 to 2011, UFS: 2002 to 2020). We estimate both the influence of stratospheric intrusions directly descending to the northern rim of the Alps from the full data filtering and the aged (“indirect”) intrusions from partial filtering with the 7Be data. The evaluated total stratospheric contribution to the annual-average ozone rises roughly from 12 ppb in 1970 to 24 ppb in 2003. It turns out that the increase of stratospheric influence is particularly strong in winter. A lowering in positive trend is seen afterwards, almost parallel to the beginning decrease of solar irradiation. The air masses hitting the Zugspitze summit have become drier in the percentile range up to at least 25 % until 2003, and we see the growing stratospheric contribution as an important factor to this drying. Both an increase of lower-stratospheric ozone and a growing width of the intrusion layer departing downward from just above the tropopause must be taken into consideration. Carbon monoxide in intrusions did not change much during the full measurement period 1990 to 2020, with perhaps a slight increase until 2005 and an almost constant behaviour afterwards. This is remarkable since outside intrusions a decrease by approximately 44 % was found, indicating a substantial improvement of the tropospheric air quality.

The Far-Infrared Radiation Mobile Observation System (FIRMOS) is a Fourier transform spectroradiometer developed to support the Far-infrared Outgoing Radiation Understanding and Monitoring (FORUM) satellite mission by validating measurement methods and instrument design concepts, both in the laboratory and in field campaigns. FIRMOS is capable of measuring the downwelling spectral radiance emitted by the atmosphere in the spectral band from 100 to 1000 cm-1 (10–100 µm in wavelength), with a maximum spectral resolution of 0.25 cm-1. We describe the instrument design and its characterisation and discuss the geophysical products obtained by inverting the atmospheric spectral radiance measured during a campaign from the high-altitude location of Mount Zugspitze in Germany, beside the Extended-range Atmospheric Emitted Radiance Interferometer (E-AERI), which is permanently installed at the site. Following the selection of clear-sky scenes, using a specific algorithm, the water vapour and temperature profiles were retrieved from the FIRMOS spectra by applying the Kyoto protocol and Informed Management of the Adaptation (KLIMA) code. The profiles were found in very good agreement with those provided by radiosondes and by the Raman lidar operating from the Zugspitze Schneefernerhaus station. In addition, the retrieval products were validated by comparing the retrieved Integrated Water Vapour values with those obtained from the E-AERI spectra. Finally, we found that the trends for the temperature, and the water vapour profiles over time were in good agreement with those provided by ERA5 reanalysis.

This publisher’s note contains corrections to Appl. Opt. 61, 8553 (2022)APOPAI0003-693510.1364/AO.463257.

We present a design of a transversely pumped and powerful Ti:sapphire laser, suitable for laser remote sensing in the near infrared (NIR) spectrum. Examining multiple pump configurations revealed that transversal pumping of Ti:sapphire crystals with a Nd:YAG laser (532 nm) from one or two sides yields maximum output power. Together with an optimized bow-tie resonator setup, we were able to extract up to 3 W (30 mJ, 100 Hz) of narrowband NIR laser emission from a cuboid 50 mm long Ti:sapphire crystal. Beam quality and divergence were determined as M x 2 = 1.1 , M y 2 = 1.7 , φ x = 0.5 m r a d , and φ y = 0.8 m r a d . The spectral purity (seeded, P s e e d ≥ 170 µ W ) was better than 99.8%. Additionally, we show a two-wavelength setup applicable to atmospheric water vapor lidar. The principle performance of this theory of operation suggests a good chance of scalability towards significantly enhanced power of future Ti:sapphire lasers.

Die Warmebehandlung von Verbundwalzen ist ein kritischer Prozessschritt, in dessen Verlauf aufgrund der unterschiedlichen thermophysikalischen Eigenschaften der verwendeten Werkstoffe grose innere Spannungen auftreten konnen. Ziel dieser Arbeit war die Erstellung eines parametrisierten FE-Modells zur einfachen Abbildung unterschiedlicher Warmebehandlungsprozessfuhrungen mit dem Ziel, neue Werkstoffe und Warmebehandlungsrouten gefahrlos einfuhren und erproben zu konnen. Diese Arbeit prasentiert die experimentellen Vorarbeiten, den Aufbau und Validierung des Simulationsmodells in Bezug auf die Warmeleitungssimulation sowie die Abschatzung der Spannungsentwicklung durch die mechanische Simulation.

Since 1988 two ozone lidar systems have been developed at IMK-IFU (Garmisch-Partenkirchen, Germany). A stationary system, operated at the institute, has yielded about 5000 vertical profiles of ozone from next to the ground to typically 3 km above the tropopause and has contributed data for a large number of scientific investigations. A mobile system was successfully operated in a number of field campaigns after its completion in 1996, before it was destroyed in major flooding in May 1999. Both systems combine a high data quality with high vertical resolution dynamically varied between 50 m in the lower troposphere and 250–500 m below the tropopause (stationary system). The stationary system has been gradually upgraded over the years. The noise level of the raw data has reached a level of about ±1 × 10-6 of the input range of the transient digitizers after minor smoothing. As a consequence, uncertainties of the ozone mixing ratios of 1.5 to 4 ppb have been achieved up to about 5 km. The performance in the upper troposphere, based on the wavelength pair 292 – 313-nm varies between 5 and 15 ppb, depending on the absorption of the 292-nm radiation in ozone and the solar background. In summer it is, therefore, planned to extend the measurement time for 41 s to a few minutes in order to improve the performance. For longer time series automatic data acquisition has been used. The number of measurements per year has been confined to less than 600 since fully automatic data evaluation has, still, had its limitations and some manual actions are needed.

Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 ± 9%) but smaller growth between 1960 and 2000 (approximately 16 ± 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050–2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation.

A semi-implicit (non-)hydrostatic free-surface numerical model for two layer flows is derived from the Navier–Stokes equations by applying kinematic boundary conditions at moving interfaces and by decomposing the pressure into the hydrostatic and the hydrodynamic part. When the latter is ignored, the algorithm conveniently transforms into a solver for a hydrostatic flow. In addition, when the vertical grid spacing is larger than the layer depths, the algorithm naturally degenerates into a solver for the shallow water equations. In this paper, the presented numerical model is developed for the horizontal centrifugal casting, a metallurgical process, in which a liquid metal is poured into a horizontally rotating cylindrical mold. The centrifugal force pushes the liquid metal toward the mold wall resulting in a formation of a sleeve with a uniform thickness. The mold gradually extracts the sensible and the latent heat from the sleeve, which eventually becomes solid. Often a second layer of another material is introduced during the solidification of the first layer. The proposed free-surface model is therefore coupled with the heat advection-diffusion equation with a stiff latent heat source term representing the solidification. The numerical results show a good agreement with measurements of temperatures performed in the plant. A validation of the proposed model is also provided with the help of using other numerical techniques such as the approximate Riemann solver for the two layer shallow water equations and the volume of fluid method.

Six months of stratospheric aerosol observations with the European Aerosol Research Lidar Network (EARLINET) from August 2017 to January 2018 are presented. The decay phase of an unprecedented, record-breaking stratospheric perturbation caused by wildfire smoke is reported and discussed in terms of geometrical, optical, and microphysical aerosol properties. Enormous amounts of smoke were injected into the upper troposphere and lower stratosphere over fire areas in western Canada on 12 August 2017 during strong thunderstorm–pyrocumulonimbus activity. The stratospheric fire plumes spread over the entire Northern Hemisphere in the following weeks and months. Twenty-eight European lidar stations from northern Norway to southern Portugal and the eastern Mediterranean monitored the strong stratospheric perturbation on a continental scale. The main smoke layer (over central, western, southern, and eastern Europe) was found at heights between 15 and 20 km since September 2017 (about 2 weeks after entering the stratosphere). Thin layers of smoke were detected at heights of up to 22–23 km. The stratospheric aerosol optical thickness at 532 nm decreased from values > 0.25 on 21–23 August 2017 to 0.005–0.03 until 5–10 September and was mainly 0.003–0.004 from October to December 2017 and thus was still significantly above the stratospheric background (0.001–0.002). Stratospheric particle extinction coefficients (532 nm) were as high as 50–200 Mm−1 until the beginning of September and on the order of 1 Mm−1 (0.5– 5 Mm−1 ) from October 2017 until the end of January 2018. The corresponding layer mean particle mass concentration was on the order of 0.05–0.5 µg m−3 over these months. Soot particles (light-absorbing carbonaceous particles) are efficient ice-nucleating particles (INPs) at upper tropospheric (cirrus) temperatures and available to influence cirrus formation when entering the tropopause from above. We estimated INP concentrations of 50–500 L−1 until the first days in September and afterwards 5–50 L−1 until the end of the year 2017 in the lower stratosphere for typical cirrus formation temperatures of −55 ◦C and an ice supersaturation level of 1.15. The measured profiles of the particle linear depolarization ratio indicated a predominance of nonspherical smoke particles. The 532 nm depolarization ratio decreased slowly with time in the main smoke layer from values of 0.15–0.25 (August–September) to values of 0.05–0.10 (October–November) and < 0.05 (December–January). The decrease of the depolarization ratio is consistent with aging of the smoke particles, growing of a coating around the solid black carbon core (aggregates), and thus change of the shape towards a spherical form. We found ascending aerosol layer features over the most southern European stations, especially over the eastern Mediterranean at 32–35◦ N, that ascended from heights of about 18–19 to 22–23 km from the beginning of October to the beginning of December 2017 (about 2 km per month). We discuss several transport and lifting mechanisms that may have had an impact on the found aerosol layering structures.

The atmospheric composition is strongly influenced by a change in atmospheric dynamics, which is potentially related to climate change. A prominent example is the doubling of the stratospheric ozone component at the Zugspitze summit station (2962 m a.s.l., Garmisch-Partenkirchen, Germany) between the mid-seventies and 2005, roughly from 11 to 23 ppb (43 %). Systematic efforts for identifying and quantifying this influence have been made since the late 1990s. Meanwhile, routine lidar measurements of ozone and water vapour carried out at Garmisch-Partenkirchen (German Alps) since 2007, combined with in situ and radiosonde data and trajectory calculations, have revealed that stratospheric intrusion layers are present on 84 % of the yearly measurement days. At Alpine summit stations the frequency of intrusions exhibits a seasonal cycle with a pronounced summer minimum that is reproduced by the lidar measurements. The summer minimum disappears if one looks at the free troposphere as a whole. The mid- and upper-tropospheric intrusion layers seem to be dominated by very long descent on up to hemispheric scale in an altitude range starting at about 4.5 km a.s.l. Without interfering air flows, these layers remain very dry, typically with RH ≤5 % at the centre of the intrusion. Pronounced ozone maxima observed above Garmisch-Partenkirchen have been mostly related to a stratospheric origin rather than to long-range transport from remote boundary layers. Our findings and results for other latitudes seem to support the idea of a rather high contribution of ozone import from the stratosphere to tropospheric ozone., Atmospheric Chemistry and Physics, 20 (1), ISSN:1680-7375, ISSN:1680-7367

International audience; Six months of stratospheric aerosol observations with the European Aerosol Research Lidar Network (EARLINET) from August 2017 to January 2018 are presented. The decay phase of an unprecedented, record-breaking stratospheric perturbation caused by wildfire smoke is reported and discussed in terms of geometrical, optical, and microphysical aerosol properties. Enormous amounts of smoke were injected into the upper troposphere and lower stratosphere over fire areas in western Canada on 12 August 2017 during strong thunderstorm-pyrocumulonimbus activity. The stratospheric fire plumes spread over the entire Northern Hemisphere in the following weeks and months. Twenty-eight European lidar stations from northern Norway to southern Portugal and the eastern Mediterranean monitored the strong stratospheric perturbation on a continental scale. The main smoke layer (over central, western, southern, and eastern Europe) was found at heights between 15 and 20 km since September 2017 (about 2 weeks after entering the stratosphere). Thin layers of smoke were detected at heights of up to 22-23 km. The stratospheric aerosol optical thickness at 532 nm decreased from values > 0.25 on 21-23 August 2017 to 0.005-0.03 until 5-10 September and was mainly 0.003-0.004 from October to December 2017 and thus was still significantly above the stratospheric background (0.001-0.002). Stratospheric particle extinction coefficients (532 nm) were as high as 50-200 Mm-1 until the beginning of September and on the order of 1 Mm-1 (0.5-5 Mm-1) from October 2017 until the end of January 2018. The corresponding layer mean particle mass concentration was on the order of 0.05-0.5 µg m-3 over these months. Soot particles (light-absorbing carbonaceous particles) are efficient ice-nucleating particles (INPs) at upper tropospheric (cirrus) temperatures and available to influence cirrus formation when entering the tropopause from above. We estimated INP concentrations of 50-500 L-1 until the first days in September and afterwards 5-50 L-1 until the end of the year 2017 in the lower stratosphere for typical cirrus formation temperatures of -55 ∘C and an ice supersaturation level of 1.15. The measured profiles of the particle linear depolarization ratio indicated a predominance of nonspherical smoke particles. The 532 nm depolarization ratio decreased slowly with time in the main smoke layer from values of 0.15-0.25 (August-September) to values of 0.05-0.10 (October-November) and < 0.05 (December-January). The decrease of the depolarization ratio is consistent with aging of the smoke particles, growing of a coating around the solid black carbon core (aggregates), and thus change of the shape towards a spherical form. We found ascending aerosol layer features over the most southern European stations, especially over the eastern Mediterranean at 32-35∘ N, that ascended from heights of about 18-19 to 22-23 km from the beginning of October to the beginning of December 2017 (about 2 km per month). We discuss several transport and lifting mechanisms that may have had an impact on the found aerosol layering structures.

From the earliest observations of ozone in the lower atmosphere in the 19th century, both measurement methods and the portion of the globe observed have evolved and changed. These methods have different uncertainties and biases, and the data records differ with respect to coverage (space and time), information content, and representativeness. In this study, various ozone measurement methods and ozone datasets are reviewed and selected for inclusion in the historical record of background ozone levels, based on relationship of the measurement technique to the modern UV absorption standard, absence of interfering pollutants, representativeness of the well-mixed boundary layer and expert judgement of their credibility. There are significant uncertainties with the 19th and early 20th-century measurements related to interference of other gases. Spectroscopic methods applied before 1960 have likely underestimated ozone by as much as 11% at the surface and by about 24% in the free troposphere, due to the use of differing ozone absorption coefficients. There is no unambiguous evidence in the measurement record back to 1896 that typical mid-latitude background surface ozone values were below about 20 nmol mol–1, but there is robust evidence for increases in the temperate and polar regions of the northern hemisphere of 30–70%, with large uncertainty, between the period of historic observations, 1896–1975, and the modern period (1990–2014). Independent historical observations from balloons and aircraft indicate similar changes in the free troposphere. Changes in the southern hemisphere are much less. Regional representativeness of the available observations remains a potential source of large errors, which are difficult to quantify. The great majority of validation and intercomparison studies of free tropospheric ozone measurement methods use ECC ozonesondes as reference. Compared to UV-absorption measurements they show a modest (~1–5% ±5%) high bias in the troposphere, but no evidence of a change with time. Umkehr, lidar, and FTIR methods all show modest low biases relative to ECCs, and so, using ECC sondes as a transfer standard, all appear to agree to within one standard deviation with the modern UV-absorption standard. Other sonde types show an increase of 5–20% in sensitivity to tropospheric ozone from 1970–1995. Biases and standard deviations of satellite retrieval comparisons are often 2–3 times larger than those of other free tropospheric measurements. The lack of information on temporal changes of bias for satellite measurements of tropospheric ozone is an area of concern for long-term trend studies.

The thermodynamic modeling of alloy systems consisting of stable and metastable phases e.g. high-alloyed mottled cast iron can be problematic. Thermodynamic databases are rather well-developed for low, medium and high alloyed steels (e.g. HSS) but the application of those databases is not yet very common for high-alloyed (mottled) cast irons. The Thermo-Calc software together with the TCFE7 database is used to calculate isopleth and property diagrams, using the CALPHAD method. Additionally Scheil-Gulliver calculations are performed to simulate the effects of microsegregation during solidification. The results from the thermodynamic calculations are compared with measurements on own samples and with literature values. Those measurements include quantitative light-optical analysis, SEM with BSE detector, EDX measurements for the distribution of the alloying elements as well as XRD and DSC measurements. The investigations show the possibilities which are offered by thermodynamic calculations for high-alloyed mottled cast iron as well as the limitations and the compromises which have to be taken into account when calculating stable and metastable phases existing next to each other.

A standardized approach for the definition, propagation, and reporting of uncertainty in the ozone differential absorption lidar data products contributing to the Network for the Detection for Atmospheric Composition Change (NDACC) database is proposed. One essential aspect of the proposed approach is the propagation in parallel of all independent uncertainty components through the data processing chain before they are combined together to form the ozone combined standard uncertainty. The independent uncertainty components contributing to the overall budget include random noise associated with signal detection, uncertainty due to saturation correction, background noise extraction, the absorption cross sections of O3, NO2, SO2, and O2, the molecular extinction cross sections, and the number densities of the air, NO2, and SO2. The expression of the individual uncertainty components and their step-by-step propagation through the ozone differential absorption lidar (DIAL) processing chain are thoroughly estimated. All sources of uncertainty except detection noise imply correlated terms in the vertical dimension, which requires knowledge of the covariance matrix when the lidar signal is vertically filtered. In addition, the covariance terms must be taken into account if the same detection hardware is shared by the lidar receiver channels at the absorbed and non-absorbed wavelengths. The ozone uncertainty budget is presented as much as possible in a generic form (i.e., as a function of instrument performance and wavelength) so that all NDACC ozone DIAL investigators across the network can estimate, for their own instrument and in a straightforward manner, the expected impact of each reviewed uncertainty component. In addition, two actual examples of full uncertainty budget are provided, using nighttime measurements from the tropospheric ozone DIAL located at the Jet Propulsion Laboratory (JPL) Table Mountain Facility, California, and nighttime measurements from the JPL stratospheric ozone DIAL located at Mauna Loa Observatory, Hawai'i.

Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

The atmospheric composition is strongly influenced by changing atmospheric dynamics, in potential relation to climate change. A prominent example is the doubling of the stratospheric ozone component at the summit station Zugspitze (2962 m a.s.l., Garmisch-Partenkirchen, Germany) between the mid-seventies and 2005, roughly from 11 ppb to 23 ppb (43 %). Systematic efforts for identifying and quantifying this influence have been made since the late 1990s. Meanwhile, routine lidar measurements of ozone and water vapour carried out since 2007, combined with in-situ and radiosonde data and trajectory calculations, have revealed the presence of stratospheric intrusion layers on 84 % of the yearly measurement days. The seasonal cycle for deep intrusions with a pronounced summer minimum seen at Alpine summit stations disappears if one looks at the entire free troposphere. The seasonal cycle previously obtained for the Zugspitze summit is rather well reproduced by the lidar data. The mid- and upper-tropospheric intrusion layers seem to be dominated by very long downward transport up to a full tour around the northern hemisphere in an altitude range starting at about 4.5 km a.s.l. Unless there is a strong perturbation, these layers remain considerably dry, typically with RH &leq; 5 % at the centre of the intrusion. It is interesting to note that, in recent years, most pronounced ozone maxima have been related to a stratospheric origin rather than to long-range transport from remote boundary layers. This fact could be caused by improving air quality in the most relevant source regions or changing transport patterns.

Since its first establishment in 2000, EARLINET (European Aerosol Research Lidar NETwork) has been devoted to providing, through its database, exclusively quantitative aerosol properties, such as aerosol backscatter and aerosol extinction coefficients, the latter only for stations able to retrieve it independently (from Raman or High Spectral Resolution Lidars). As these coefficients are provided in terms of vertical profiles, EARLINET database must also include the details on the range resolution of the submitted data. In fact, the algorithms used in the lidar data analysis often alter the spectral content of the data, mainly working as low pass filters with the purpose of noise damping. Low pass filters are mathematically described by the Digital Signal Processing (DSP) theory as a convolution sum. As a consequence, this implies that each filter's output, at a given range (or time) in our case, will be the result of a linear combination of several lidar input data relative to different ranges (times) before and after the given range (time): a first hint of loss of resolution of the output signal. The application of filtering processes will also always distort the underlying true profile whose relevant features, like aerosol layers, will then be affected both in magnitude and in spatial extension. Thus, both the removal of noise and the spatial distortion of the true profile produce a reduction of the range resolution. This paper provides the determination of the effective resolution (ERes) of the vertical profiles of aerosol properties retrieved starting from lidar data. Large attention has been addressed to provide an assessment of the impact of low-pass filtering on the effective range resolution in the retrieval procedure.

Water vapor is the most important greenhouse gas and its spatiotemporal variability strongly exceeds that of all other greenhouse gases. However, this variability has hardly been studied quantitatively so far. We present an analysis of a 5-year period of water vapor measurements in the free troposphere above the Zugspitze (2962 m a.s.l., Germany). Our results are obtained from a combination of measurements of vertically integrated water vapor (IWV), recorded with a solar Fourier transform infrared (FTIR) spectrometer on the summit of the Zugspitze and of water vapor profiles recorded with the nearby differential absorption lidar (DIAL) at the Schneefernerhaus research station. The special geometrical arrangement of one zenith-viewing and one sun-pointing instrument and the temporal resolution of both instruments allow for an investigation of the spatiotemporal variability of IWV on a spatial scale of less than 1 km and on a timescale of less than 1 h. The standard deviation of differences between both instruments σIWV calculated for varied subsets of data serves as a measure of variability. The different subsets are based on various spatial and temporal matching criteria. Within a time interval of 20 min, the spatial variability becomes significant for horizontal distances above 2 km, but only in the warm season (σIWV =0.35 mm). However, it is not sensitive to the horizontal distance during the winter season. The variability of IWV within a time interval of 30 min peaks in July and August (σIWV > 0.55 mm, mean horizontal distance = 2.5 km) and has its minimum around midwinter (σIWV < 0.2 mm, mean distance > 5 km). The temporal variability of IWV is derived by selecting subsets of data from both instruments with optimal volume matching. For a short time interval of 5 min, the variability is 0.05 mm and increases to more than 0.5 mm for a time interval of 15 h. The profile variability of water vapor is determined by analyzing subsets of water vapor profiles recorded by the DIAL within time intervals from 1 to 5 h. For all altitudes, the variability increases with widened time intervals. The lowest relative variability is observed in the lower free troposphere around an altitude of 4.5 km. Above 5 km, the relative variability increases continuously up to the tropopause by about a factor of 3. Analysis of the covariance of the vertical variability reveals an enhanced variability of water vapor in the upper troposphere above 6 km. It is attributed to a more coherent flow of heterogeneous air masses, while the variability at lower altitudes is also driven by local atmospheric dynamics. By studying the short-term variability of vertical water vapor profiles recorded within a day, we come to the conclusion that the contribution of long-range transport and the advection of heterogeneous layer structures may exceed the impact of local convection by 1 order of magnitude even in the altitude range between 3 and 5 km.

This paper presents stratospheric aerosol climate records developed in the framework of the Aerosol_cci project, one of the 14 parallel projects from the ESA Climate Change Initiative. These data records were processed from a stratospheric aerosol dataset derived from the GOMOS experiment, using an inversion algorithm optimized for aerosol retrieval, called AerGOM. They provide a suite of aerosol parameters, such as the aerosol extinction coefficient at different wavelengths in the UV-visible range.The extinction record includes the total extinction as well as separate fields for liquid sulfate aerosols and polar stratospheric clouds (PSCs). Several additional fields (PSC flag, etc.) are also provided. The resulting stratospheric aerosol dataset, which spans the whole duration of the GOMOS mission (2002-2012), was validated using different reference datasets (lidar and balloon profiles). In the present paper, the emphasis is put on the extinction records. After a thorough analysis of the original AerGOM dataset, we describe the methodology used to construct the gridded CCI-GOMOS dataset and the resulting improvements on both the AerGOM algorithm and the binning procedure, in terms of spatio-temporal resolution, coverage and data quality. The extinction datasets were validated using lidar profiles from three ground-based stations (Mauna Loa, Garmisch-Partenkirchen, Dumont d'Urville). The median difference of the CCI-GOMOS (Level 3) extinction and ground-based lidar profiles is between similar to 15% and similar to 45% in the 16-21 km altitude range, depending on the considered site and aerosol type. The CCI-GOMOS dataset was subsequently used, together with a MIPAS SO2 time series, to update a volcanic eruption inventory published previously, thus providing a more comprehensive list of eruptions for the ENVISAT period (2002-2012). The number of quantified eruptions increases from 102 to 230 in the updated inventory. This new inventory was used to simulate the evolution of the global radiative forcing by application of the EMAC chemistry-climate model. Results of this simulation improve the agreement between modelled global radiative forcing of stratospheric aerosols at about 100 hPa compared to values estimated from observations. Medium eruptions like the ones of Soufriere Hills/Rabaul (2006), Sarychev (2009) and Nabro (2011) cause a forcing change from about -0.1 W/m(2) to -0.2 W/m(2). (C) 2017 The Authors. Published by Elsevier Inc.

Critical data selection is essential for determining representative baseline levels of atmospheric trace gas measurements even at remote measuring sites. Different data selection techniques have been used around the world which could potentially lead to bias when comparing data from different stations. This paper presents a novel statistical data selection method based on CO2 diurnal pattern occurring typically at high elevated mountain stations. Its capability and applicability was studied for atmospheric measuring records of CO2 from 2010 to 2016 at six Global Atmosphere Watch (GAW) stations in Europe, namely Zugspitze-Schneefernerhaus (Germany), Sonnblick (Austria), Jungfraujoch (Switzerland), Izaña (Spain), Schauinsland (Germany) and Hohenpeissenberg (Germany). Three other frequently applied statistical data selection methods were implemented for comparison. Among all selection routines, the new method named Adaptive Baseline Finder (ABF) resulted in lower selection percentages with lower maxima during winter and higher minima during summer in the selected data. To investigate long-term trend and seasonality, seasonal decomposition technique STL was applied. Compared with the unselected data, mean annual growth rates of all selected data sets were not significantly different except for Schauinsland. However, clear differences were found in the annual amplitudes as well as for the seasonal time structure. Based on correlation analysis, results by ABF selection showed a better representation of the lower free tropospheric conditions.

We present vertical soundings (2005–2015) of tropospheric water vapor (H2O) and its D/H isotope ratio (δD) at Mt. Zugspitze (47° N, 11° E, 2964 m a.s.l.) derived from ground-based solar Fourier transform infrared (FTIR) measurements. Beside water vapor profiles with optimized vertical resolution (degrees of freedom for signal DOFS = 2.8), the retrieval provides {H2O, δD} pairs with consistent vertical resolution (DOFS = 1.6 for H2O and δD) applied in this study. The integrated water vapor (IWV) trend of 2.4 [−5.8, 10.6] % per decade (statistically insignificant, 95 % confidence interval) can be reconciled with the 2005–2015 temperature increase at Mt. Zugspitze (1.3 [0.5, 2.1] K per decade) assuming constant relative humidity. Seasonal variations in free-tropospheric H2O and δD exhibit amplitudes of 140 % and 50 % of the respective overall means. The minima (maxima) in January (July) are in agreement with changing sea surface temperature of the Atlantic Ocean. Using extensive backward trajectory analysis, distinct moisture pathways are identified depending on observed δD levels: low column-based δD values (δDcol < 5th percentile) are associated with air masses originating in higher latitudes (62° N on average) and altitudes (6.5 km) compared to high δD values (δDcol > 95th percentile: 46° N, 4.6 km). Backward trajectory classification indicates that {H2O, δD} observations are influenced by three long-range transport patterns towards Mt. Zugspitze assessed in previous studies: (i) intercontinental transport from North America (TUS; source region: 25–45° N, 70–110° W, 0–2 km altitude), (ii) intercontinental transport from Northern Africa (TNA; source region: 15–30° N, 15° W–35° E, 0–2 km altitude), and (iii) stratospheric air intrusions (STI; source region: > 20° N, above zonal mean tropopause). The FTIR data exhibit significantly differing signatures in free-tropospheric {H2O, δD} pairs (given as mean with uncertainty of ±2 standard errors) for TUS (VMRH2O = 2.4 [2.3, 2.6] × 103 ppmv, δD = −315 [−326, −303] ‰), TNA (2.8 [2.6, 2.9] × 103 ppmv, −251 [−257, −246] ‰), and STI (1.2 [1.1, 1.3] × 103 ppmv, −384 [−397, −372] ‰). For TUS events, {H2O, δD} observations depend on surface temperature in the source region and the degree of dehydration having occurred during updraft in warm conveyor belts. During TNA events (dry convection of boundary layer air) relatively moist and weakly HDO-depleted air masses are imported. In contrast, STI events are associated to import of predominantly dry and HDO-depleted air masses. These long-range transport patterns potentially involve the import of various trace constituents to the Central European free troposphere, i.e., import of pollution from North America (e.g., aerosol, ozone, carbon monoxide), Saharan mineral dust, stratospheric ozone and other airborne species such as pollen. Our above results provide evidence that {H2O, δD} observations are a valuable proxy for the potential transport of such tracers. To validate this finding, we consult a data base of transport events (TNA and STI) covering 2013–2015 deduced by data filtering from in situ measurements at Mt. Zugspitze and lidar profiles at near-by Garmisch. Indeed, the FTIR data related to these verified TNA events (27 days) exhibit characteristic fingerprints in IWV (5.5 [4.9, 6.1] mm) and δDcol (−266 [−284, −247] ‰), which are significantly distinguishable from the rest of the time series (4.3 [4.1, 4.5] mm, −316 [−324, −308] ‰). This holds true on 1-σ level for 136 STI days (mean ± 1 standard error: 4.2 [4.0, 4.3] mm, −322 [−327, −316] ‰) with respect to the remainder (4.6 [4.5, 4.8] mm, −302 [−307, −297] ‰). Furthermore, deep stratospheric intrusions to the Zugspitze summit (in situ humidity and beryllium-7 data filtering) show a significantly lower mean value (−334 [−337, −330] ‰) of lower-tropospheric δD (3–5 km a.s.l.) on 2-σ level than the rest of the 2005–2015 time series (−284 [−286, −282] ‰). Our results show that consistent {H2O, δD} observations at Mt. Zugspitze can serve as an operational indicator for long-range transport events potentially affecting regional climate, air quality, as well as human health in Central Europe.

Preliminary attempts of quantifying the stratospheric ozone contribution in the observations at the Zugspitze summit (2962 m a.s.l.) next to Garmisch-Partenkirchen 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 7Be 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., Atmospheric Chemistry and Physics, 14 (18), ISSN:1680-7375, ISSN:1680-7367

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.

A large-scale comparison of water-vapour vertical-sounding instruments took place over central Europe on 17 October 2008, during a rather homogeneous deep stratospheric intrusion event (LUAMI, Lindenberg Upper-Air Methods Intercomparison). The measurements were carried out at four observational sites: Payerne (Switzerland), Bilthoven (the Netherlands), Lindenberg (north-eastern Germany), and the Zugspitze mountain (Garmisch-Partenkichen, German Alps), and by an airborne water-vapour lidar system creating a transect of humidity profiles between all four stations. A high data quality was verified that strongly underlines the scientific findings. The intrusion layer was very dry with a minimum mixing ratios of 0 to 35ppm on its lower west side, but did not drop below 120ppm on the higher-lying east side (Lindenberg). The dryness hardens the findings of a preceding study (“Part 1”, Trickl et al., 2014) that, e.g., 73% of deep intrusions reaching the German Alps and travelling 6 days or less exhibit minimum mixing ratios of 50ppm and less. These low values reflect values found in the lowermost stratosphere and indicate very slow mixing with tropospheric air during the downward transport to the lower troposphere. The peak ozone values were around 70ppb, confirming the idea that intrusion layers depart from the lowermost edge of the stratosphere. The data suggest an increase of ozone from the lower to the higher edge of the intrusion layer. This behaviour is also confirmed by stratospheric aerosol caught in the layer. Both observations are in agreement with the idea that sections of the vertical distributions of these constituents in the source region were transferred to central Europe without major change. LAGRANTO trajectory calculations demonstrated a rather shallow outflow from the stratosphere just above the dynamical tropopause, for the first time confirming the conclusions in “Part 1” from the Zugspitze CO observations. The trajectories qualitatively explain the temporal evolution of the intrusion layers above the four stations participating in the campaign., Atmospheric Chemistry and Physics, 16 (14), ISSN:1680-7375, ISSN:1680-7367

A standardized approach for the definition and reporting of vertical resolution of the ozone and temperature lidar profiles contributing to the Network for the Detection for Atmospheric Composition Change (NDACC) database is proposed. Two standardized definitions homogeneously and unequivocally describing the impact of vertical filtering are recommended. The first proposed definition is based on the width of the response to a finite-impulse-type perturbation. The response is computed by convolving the filter coefficients with an impulse function, namely, a Kronecker delta function for smoothing filters, and a Heaviside step function for derivative filters. Once the response has been computed, the proposed standardized definition of vertical resolution is given by Δz = δz × HFWHM, where δz is the lidar's sampling resolution and HFWHM is the full width at half maximum (FWHM) of the response, measured in sampling intervals. The second proposed definition relates to digital filtering theory. After applying a Laplace transform to a set of filter coefficients, the filter's gain characterizing the effect of the filter on the signal in the frequency domain is computed, from which the cut-off frequency fC, defined as the frequency at which the gain equals 0.5, is computed. Vertical resolution is then defined by Δz = δz∕(2fC). Unlike common practice in the field of spectral analysis, a factor 2fC instead of fC is used here to yield vertical resolution values nearly equal to the values obtained with the impulse response definition using the same filter coefficients. When using either of the proposed definitions, unsmoothed signals yield the best possible vertical resolution Δz = δz (one sampling bin). Numerical tools were developed to support the implementation of these definitions across all NDACC lidar groups. The tools consist of ready-to-use “plug-in” routines written in several programming languages that can be inserted into any lidar data processing software and called each time a filtering operation occurs in the data processing chain. When data processing implies multiple smoothing operations, the filtering information is analytically propagated through the multiple calls to the routines in order for the standardized values of vertical resolution to remain theoretically and numerically exact at the very end of data processing.

Routine high-quality lidar measurements of ozone, water vapour and aerosol at Garmisch-Partenkirchen since 2007 have made possible more comprehensive atmospheric studies and lead to a growing insight concerning the most frequently occurring long-range transport pathways. In this contribution we present as examples results on stratospheric layers travelling in the free troposphere for extended periods of time without eroding. In particular, we present a case of an intrusion layer that subsided over as many as fifteen days and survived the interference by strong Canadian fires. These results impose a challenge on atmospheric modelling that grossly overestimates free-tropospheric mixing.

A high-power Raman lidar system has been installed at the high-altitude research station Schneefernerhaus (Garmisch-Partenkirchen, Germany) at 2675 m a.s.l., at the side of the existing wide-range differrential-absorption lidar. An industrial XeCl laser was modified for polarized single-line operation at an average power of about 175 W. This high power and a 1.5-m-diameter receiver are expected to allow us to extend the operating range for water-vapour sounding to more than 25 km, at an accuracy level of the order of 10 %. In addition, temperature measurements in the free troposphere and to altitudes beyond 80 km are planned. The system is currently thoroughly tested and exhibits an excellent performance up to the lowermost stratosphere. We expect that results for higher altitudes can be presented at the meeting.

We report on the free tropospheric spatio-temporal variability of water vapor investigated by the analysis of a five-year period of water vapor vertical soundings above Mt. Zugspitze (2962 m a.s.l., Germany). Our results are obtained from a combination of measurements of vertically integrated water vapor (IWV), recorded with a solar Fourier Transform InfraRed (FTIR) spectrometer and of water vapor profiles recorded with the nearby differential absorption lidar (DIAL). The special geometrical arrangement of one zenith-viewing and one sun-pointing instrument and the temporal resolution of both optical instruments allow for an investigation of the spatiotemporal variability of IWV on a spatial scale of less than one kilometer and on a time scale of less than one hour. We investigated the short-term variability of both IWV and water vapor profiles from statistical analyses. The latter was also examined by case studies with a clear assignment to certain atmospheric processes as local convection or long-range transport. This study is described in great detail in our recent publication [1]. 1. INSTRUMENTATION AND GEOGRAPHICAL ARRANGEMENT The Zugspitze (47:42 ◦ N, 10:98 ◦ E, 2962 m a.s.l.) is by far the highest mountain on the northern rim of the Alps. The free troposphere above this site is representative of Central Europe. The mountain is above the moist boundary layer for most of the year. Due to reduced absorption losses this site is ideal for sensitive spectroscopic measurements of water vapor throughout the free troposphere. While the FTIR instrument is located on the summit of Mt. Zugspitze the DIAL instrument is located at the Schneefernerhaus research station (UFS) on the steep southern slope of Mt. Zugspitze at an altitude of 2675 m a.s.l., 680 m southwest of the FTIR instrument (Fig. 1). The solar FTIR instrument uses direct radiation from the sun in the mid-infrared as light source (Table). The instrument provides water vapor columns integrated along its slanted viewline towards the sun with a precision better than 0.05 mm. It is based on a Bruker IFS125HR interferometer and is described in detail by [2].

Specific very dry high-ozone layers, starting roughly two days after the onset of high-pressure periods during the warm season, have been reproducibly observed in the middle and upper troposphere with the ozone lidar in Garmisch-Partenkirchen (Germany). These episodes, previously not understood, were recently analysed based on extending backward simulations with the FLEXPART particle dispersion model to as many as twenty days and on jet-stream analyses including calculations with the LAGRANTO transport model. In all six cases analysed the model results indicate ozone import from the stratosphere on an extremely long path along the subtropical jet stream over the Pacific Ocean, Asia and, in part, all the way back to the Atlantic Ocean. The analysis suggests that stratospheric influence is the most important factor for the increase in ozone and is related to rather shallow transfer of air from the stratosphere into the upper- and mid-tropospheric air streams observed with the lidar. Contributions from the boundary layers of East Asia and North America are just occasionally present, in one case documented by a very dense aerosol plume from the Asian deserts. The considerable vertical and temporal extent of many of these layers and peak ozone mixing ratios between 80 and 150 ppb suggest that the observations are related to an important mechanism for stratosphere-to-troposphere transport (STT) and also confirm the model predictions of pronounced and persistent STT along the subtropical jet stream., Atmospheric Chemistry and Physics, 11 (17), ISSN:1680-7375, ISSN:1680-7367

We describe the development and application of a differentially pumped pulsed cold H2 and (H2)2 beam source. The nozzle was cooled with liquid nitrogen and, actuated by a piezoelectric valve with pressures up to 5 bar, produced gas pulses 250 μs long. Strong limitations by collisions with the fast hydrogen molecules returning from the walls of the source chamber could be overcome by surrounding the volume around nozzle and skimmer with cold surfaces. As a consequence, the beam intensities for both the monomer and the clusters could be greatly enhanced. The valve was operated without any realignment for more than one year. The beam source was characterized by a number of photo-ionization studies. As a part of these efforts the presumably first laser-based single-photon ionization spectra of H2 and (H2)2 were obtained. We estimate that more than ten $\mathrm{H}_{3}^{+}$ ions could be detected per laser shot at a wavelength of 74.2 nm and a pressure of 5 bar. The auto-ionization lines of H2 were recorded with a resolution of about 0.54 cm−1. A line width of about 629 MHz was obtained in the B←X band system of hydrogen observed by resonance-enhanced two-photon ionization. Further potential improvements of the experiment are discussed.