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The Midlatitude Cirrus experiment (ML-CIRRUS) deployed the High Altitude and Long Range Research Aircraft (HALO) to obtain new insights into nucleation, life cycle, and climate impact of natural cirrus and aircraft-induced contrail cirrus. Direct observations of cirrus properties and their variability are still incomplete, currently limiting our understanding of the clouds’ impact on climate. Also, dynamical effects on clouds and feedbacks are not adequately represented in today’s weather prediction models. Here, we present the rationale, objectives, and selected scientific highlights of ML-CIRRUS using the G-550 aircraft of the German atmospheric science community. The first combined in situ–remote sensing cloud mission with HALO united state-of-the-art cloud probes, a lidar and novel ice residual, aerosol, trace gas, and radiation instrumentation. The aircraft observations were accompanied by remote sensing from satellite and ground and by numerical simulations. In spring 2014, HALO performed 16 flights above Europe with a focus on anthropogenic contrail cirrus and midlatitude cirrus induced by frontal systems including warm conveyor belts and other dynamical regimes (jet streams, mountain waves, and convection). Highlights from ML-CIRRUS include 1) new observations of microphysical and radiative cirrus properties and their variability in meteorological regimes typical for midlatitudes, 2) insights into occurrence of in situ–formed and lifted liquid-origin cirrus, 3) validation of cloud forecasts and satellite products, 4) assessment of contrail predictability, and 5) direct observations of contrail cirrus and their distinction from natural cirrus. Hence, ML-CIRRUS provides a comprehensive dataset on cirrus in the densely populated European midlatitudes with the scope to enhance our understanding of cirrus clouds and their role for climate and weather

Abstract. The temporal and spatial distribution of enhanced boundary layer BrO concentrations in both hemispheres during 1997 is presented using observations of the Global Ozone Monitoring Experiment (GOME) on board the European research satellite ERS-2. BrO concentrations (up to 50 ppt) are the major cause for catalytic boundary layer ozone destruction typically observed during polar spring in both hemispheres. While autocatalytic mechanisms are most probably responsible for the release of the observed high concentrations of reactive bromine compounds, uncertainties still remain with respect to the primary release mechanisms and whether the autocatalytic reactions are taking place on sea-salt aerosol or the surface of sea ice. We find that enhanced boundary layer BrO concentrations correlate very well with ozone depletion events. Enhanced BrO concentrations are always found over or near to areas of frozen salt water (above sea ice or also above the frozen surface of the Caspian Sea) consistent with the assumption that such conditions are a prerequisite for the autocatalytic release of high BrO concentrations to the troposphere.

Abstract. Tropospheric NO2 columns derived from the data products of the Global Ozone Monitoring Experiment (GOME), deployed on the ESA ERS-2 satellite, have been compared with model calculations from two global three-dimensional chemistry transport models, IMAGES and MOZART. The main objectives of the study are an analysis of the tropospheric NO2 data derived from satellite measurements, an interpretation of it and evaluation of its quality using global models, and an estimation the role of NO2 in radiative forcing. The measured and modeled NO2 columns show similar spatial and seasonal patterns, with large tropospheric column amounts over industrialized areas and small column amounts over remote areas. The comparison of the absolute values of the measured and modeled tropospheric column amounts are particularly dependent upon uncertainties in the derivation of the tropospheric NO2 columns from GOME and the difficulty of modeling the boundary layer in global models, both of which are discussed below. The measured tropospheric column amounts derived from GOME data are of the same order as those calculated by the MOZART model over the industrialized areas of the United States and Europe, but a factor of 2-3 larger for Asia. The modeled tropospheric NO2 columns from MOZART as well as the column amounts measured by GOME are in good agreement with NO2 columns derived from observed NO2 mixing ratios in the boundary layer in eastern North America. The comparison of the models to the GOME data illustrates the degree to which present models reproduce the hot spots seen in the GOME data.

Abstract. The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated (nine chemical transport models and two chemistry–climate models) by simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993–2012). Except for three model simulations, all others were driven offline by (or nudged to) reanalysed meteorology. The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes. Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA's long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements – including high-altitude observations from the NASA Global Hawk platform. The models generally capture the observed seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model–measurement correlation (r  ≥  0.7) at most sites. In a given model, the absolute model–measurement agreement at the surface is highly sensitive to the choice of emissions. Large inter-model differences are apparent when using the same emission inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve best agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2Br2). In general, the models reproduce observations of CHBr3 and CH2Br2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific well. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr3 (and to a lesser extent CH2Br2) most elevated over the tropical western Pacific during boreal winter. The models also indicate the Asian monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr3 and CH2Br2 of 2.0 (1.2–2.5) ppt,  ∼  57 % larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. The transport-driven interannual variability in the annual mean bromine SGI is of the order of ±5 %, with SGI exhibiting a strong positive correlation with the El Niño–Southern Oscillation (ENSO) in the eastern Pacific. Overall, our results do not show systematic differences between models specific to the choice of reanalysis meteorology, rather clear differences are seen related to differences in the implementation of transport processes in the models.

Abstract. Measurements of OC10 total column amounts by means of the Global OzoneMonitoring Experiment (GOME) instrument conducted in the austral and boreal winter stratospheres from 1995 through 1999 are presented, GOME is a four-channel UV/visible spectrometer (240-790 nm) deployed on the polar orbiting European ERS-2 satellite since April 1995. Previous studies have shown that the observations of OC10, the symmetric chlorine dioxide formed in a side channel of the reaction of BrO + CIO, can serve as an indicator for a stratospheric chlorine activation. GOME's 3-day coverage of the global atmosphere allows us to infer the first global data set of OC10, and to study continuous time series of its occurrence in both winter stratospheres. It is found that, while OC10 regularly occurs over Antarctica in similar amounts and seasonal timing during the different winters, its occurrence is much more variable in the Arctic winter stratosphere, primarily because of the larger dynamic activity that result in warmer temperatures there. About 40% higher OC10 column amounts are found in the Antarctic polar stratosphere than in its northern counterpart, a further indication for a significantly more efficient chlorine activation in the Antarctic than the Arctic late winter and spring stratosphere.

Homogeneous freezing of supercooled droplets occurs in convective systems in low-and in mid-latitudes. This droplet freezing process leads to the formation of a large amount of small ice particles, so called frozen droplets, that are transported to the upper parts of anvil outflows, where they can influence the cloud radiative properties. However, the detailed microphysics and, thus, the scattering properties of these small ice particles are highly uncertain.Here, we investigate the link between the microphysical and optical properties of frozen droplets in cloud chamber experiments, where the frozen droplets were formed, grown and sublimated under controlled conditions. It was found that frozen droplets developed a high degree of small-scale complexity after their initial formation and subsequent growth. During sublimation the smallscale complexity disappeared releasing a smooth and near-spherical ice particle. Angular light scattering and depolarization measurements confirmed that these sublimating frozen droplets scattered light similar to spherical particles, i.e. they had angular light scattering properties similar to water droplets. The knowledge gained from this laboratory study was applied to two case studies of aircraft measurements in a mid-latitude and in a tropical convective systems. The in-situ aircraft measurements confirmed that the microphysics of frozen droplets is dependent on the humidity conditions they are exposed to (growth or sublimation). The existence of optically spherical frozen droplets can be important for the radiative properties of detraining convective outflows.

Examples for the influence of tropospheric clouds on the ground‐based measurement of stratospheric species using the DOAS‐technique (Differential Optical Absorption Spectroscopy) are reported. At Camborne/Great Britain (50.216°N, 5.316°W) on Sept. 11–15, 1994, episodic enhancement of absorption lines of O4, H2O, O3 and NO2 were observed in coincidence with tropospheric clouds being in the instrumental field of view (1.1° full angle). At a solar zenith angle (SZA) of 88°, absorption enhancements up to roughly a factor of 3 were detected for the tropospheric species O4 and H2O and the tropospheric fractions of the total column of O3 and NO2. The additional absorptions in the visible spectral range are probably caused by multiple Mie‐scattering in tropospheric clouds. For our conditions, a tropospheric light path enhancement (TLPE) of 135±40 km can be inferred, being largely independent of SZA. This observation has several important implications for the atmospheric radiative transport, which are briefly discussed.