Abstract. Through measurements of NO2, O3 and NO3 during the PARADE campaign (PArticles and RAdicals, Diel observations of mEchanisms of oxidation) in the German Taunus mountains we derive nighttime steady-state lifetimes (τss) of NO3 and N2O5. During some nights, high NO3 (∼ 200 pptv) and N2O5 (∼ 1 ppbv) mixing ratios were associated with values of τss that exceeded 1 h for NO3 and 3 h for N2O5 near the ground. Such long boundary-layer lifetimes for NO3 and N2O5 are usually only encountered in very clean/unreactive air masses, whereas the PARADE measurement site is impacted by both biogenic emissions from the surrounding forest and anthropogenic emissions from the nearby urbanised/industrialised centres. Measurement of several trace gases which are reactive towards NO3 indicates that the inferred lifetimes are significantly longer than those calculated from the summed loss rate. Several potential causes for the apparently extended NO3 and N2O5 lifetimes are examined, including additional routes to formation of NO3 and the presence of a low-lying residual layer. Overall, the most likely cause of the anomalous lifetimes are related to the meteorological conditions, though additional NO3 formation due to reactions of Criegee intermediates may contribute.

Airborne trace gas, microphysical, and radiation measurements were performed during the AIRcraft TOwed Sensor Shuttle -Inhomogeneous Cirrus Experiment over northern Germany in 2013. Based on high-precision nitrous oxide (N 2 O) and carbon monoxide (CO) in situ data, stratospheric air could be identified, which contained cirrus cloud particles. Consistent with the stratospheric N 2 O data, backward trajectories indicate that the sampled air masses crossed the dynamical tropopause in the last 3 h before the measurement. These air masses contained cirrus particles, which were formed during slow ascent in the troposphere and subsequently mixed with stratospheric air. From the CO-N 2 O correlation the irreversibility of this transport is deduced. To our knowledge, this is the first in situ detection of cirrus particles mixed with stratospheric air in the midlatitudes.

IAGOS (In-service Aircraft for a Global Observing System) performs long-term routine in situ observations of atmospheric chemical composition (O, CO, NO, NO, CO, CH), water vapour, aerosols, clouds, and temperature on a global scale by operating compact instruments on board of passenger aircraft. The unique characteristics of the IAGOS data set originate from the global scale sampling on air traffic routes with similar instrumentation such that the observations are truly comparable and well suited for atmospheric research on a statistical basis. Here, we present the analysis of 15 months of simultaneous observations of relative humidity with respect to ice (RH) and ice crystal number concentration in cirrus (N) from July 2014 to October 2015. The joint data set of 360 hours of RH-N observations in the global upper troposphere and tropopause region is analysed with respect to the in-cloud distribution of RH and related cirrus properties. The majority of the observed cirrus is thin with N < 0.1 cm. The respective fractions of all cloud observations range from 90% over the mid-latitude North Atlantic Ocean and the Eurasian Continent to 67% over the subtropical and tropical Pacific Ocean. The in-cloud RH distributions do not depend on the geographical region of sampling. Types of cirrus origin (in situ origin, liquid origin) are inferred for different N regimes and geographical regions. Most importantly, we found that in-cloud RH shows a strong correlation to N with slightly supersaturated dynamic equilibrium RH associated with higher N values in stronger updrafts.

This study presents the analysis of the structure and air mass characteristics of the lower atmosphere during the field campaign PARADE (PArticles and RAdicals: Diel observations of the impact of urban and biogenic Emissions) on Mount Kleiner Feldberg in southwestern Germany during late summer 2011. We analysed measurements of meteorological variables (temperature, moisture, pressure, wind speed and direction) from radio soundings and of chemical tracers (carbon dioxide, ozone) from aircraft measurements. We focus on the thermodynamic and dynamic properties that control the chemical distribution of atmospheric constituents in the boundary layer. We show that the evolution of tracer profiles of CO2 and O-3 indicate mixing across the inversion layer (or entrainment zone). This finding is supported by the analysis of tracer-tracer correlations which are indicative for mixing and the relation of tracer profiles in relation to the evolution of the boundary layer height deduced from radio soundings. The study shows the relevance of entrainment processes for the lower troposphere in general and specifically that the tracer-tracer correlation method can be used to identify mixing and irreversible exchange processes across the inversion layer

Abstract. The vertical distribution and seasonal variation of water vapour volume mixing ratio (H2O VMR), of relative humidity with respect to ice (RHice) and particularly of regions with ice-supersaturated air masses (ISSRs) in the extratropical upper troposphere and lowermost stratosphere are investigated at northern mid-latitudes over the eastern North American, North Atlantic and European regions for the period 1995 to 2010. Observation data originate from regular and continuous long-term measurements on board instrumented passenger aircraft in the framework of the European research programme MOZAIC (1994–2010), which continues as the European research infrastructure IAGOS (from 2011). Data used in our study result from collocated observations of O3 VMR, RHice and temperature, as well as H2O VMR deduced from RHice and temperature data. The in situ observations of H2O VMR and RHice with a vertical resolution of 30 hPa (< 750 m at the extratropical tropopause level) and a horizontal resolution of 1 km resolve detailed features of the distribution of water vapour and ice-supersaturated air relative to the thermal tropopause, including their seasonal and regional variability and chemical signatures at various distances from the tropopause layer. Annual cycles of the investigated properties document the highest H2O VMR and temperatures above the thermal tropopause in the summer months, whereas RHice above the thermal tropopause remains almost constant in the course of the year. Over all investigated regions, upper tropospheric air masses close to the tropopause level are nearly saturated with respect to ice and contain a significant fraction of ISSRs with a distinct seasonal cycle of minimum values in summer (30 % over the ocean, 20 %–25 % over land) and maximum values in late winter (35 %–40 % over both land and ocean). Above the thermal tropopause, ISSRs are occasionally observed with an occurrence probability of 1.5 ± 1.1 %, whereas above the dynamical tropopause at 2 PVU (PVU: potential vorticity unit), the occurrence probability increases 4-fold to 8.4 ± 4.4 %. In both coordinate systems related to tropopause height (TPH), the ISSR occurrence probabilities drop to values below 1 % for the next higher air mass layer with pressure levels p < pTPH−15 hPa. For both tropopause definitions, the tropospheric nature or fingerprint, based on O3 VMR, indicates the continuing tropospheric influence on ISSRs inside and above the respective tropopause layer. For the non-ISSRs, however, the stratospheric nature is clearly visible above the thermal tropopause, whereas above the dynamical tropopause the air masses show a still substantial tropospheric influence. For all three regions, seasonal deviations from the long-term annual cycle of ISSR occurrence show no significant trends over the observation period of 15 years, whereas a statistically significant correlation between the North Atlantic Oscillation (NAO) index and the deviation of ISSR occurrence from the long-term average is observed for the North Atlantic region but not for the eastern North American and European regions.

Abstract. Despite several studies on temperature trends in the tropopause region, a comprehensive understanding of the evolution of temperatures in this climate-sensitive region of the atmosphere remains elusive. Here we present a unique global-scale, long-term data set of high-resolution in situ temperature data measured aboard passenger aircraft within the European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System; http: //www.iagos.org). This data set is used to investigate temperature trends within the global upper troposphere and lowermost stratosphere (UTLS, < 13 km) for the period of 1995-2012 in different geographical regions and vertical layers of the UTLS. The largest number of observations is available over the North Atlantic. Here, a neutral temperature trend is found within the lowermost stratosphere. This contradicts the temperature trend in the European Centre for MediumRange Weather Forecasts (ECMWF) ERA-Interim reanalysis, in which a significant (95 % confidence) temperature increase of +0.56 K decade −1 is found. Differences between trends derived from observations and reanalysis data can be traced back to changes in the temperature difference between observation and model data over the period studied. This study underpins the value of the IAGOS temperature observations as an anchor point for the evaluation of reanalyses and its suitability for independent trend analyses.

Abstract. The vertical distribution and seasonal variation of upper tropospheric humidity (UTH) and particularly of ice-supersaturated air masses in the extratropical upper troposphere and lowermost stratosphere (Ex-UTLS) is investigated at northern mid-latitudes over the regions Eastern North America, the North Atlantic and Europe for the period 1995 to 2010. Observation data originate from regular and continuous long-term measurements of water vapour volume mixing ratio (H2O VMR), temperature and relative humidity with respect to ice (RHice) by instrumented passenger aircraft in the framework of the European research program MOZAIC (1994–2010) which is continued as European research infrastructure IAGOS (from 2011). The in-situ observations of UTH with a vertical resolution of 30 hPa (

Abstract. We describe the nitrogen oxide instrument designed for the autonomous operation on board passenger aircraft in the framework of the European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System). We demonstrate the performance of the instrument using data from two deployment periods aboard an A340-300 aircraft of Deutsche Lufthansa. The well-established chemiluminescence detection method is used to measure nitrogen monoxide (NO) and nitrogen oxides (NO x ). NO x is measured using a photolytic converter, and nitrogen dioxide (NO 2 ) is determined from the difference between NO x and NO. This technique allows measuring at high time resolution (4 s) and high precision in the low ppt range (NO: 2σ = 24 pptv; NO x : 2σ = 35 pptv) over different ambient temperature and ambient pressure altitude ranges (from surface pressure down to 190 hPa). The IAGOS NO x instrument is characterized for (1) calibration stability and total uncertainty, (2) humidity and chemical interferences (e.g., ozone; nitrous acid, HONO; peroxyacetyl nitrate, PAN) and (3) inter-instrumental precision. We demonstrate that the IA-GOS NO x instrument is a robust, fully automated, and longterm stable instrument suitable for unattended operation on airborne platforms, which provides useful measurements for future air quality studies and emission estimates.