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Nitrous oxide (N2O) is the third most important greenhouse gas modified by human activities after carbon dioxide and methane. This study examines the feasibility of airborne differential absorption lidar to measure N2O concentration enhancements over agricultural, fossil fuel combustion, industrial, and biomass burning sources. The mid-infrared spectral region, where suitably strong N2O absorption lines exist, challenges passive remote sensing by means of spectroscopy due to both low solar radiation and thermal emission. Lidar remote sensing is principally possible thanks to the laser as an independent radiation source but has not yet been realized due to technological challenges. Mid-infrared N2O absorption bands suitable for remote sensing are investigated. Simulations show that a spectral trough position between two strong N2O lines in the 4.5 µm band is the favored option. A second option exists in the 3.9 µm band at the cost of higher laser frequency stability constraints and less measurement sensitivity. Both options fulfill the N2O measurement requirements for agricultural areal or point-source emission quantification (0.5 % measurement precision, 500 m spatial resolution) with technically realizable and affordable transmitter (100 mW average laser power) and receiver (20 cm telescope) characteristics for integrated-path differential absorption lidar that measures the column concentration beneath the aircraft. The development of an airborne N2O lidar is feasible yet would benefit from progress in infrared laser transmitter and low-noise-detection technology. It will also serve as a precursor to space versions, which are still out of reach due to the lack of space technology.

Global warming is amplified in the Arctic. However, numerical models struggle to represent key processes that determine Arctic weather and climate. To collect data that help to constrain the models, the HALO–(𝒜𝒞)3 aircraft campaign was conducted over the Norwegian and Greenland seas, the Fram Strait, and the central Arctic Ocean in March and April 2022. The campaign focused on one specific challenge posed by the models, namely the reasonable representation of transformations of air masses during their meridional transport into and out of the Arctic via northward moist- and warm-air intrusions (WAIs) and southward marine cold-air outbreaks (CAOs). Observations were made over areas of open ocean, the marginal sea ice zone, and the central Arctic sea ice. Two low-flying and one long-range, high-altitude research aircraft were flown in colocated formation whenever possible. To follow the air mass transformations, a quasi-Lagrangian flight strategy using trajectory calculations was realized, enabling us to sample the same moving-air parcels twice along their trajectories. Seven distinct WAI and 12 CAO cases were probed. From the quasi-Lagrangian measurements, we have quantified the diabatic heating/cooling and moistening/drying of the transported air masses. During CAOs, maximum values of 3 K h−1 warming and 0.3 g kg−1 h−1 moistening were obtained below 1 km altitude. From the observations of WAIs, diabatic cooling rates of up to 0.4 K h−1 and a moisture loss of up to 0.1 g kg−1 h−1 from the ground to about 5.5 km altitude were derived. Furthermore, the development of cloud macrophysical (cloud-top height and horizontal cloud cover) and microphysical (liquid water path, precipitation, and ice index) properties along the southward pathways of the air masses were documented during CAOs, and the moisture budget during a specific WAI event was estimated. In addition, we discuss the statistical frequency of occurrence of the different thermodynamic phases of Arctic low-level clouds, the interaction of Arctic cirrus clouds with sea ice and water vapor, and the characteristics of microphysical and chemical properties of Arctic aerosol particles. Finally, we provide a proof of concept to measure mesoscale divergence and subsidence in the Arctic using data from dropsondes released during the flights.

Warm-air intrusions (WAIs) are responsible for the transportation of warm and moist air masses from the mid-latitudes into the high Arctic (> 70° N). In this work, we study cirrus clouds that form during WAI events (WAI cirrus) and during undisturbed Arctic conditions (AC cirrus) and investigate possible differences between the two cloud types based on their macrophysical and optical properties with a focus on relative humidity over ice (RHi). We use airborne measurements from the combined high-spectral-resolution and differential-absorption lidar, WALES, performed during the HALO-(AC)3 campaign. We classify each research flight and the measured clouds as either AC or WAI, based on the ambient conditions, and study the macrophysical, geometrical and optical characteristics for each cirrus group. As our main parameter we choose the relative humidity over ice (RHi), which we calculate RHi by combining the lidar water vapor measurements with model temperatures. Ice formation occurs at certain RHi values depending on the dominant nucleation process taking place. RHi can thus be used as an indication of the nucleation process and the structure of cirrus clouds. We find that during WAI events the Arctic is warmer and moister and WAI cirrus clouds are both geometrically and optically thicker compared to AC cirrus. WAI cirrus clouds and the layer directly surrounding them are more frequently supersaturated, also at high supersaturations over the threshold for homogeneous ice nucleation (HOM). AC cirrus clouds have a supersaturation-dominated cloud top and a subsaturated cloud base. WAI cirrus clouds also have high supersaturations at cloud top but also at cloud base.

Aviation has a large impact on the Earth's atmosphere and climate by various processes. Line-shaped contrails and contrail cirrus clouds lead to changes in the natural cirrus cloud cover and have a major contribution to the effective radiative forcing from aviation. In addition, aviation-induced aerosols might also change the microphysical properties and optical properties of naturally formed cirrus clouds. Latter aerosol–cloud interactions show large differences in the resulting effective radiative forcing, and our understanding on how aviation-induced aerosols affect cirrus cloud properties is still poor. Up to now, observations of this aviation-induced aerosol effect have been rare. In this study, we use combined airborne lidar and in situ ice cloud measurements to investigate differences in the microphysical and optical properties of naturally formed cirrus clouds, which formed in regions that are highly affected by aviation-induced aerosol emissions and, of those, which formed in regions rather unaffected by aviation. Urbanek et al. (2018) showed that those cirrus clouds, which are more affected by aviation-induced soot emission, are characterized by larger values of the particle linear depolarization ratio (PLDR). In this follow-on study we relate collocated lidar measurements performed aboard HALO during the ML-CIRRUS mission of the particle linear depolarization ratio with in situ cloud probe measurements of the number concentration and effective diameter of the ice particles. In situ measurements for both cloud types (high-PLDR-mode – aviation-affected – and low-PLDR-mode – pristine – cirrus) can be reliably compared in a temperature range between 210 and 215 K. Within this temperature range we find that high-PLDR-mode cirrus clouds tend to show larger effective ice particle diameters with a median value of 61.4 compared to 50.7 µm for low-PLDR-mode pristine cirrus clouds. Larger effective ice particles in aviation-influenced (high-PLDR-mode) cirrus are connected to lower ice particle number concentration with a median value of 0.05 compared to 0.11 cm−3 (low-PLDR-mode), which evolved in more pristine regions with only little impact from aviation. We suspect that a suppression of homogeneous ice formation by the heterogeneously freezing soot aerosol particles included in the areas affected by air traffic is the cause of the reduced ice crystal concentrations.

Water vapor measurements of midlatitude cirrus clouds, obtained by the WAter vapour Lidar Experiment in Space (WALES) lidar system during the Mid-Latitude Cirrus (ML-CIRRUS) airborne campaign, which took place in the spring of 2014 over central Europe and the NE Atlantic Ocean, are combined with model temperatures from the European Centre for Medium-Range Weather Forecasts (ECMWF) and analyzed. Our main focus is to derive the distribution and temporal evolution of humidity with respect to ice within cirrus clouds and in their adjacent cloud-free air. We find that 34.1 % of in-cloud data points are supersaturated with respect to ice. Supersaturation is also detected in 6.8 % of the cloud-free data points. When the probability density of the relative humidity over ice (RHi) is calculated with respect to temperature for the in-cloud data points from the ML-CIRRUS dataset, there are two peaks: one around 225 K and close to saturation, RHi = 100 %, and a second one at colder temperatures around 218 K in subsaturation, RHi = 79 %. These two regions seem to represent two cirrus cloud categories: in situ formed and liquid origin. Regarding their vertical structure, most clouds have higher supersaturations close to the cloud top and become subsaturated near the cloud bottom. Finally, we find that the vertical structure of RHi within the clouds is also indicative of their life stage. RHi skewness tends to go from positive to negative values as the cloud ages. RHi modes are close to saturation in young clouds, supersaturated in mature clouds and subsaturated in dissipating clouds.

Contrail cirrus constitute the largest radiative forcing (RF) component to the total aviation effect on climate. However, the microphysical properties and radiative effects of contrail cirrus and natural cirrus clouds in the same meteorological conditions are still not completely resolved. Motivated by these uncertainties, we investigate an extended cirrus region perturbed by aviation in the North Atlantic region (NAR) on 26 March 2014 during the Midlatitude Cirrus (ML-CIRRUS) experiment. On that day, high air traffic density in the NAR combined with large scale cold and humid ambient conditions favored the formation of a contrail cirrus outbreak situation. In addition, low coverage by low-level water clouds and the homogeneous oceanic albedo increased the sensitivity for retrieving cirrus properties and their radiative effect from satellite remote sensing. This allowed us to extend the current knowledge on contrail cirrus by combining airborne in situ, lidar and satellite observations. In the synoptic context of a ridge cirrus, an extended thin ice cloud with many persistent contrails and contrail cirrus has been observed for many hours with the geostationary Meteosat Second Generation (MSG)/Spinning Enhanced Visible and InfraRed Imager (SEVIRI) from the early morning hours until dissipation after noon. Airborne lidar observations aboard the German High Altitude and LOng Range Research Aircraft (HALO) suggest that this cirrus has a significant anthropogenic contribution from aviation. A new method based on in situ measurements was used to distinguish between contrails, contrail cirrus and natural cirrus based on ice number and gas phase NO concentrations. Results show that contrail effective radii (Reff) reach at most 11 µm, while contrail cirrus Reff can be as large as 51 µm. Contrail and contrail cirrus mean Reff is 18 % smaller than that of natural cirrus. We find that a difference in Reff between contrail cirrus and natural cirrus survives in this contrail cirrus outbreak event. As for radiative effects, a new method to estimate top-of-atmosphere instantaneous RF in the solar and thermal range is developed based on radiative transfer model simulations exploiting in situ and lidar measurements, satellite observations and ERA5 reanalysis data for both cirrus and cirrus-free regions. Broadband irradiances estimated from our simulations compare well with satellite observations from MSG, indicating that our method provides a good representation of the real atmosphere and can thus be used to determine the RF of ice clouds. For a larger spatial area around the flight path, we find that the contrail cirrus outbreak is warming in the early morning and cooling during the day. The methods presented here and the results will be valuable for future research to constrain uncertainties in the assessment of radiative impacts of contrail cirrus and natural cirrus and for the formulation and evaluation of contrail mitigation options.

During a research flight of the Wave-driven ISentropic Exchange (WISE) campaign, which was conducted over the eastern North Atlantic on 1 October 2017, the composition of the upper troposphere and lower stratosphere (UTLS) across the North Atlantic jet stream was observed by airborne, range-resolved differential absorption lidar (DIAL) profiles. We investigate how the high variability in the paired H2O and O3 distribution along the two-dimensional lidar cross section is affected by synoptic-scale weather systems, as revealed by the Lagrangian history of the observed air masses. To this aim, the lidar observations are combined with 10 d backward trajectories along which meteorological parameters and derived turbulence diagnostics are traced. The transport and mixing characteristics are then projected to the vertical cross sections of the lidar measurements and to the H2O–O3 phase space to explore linkages with the evolution of synoptic-scale weather systems and their interaction. Tropical, midlatitude, and arctic weather systems in the region of the jet stream and the related transport and mixing explain the complex H2O and O3 distribution to a large extent: O3-rich stratospheric air from the high Arctic interacts with midlatitude air from the North Pacific in a northward-deflected jet stream associated with an anticyclone over the US and forms a filament extending into the tropopause fold beneath the jet stream. In the troposphere, lifting related to convection in the intertropical convergence zone (ITCZ) and two tropical cyclones that continuously injected H2O into dry descending air from the tropical Atlantic and Pacific form filamentary H2O structures. One tropical cyclone that transitioned into a midlatitude cyclone lifted moist boundary layer air, explaining the highest tropospheric H2O values. During the two days before the observations, the air with mixed tropospheric and stratospheric characteristics experienced frequent turbulence along the North Atlantic jet stream, indicating a strong influence of turbulence on the formation of the extratropical transition layer (ExTL). This investigation highlights the complexity of stirring and mixing processes and their close connection to interacting tropospheric weather systems from the tropics to the polar regions, which strongly influenced the observed fine-scale H2O and O3 distributions. The identified non-local character of mixing should be kept in mind when interpreting mixing lines in tracer–tracer phase space diagrams.

Numerical weather prediction (NWP) models are known to possess a distinct moist bias in the mid-latitude lower stratosphere, which is expected to affect the ability to accurately predict weather and climate. This paper investigates the vertical structure of the moist bias in the European Centre for Medium-Range Weather Forecasts (ECMWF) latest global reanalysis ERA5 using a unique multi-campaign data set of highly resolved water vapour profiles observed with a differential absorption lidar (DIAL) on board the High Altitude and LOng range research aircraft (HALO). In total, 41 flights in the mid-latitudes from six field campaigns provide roughly 33 000 profiles with humidity varying by 4 orders of magnitude. The observations cover different synoptic situations and seasons and thus are suitable to characterize the strong vertical gradients of moisture in the upper troposphere and lower stratosphere (UTLS). The comparison to ERA5 indicates high positive and negative deviations in the UT, which on average lead to a slightly positive bias (15 %–20 %). In the LS, the moist bias rapidly increases up to a maximum of 55 % at 1.3 km altitude above the thermal tropopause (tTP) and decreases again to 15 %–20 % at 4 km altitude. Such a vertical structure is frequently observed, although the magnitude varies from flight to flight. The layer depth of increased moist bias is smaller at high tropopause altitudes and larger when the tropopause is low. Our results also suggest a seasonality of the moist bias, with the maximum in summer exceeding autumn by up to a factor of 3. During one field campaign, collocated ozone and water vapour profile observations enable a classification of tropospheric, stratospheric, and mixed air using water vapour–ozone correlations. It is revealed that the moist bias is high in the mixed air while being small in tropospheric and stratospheric air, which highlights that excessive transport of moisture into the LS plays a decisive role for the formation of the moist bias. Our results suggest that a better representation of mixing processes in NWP models could lead to a reduced LS moist bias that, in turn, may lead to more accurate weather and climate forecasts. The lower-stratospheric moist bias should be borne in mind for climatological studies using reanalysis data.

Wintertime Saharan dust plumes in the vicinity of Barbados are investigated by means of airborne lidar measurements. The measurements were conducted in the framework of the EUREC4A (Elucidating the Role of Cloud-Circulation Coupling in Climate) field experiment upstream the Caribbean island in January–February 2020. The combination of the water vapor differential absorption and high spectral resolution lidar techniques together with dropsonde measurements aboard the German HALO (High Altitude and Long-Range) research aircraft enable a detailed vertical and horizontal characterization of the measured dust plumes. In contrast to summertime dust transport, mineral dust aerosols were transported at lower altitudes and were always located below 3.5 km. Calculated backward trajectories affirm that the dust-laden layers have been transported in nearly constant low-level altitude over the North Atlantic Ocean. Only mixtures of dust particles with other aerosol species, i.e., biomass-burning aerosol from fires in West Africa and marine aerosol, were detected by the lidar. No pure mineral dust regimes were observed. Additionally, all the dust-laden air masses that were observed during EUREC4A came along with enhanced water vapor concentrations compared with the free atmosphere above. Such enhancements have already been observed during summertime and were found to have a great impact on radiative transfer and atmospheric stability.

We develop a new method to describe the total cloud cover including optically thin clouds in trade wind cumulus cloud fields. Climate models and large eddy simulations commonly underestimate the cloud cover, while estimates from observations largely disagree on the cloud cover in the trades. Currently, trade wind clouds significantly contribute to the uncertainty in climate sensitivity estimates derived from model perturbation studies. To simulate clouds well, especially how they change in a future climate, we have to know how cloudy it is. In this study we develop a method to quantify the cloud cover from a cloud-free perspective. Using well-known radiative transfer relations we retrieve the cloud-free contribution in high-resolution satellite observations of trade cumulus cloud fields during EUREC4A. Knowing the cloud-free part, we can investigate the remaining cloud-related contributions consisting of areas detected by common cloud-masking algorithms and undetected areas related to optically thin clouds. We find that the cloud-mask cloud cover underestimates the total cloud cover by 33 %. Aircraft lidar measurements support our findings by showing a high abundance of optically thin clouds during EUREC4A. Mixing the undetected optically thin clouds into the cloud-free signal can cause an underestimation of the cloud radiative effect of up to −7.5 %. We further discuss possible artificial correlations in aerosol–cloud cover interaction studies that might arise from undetected optically thin low clouds. Our analysis suggests that the known underestimation of trade wind cloud cover and simultaneous overestimation of cloud brightness in models are even higher than assumed so far.

3D printing allows the fabrication of complex microstructures that would traditionally require specialized machinery. In the fabrication of textiles, 3D printing may enable unique yarn structures, greater manufacturing flexibility and facilitate the development of personalized and tunable devices. In literature, 3D printed textiles have not been subjected to a thorough mechanical characterization. In this paper, a generative model of 3D printed biaxial weaves is developed and a parametric study to effectively map the design parameters to the weaves’ mechanical properties is performed via a two-stage Design-of-Experiments methodology. The samples are printed with material jetting layer by layer in planar direction and destructively tested in tension to obtain the resulting stress–strain behavior. The stress–strain curves are approximated by a bilinear model characterized predominantly by a transition strain and the major modulus after transition. The transition strain is influenced by the load direction and the weave pattern, while the major modulus is impacted by the load direction, the yarn diameter, the weave pattern and the yarn spacing in descending order. Further evaluation of the fracture behavior shows a mitigation of layer-wise delamination. This result indicates that material jetting can enable the production of arbitrary, quasi-continuous textile structures. The characterization results presented here may pave the way towards the design of textiles with spatially varying mechanical properties.

As part of the EUREC4A (Elucidating the role of cloud–circulation coupling in climate) field campaign, the German research aircraft HALO (High Altitude and Long Range Research Aircraft), configured as a cloud observatory, conducted 15 research flights in the trade-wind region east of Barbados in January and February 2020. Narrative text, aircraft state data, and metadata describing HALO's operation during the campaign are provided. Each HALO research flight is segmented by timestamp intervals into standard elements to aid the consistent analysis of the flight data. Photographs from HALO's cabin and animated satellite images synchronized with flight tracks are provided to visually document flight conditions. As a comprehensive product from the remote sensing observations, a multi-sensor cloud mask product is derived and quantifies the incidence of clouds observed during the flights. In addition, to lower the threshold for new users of HALO's data, a collection of use cases is compiled into an online book, How to EUREC4A, included as an asset with this paper. This online book provides easy access to most of EUREC4A's HALO data through an intake catalogue. Code and data are freely available at the locations specified in Table 6.

Laser cooling of single atoms in optical tweezers is a prerequisite for neutral atom quantum computing and simulation. Resolved sideband cooling comprises a well-established method for efficient motional ground-state preparation, but typically requires careful cancellation of light shifts in so-called magic traps. Here, we study a novel laser cooling scheme which overcomes such constraints, and applies when the ground state of a narrow cooling transition is trapped stronger than the excited state. We demonstrate our scheme, which exploits sequential addressing of red sideband transitions via frequency chirping of the cooling light, at the example of ^{88}Sr atoms and report ground-state populations compatible with recent experiments in magic tweezers. The scheme also induces light-assisted collisions, which are key to the assembly of large atom arrays. Our work enriches the toolbox for tweezer-based quantum technology, also enabling applications for tweezer-trapped molecules and ions that are incompatible with resolved sideband cooling conditions.

The science guiding the EUREC4A campaign and its measurements is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced ground-based cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement.

Ice clouds and their effect on earth's radiation budget are one of the largest sources of uncertainty in climate change predictions. The uncertainty in predicting ice cloud feedbacks in a warming climate arises due to uncertainties in measuring and explaining their current optical and microphysical properties as well as from insufficient knowledge about their spatial and temporal distribution. This knowledge can be significantly improved by active remote sensing, which can help to explore the vertical profile of ice cloud microphysics, such as ice particle size and ice water content. This study focuses on the well-established variational approach VarCloud to retrieve ice cloud microphysics from radar–lidar measurements. While active backscatter retrieval techniques surpass the information content of most passive, vertically integrated retrieval techniques, their accuracy is limited by essential assumptions about the ice crystal shape. Since most radar–lidar retrieval algorithms rely heavily on universal mass–size relationships to parameterize the prevalent ice particle shape, biases in ice water content and ice water path can be expected in individual cloud regimes. In turn, these biases can lead to an erroneous estimation of the radiative effect of ice clouds. In many cases, these biases could be spotted and corrected by the simultaneous exploitation of measured solar radiances. The agreement with measured solar radiances is a logical prerequisite for an accurate estimation of the radiative effect of ice clouds. To this end, this study exploits simultaneous radar, lidar, and passive measurements made on board the German High Altitude and Long Range Research Aircraft. By using the ice clouds derived with VarCloud as an input to radiative transfer calculations, simulated solar radiances are compared to measured solar radiances made above the actual clouds. This radiative closure study is done using different ice crystal models to improve the knowledge of the prevalent ice crystal shape. While in one case aggregates were capable of reconciling radar, lidar, and solar radiance measurements, this study also analyses a more problematic case for which no radiative closure could be achieved. In this case, collocated in situ measurements indicate that the lack of closure may be linked to unexpectedly high values of the ice crystal number density.

The composition of the extratropical transition layer (ExTL), which is the transition zone between the stratosphere and the troposphere in the midlatitudes, largely depends on dynamical processes fostering the exchange of air masses. The Wave-driven ISentropic Exchange (WISE) field campaign in 2017 aimed for a better characterization of the ExTL in relation to the dynamic situation. This study investigates the potential of the first-ever collocated airborne lidar observations of ozone (O3) and water vapor (H2O) across the tropopause to depict the complex trace gas distributions and mixing in the ExTL. A case study of a perpendicular jet stream crossing with a coinciding strongly sloping tropopause is presented that was observed during a research flight over the North Atlantic on 1 October 2017. The collocated and range-resolved lidar data that are applied to established tracer–tracer (T–T) space diagnostics prove to be suitable to identify the ExTL and to reveal distinct mixing regimes that enabled a subdivision of mixed and tropospheric air. A back projection of this information to geometrical space shows remarkably coherent structures of these air mass classes along the cross section. This represents the first almost complete observation-based two-dimensional (2D) illustration of the shape and composition of the ExTL and a confirmation of established conceptual models. The trace gas distributions that represent typical H2O and O3 values for the season reveal tropospheric transport pathways from the tropics and extratropics that have influenced the ExTL. Although the combined view of T–T and geometrical space does not inform about the process, location and time of the mixing event, it gives insight into the formation and interpretation of mixing lines. A mixing factor diagnostic and a consideration of data subsets show that recent quasi-instantaneous isentropic mixing processes impacted the ExTL above and below the jet stream which is a confirmation of the well-established concept of turbulence-induced mixing in strong wind shear regions. At the level of maximum winds reduced mixing is reflected in jumps in T–T space that occurred over small horizontal distances along the cross section. For a better understanding of the dynamical and chemical discontinuities at the tropopause, the lidar data are illustrated in isentropic coordinates. The strongest gradients of H2O and O3 are found to be better represented by a potential vorticity-gradient-based tropopause compared to traditional dynamical tropopause definitions using constant potential vorticity values. The presented 2D lidar data are considered to be of relevance for the investigation of further meteorological situations leading to mixing across the tropopause and for future validation of chemistry and numerical weather prediction models.

Anthropogenic point sources, such as coal-fired power plants, produce a major share of global CO2 emissions. International climate agreements demand their independent monitoring. Due to the large number of point sources and their global spatial distribution, the implementation of a satellite-based observation system is convenient. Airborne active remote sensing measurements demonstrate that the deployment of lidar is promising in this respect. The integrated path differential absorption lidar CHARM-F is installed on board an aircraft in order to detect weighted column-integrated dry-air mixing ratios of CO2 below the aircraft along its flight track. During the Carbon Dioxide and Methane Mission (CoMet) in spring 2018, airborne greenhouse gas measurements were performed, focusing on the major European sources of anthropogenic CO2 emissions, i.e., large coal-fired power plants. The flights were designed to transect isolated exhaust plumes. From the resulting enhancement in the CO2 mixing ratios, emission rates can be derived via the cross-sectional flux method. On average, our results roughly correspond to reported annual emission rates, with wind speed uncertainties being the major source of error. We observe significant variations between individual overflights, ranging up to a factor of 2. We hypothesize that these variations are mostly driven by turbulence. This is confirmed by a high-resolution large eddy simulation that enables us to give a qualitative assessment of the influence of plume inhomogeneity on the cross-sectional flux method. Our findings suggest avoiding periods of strong turbulence, e.g., midday and afternoon. More favorable measurement conditions prevail during nighttime and morning. Since lidars are intrinsically independent of sunlight, they have a significant advantage in this regard.

We examine the capability of near-spherical-shaped particles to reproduce the triple-wavelength particle linear depolarization ratio (PLDR) and lidar ratio (LR) values measured over Europe for stratospheric smoke originating from Canadian wildfires. The smoke layers were detected both in the troposphere and the stratosphere, though in the latter case the particles presented PLDR values of almost 18 % at 532 nm as well as a strong spectral dependence from the UV to the near-IR wavelength. Although recent simulation studies of rather complicated smoke particle morphologies have shown that heavily coated smoke aggregates can produce large PLDR, herein we propose a much simpler model of compact near-spherical smoke particles. This assumption allows for the reproduction of the observed intensive optical properties of stratospheric smoke, as well as their spectral dependence. We further examine whether an extension of the current Aerosol Robotic Network (AERONET) scattering model to include the near-spherical shapes could be of benefit to the AERONET retrieval for stratospheric smoke cases associated with enhanced PLDR. Results of our study illustrate the fact that triple-wavelength PLDR and LR lidar measurements can provide us with additional insight when it comes to particle characterization.

The radiative effect of long-range-transported Saharan air layers is investigated on the basis of simultaneous airborne high-spectral-resolution and differential-absorption lidar measurements in the vicinity of Barbados. Within the observed Saharan air layers, increased water vapor concentrations compared to the dry trade wind atmosphere are found. The measured profiles of aerosol optical properties and water vapor mixing ratios are used to characterize the atmospheric composition in radiative transfer calculations, to calculate radiative effects of moist Saharan air layers and to determine radiative heating rate profiles. An analysis based on three case studies reveals that the observed enhanced amounts of water vapor within Saharan air layers have a much stronger impact on heating rate calculations than mineral dust aerosol. Maximum mineral dust short-wave heating and long-wave cooling rates are found at altitudes of highest dust concentration (short wave: +0.5 K d−1; long wave: −0.2 K d−1; net: +0.3 K d−1). However, when considering both aerosol concentrations and measured water vapor mixing ratios in radiative transfer calculations, the maximum heating/cooling rates shift to the top of the dust layer (short wave: +2.2 K d−1; long wave: −6.0 to −7.0 K d−1; net: −4.0 to −5.0 K d−1). Additionally, the net heating rates decrease with height – indicating a destabilizing effect in the dust layers. Long-wave counter-radiation of Saharan air layers is found to reduce cooling at the tops of the subjacent marine boundary layers and might lead to less convective mixing in these layers. The overall short-wave radiative effect of mineral dust particles in Saharan air layers indicates a maximum magnitude of −40 W m−2 at surface level and a maximum of −25 W m−2 at the top of the atmosphere.

The Next-generation Aircraft Remote-Sensing for Validation Studies (NARVAL) aimed at providing a better understanding of shallow marine trade wind clouds and their interplay with long-range-transported elevated Saharan dust layers over the subtropical North Atlantic Ocean. Two airborne campaigns were conducted – the first one in December 2013 (winter) and the second one in August 2016, the latter one during the peak season of transatlantic Saharan dust transport (summer). In this study airborne lidar measurements in the vicinity of Barbados performed during both campaigns are used to investigate possible differences between shallow marine cloud macro-physical properties in dust-free regions and regions comprising elevated Saharan dust layers as well as between different seasons. The cloud top height distribution derived in dust-laden regions differs from the one derived in dust-free regions and indicates that there are less and shallower clouds in the dust-laden than in dust-free trades. Additionally, a clear shift of the distribution to higher altitudes is observed in the dust-free winter season, compared to the summer season. While during the summer season most cloud tops are observed in heights ranging from 0.5 to 1.0 km, most cloud tops in winter season are detected between 2.0 and 2.5 km. Moreover, it is found that regions comprising elevated Saharan dust layers show a larger fraction of small clouds and larger cloud-free regions, compared to dust-free regions. The cloud fraction in the dust-laden summer trades is only 14 % compared to a fraction of 31 % and 37 % in dust-free trades and the winter season. Dropsonde measurements show that long-range-transported Saharan dust layers come along with two additional inversions which counteract convective development, stabilize the stratification and may lead to a decrease in convection in those areas. Moreover, a decreasing trend of cloud fractions and cloud top heights with increasing dust layer vertical extent as well as aerosol optical depth is found.

Liquid water path (LWP) is an important quantity to characterize clouds. Passive microwave satellite sensors provide the most direct estimate on a global scale but suffer from high uncertainties due to large footprints and the superposition of cloud and precipitation signals. Here, we use high spatial resolution airborne microwave radiometer (MWR) measurements together with cloud radar and lidar observations to better understand the LWP of warm clouds over the tropical North Atlantic. The nadir measurements were taken by the German High Altitude and LOng range research aircraft (HALO) in December 2013 (dry season) and August 2016 (wet season) during two Next-generation Advanced Remote sensing for VALidation (NARVAL) campaigns. Microwave retrievals of integrated water vapor (IWV), LWP, and rainwater path (RWP) are developed using artificial neural network techniques. A retrieval database is created using unique cloud-resolving simulations with 1.25 km grid spacing. The IWV and LWP retrievals share the same eight MWR frequency channels in the range from 22 to 31 GHz and at 90 GHz as their sole input. The RWP retrieval combines active and passive microwave observations and is able to detect drizzle and light precipitation. The comparison of retrieved IWV with coincident dropsondes and water vapor lidar measurements shows root-mean-square deviations below 1.4 kg m−2 over the range from 20 to 60 kg m−2. This comparison raises the confidence in LWP retrievals which can only be assessed theoretically. The theoretical analysis shows that the LWP error is constant with 20 g m−2 for LWP below 100 g m−2. While the absolute LWP error increases with increasing LWP, the relative one decreases from 20 % at 100 g m−2 to 10 % at 500 g m−2. The identification of clear-sky scenes by ancillary measurements, here backscatter lidar, is crucial for thin clouds (LWP < 12 g m−2) as the microwave retrieved LWP uncertainty is higher than 100 %. The analysis of both campaigns reveals that clouds were more frequent (47 % vs. 30 % of the time) in the dry than in the wet season. Their average LWP (63 vs. 40 g m−2) and RWP (6.7 vs. 2.7 g m−2) were higher as well. Microwave scattering of ice, however, was observed less frequently in the dry season (0.5 % vs. 1.6 % of the time). We hypothesize that a higher degree of cloud organization on larger scales in the wet season reduces the overall cloud cover and observed LWP. As to be expected, the observed IWV clearly shows that the dry season is on average less humid than the wet season (28 vs. 41 kg m−2). The results reveal that the observed frequency distributions of IWV are substantially affected by the choice of the flight pattern. This should be kept in mind when using the airborne observations to carefully mediate between long-term ground-based and spaceborne measurements to draw statistically sound conclusions.

In situ measurements of cloud droplet number concentration N are limited by the sampled cloud volume. Satellite retrievals of N suffer from inherent uncertainties, spatial averaging, and retrieval problems arising from the commonly assumed strictly adiabatic vertical profiles of cloud properties. To improve retrievals of N it is suggested in this paper to use a synergetic combination of passive and active airborne remote sensing measurement, to reduce the uncertainty of N retrievals, and to bridge the gap between in situ cloud sampling and global averaging. For this purpose, spectral solar radiation measurements above shallow trade wind cumulus were combined with passive microwave and active radar and lidar observations carried out during the second Next Generation Remote Sensing for Validation Studies (NARVAL-II) campaign with the High Altitude and Long Range Research Aircraft (HALO) in August 2016. The common technique to retrieve N is refined by including combined measurements and retrievals of cloud optical thickness τ, liquid water path (LWP), cloud droplet effective radius reff, and cloud base and top altitude. Three approaches are tested and applied to synthetic measurements and two cloud scenarios observed during NARVAL-II. Using the new combined retrieval technique, errors in N due to the adiabatic assumption have been reduced significantly.

Low planetary wave activity led to a stable vortex with exceptionally cold temperatures in the 2015–2016 Arctic winter. Extended areas with temperatures below the ice frost point temperature Tice persisted over weeks in the Arctic stratosphere as derived from the 36-year temperature climatology of the ERA-Interim reanalysis data set of the European Centre for Medium-Range Weather Forecasts (ECMWF). These extreme conditions promoted the formation of widespread polar stratospheric ice clouds (ice PSCs). The space-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on board the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite continuously measured ice PSCs for about a month with maximum extensions of up to 2×106 km2 in the stratosphere.On 22 January 2016, the WALES (Water Vapor Lidar Experiment in Space – airborne demonstrator) lidar on board the High Altitude and Long Range Research Aircraft HALO detected an ice PSC with a horizontal length of more than 1400 km. The ice PSC extended between 18 and 24 km altitude and was surrounded by nitric acid trihydrate (NAT) particles, supercooled ternary solution (STS) droplets and particle mixtures. The ice PSC occurrence histogram in the backscatter ratio to particle depolarization ratio optical space exhibits two ice modes with high or low particle depolarization ratios. Domain-filling 8-day back-trajectories starting in the high particle depolarization (high-depol) ice mode are continuously below the NAT equilibrium temperature TNAT and decrease below Tice ∼ 10 h prior to the observation. Their matches with CALIPSO PSC curtain plots demonstrate the presence of NAT PSCs prior to high-depol ice, suggesting that the ice had nucleated on NAT. Vice versa, STS or no PSCs were detected by CALIPSO prior to the ice mode with low particle depolarization ratio. In addition to ice nucleation in STS potentially having meteoric inclusions, we find evidence for ice nucleation on NAT in the Arctic winter 2015–2016. The observation of widespread Arctic ice PSCs with high or low particle depolarization ratios advances our understanding of ice nucleation in polar latitudes. It further provides a new observational database for the parameterization of ice nucleation schemes in atmospheric models.

The CNES (French Space Agency) and DLR (German Space Agency) project MERLIN is a future integrated path differential absorption (IPDA) lidar satellite mission that aims at measuring methane dry-air mixing ratio columns (XCH4) in order to improve surface flux estimates of this key greenhouse gas. To reach a 1 % relative random error on XCH4 measurements, MERLIN signal processing performs an averaging of data over 50 km along the satellite trajectory. This article discusses how to process this horizontal averaging in order to avoid the bias caused by the non-linearity of the measurement equation and measurements affected by random noise and horizontal geophysical variability. Three averaging schemes are presented: averaging of columns of XCH4, averaging of columns of differential absorption optical depth (DAOD) and averaging of signals. The three schemes are affected both by statistical and geophysical biases that are discussed and compared, and correction algorithms are developed for the three schemes. These algorithms are tested and their biases are compared on modelled scenes from real satellite data. To achieve the accuracy requirements that are limited to 0.2 % relative systematic error (for a reference value of 1780 ppb), we recommend performing the averaging of signals corrected from the statistical bias due to the measurement noise and from the geophysical bias mainly due to variations of methane optical depth and surface reflectivity along the averaging track. The proposed method is compliant with the mission relative systematic error requirements dedicated to averaging algorithms of 0.06 % (±1 ppb for XCH4 = 1780 ppb) for all tested scenes and all tested ground reflectivity values.

Cirrus clouds impose high uncertainties on climate prediction, as knowledge on important processes is still incomplete. For instance it remains unclear how cloud microphysical and radiative properties change as the cirrus evolves. Recent studies classify cirrus clouds into categories including in situ, orographic, convective and liquid origin clouds and investigate their specific impact. Following this line, we present a novel scheme for the classification of cirrus clouds that addresses the need to determine specific stages of cirrus evolution. Our classification scheme is based on airborne Differential Absorption and High Spectral Resolution Lidar measurements of atmospheric water vapor, aerosol depolarization, and backscatter, together with model temperature fields and simplified parameterizations of freezing onset conditions. It identifies regions of supersaturation with respect to ice (ice-supersaturated regions, ISSRs), heterogeneous and homogeneous nucleation, depositional growth, and ice sublimation and sedimentation with high spatial resolution. Thus, all relevant stages of cirrus evolution can be classified and characterized. In a case study of a gravity lee-wave-influenced cirrus cloud, encountered during the ML-CIRRUS flight campaign, the applicability of our classification is demonstrated. Revealing the structure of cirrus clouds, this valuable tool might help to examine the influence of evolution stages on the cloud's net radiative effect and to investigate the specific variability of optical and microphysical cloud properties in upcoming research.

Spectral radiance measurements collected in nadir and sideward viewing directions by two airborne passive solar remote sensing instruments, the Spectral Modular Airborne Radiation measurement sysTem (SMART) and the Differential Optical Absorption Spectrometer (mini-DOAS), are used to compare the remote sensing results of cirrus optical thickness τ. The comparison is based on a sensitivity study using radiative transfer simulations (RTS) and on data obtained during three airborne field campaigns: the North Atlantic Rainfall VALidation (NARVAL) mission, the Mid-Latitude Cirrus Experiment (ML-CIRRUS) and the Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems (ACRIDICON) campaign. Radiative transfer simulations are used to quantify the sensitivity of measured upward radiance I with respect to τ, ice crystal effective radius reff, viewing angle of the sensor θV, spectral surface albedo α, and ice crystal shape. From the calculations it is concluded that sideward viewing measurements are generally better suited than radiance data from the nadir direction to retrieve τ of optically thin cirrus, especially at wavelengths larger than λ = 900 nm. Using sideward instead of nadir-directed spectral radiance measurements significantly improves the sensitivity and accuracy in retrieving τ, in particular for optically thin cirrus of τ ≤ 2. The comparison of retrievals of τ based on nadir and sideward viewing radiance measurements from SMART, mini-DOAS and independent estimates of τ from an additional active remote sensing instrument, the Water Vapor Lidar Experiment in Space (WALES), shows general agreement within the range of measurement uncertainties. For the selected example a mean τ of 0.54 ± 0.2 is derived from SMART, and 0.49 ± 0.2 by mini-DOAS nadir channels, while WALES obtained a mean value of τ = 0.32 ± 0.02 at 532 nm wavelength, respectively. The mean of τ derived from the sideward viewing mini-DOAS channels is 0.26 ± 0.2. For the few simultaneous measurements, the mini-DOAS sideward channel measurements systematically underestimate (−17.6 %) the nadir observations from SMART and mini-DOAS. The agreement between mini-DOAS sideward viewing channels and WALES is better, showing the advantage of using sideward viewing measurements for cloud remote sensing for τ ≤ 1. Therefore, we suggest sideward viewing measurements for retrievals of τ of thin cirrus because of the significantly enhanced capability of sideward viewing compared to nadir measurements.

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 35 ppm on its lower west side, but did not drop below 120 ppm 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 50 ppm 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 70 ppb, 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.

Aerosol and water vapour measurements were performed with the lidar system WALES of Deutsches Zentrum für Luft- und Raumfahrt (DLR) in October and November 2010 during the first mission with the new German research aircraft G55-HALO. Curtains composed of lidar profiles beneath the aircraft show the vertical and horizontal distribution and variability of water vapour mixing ratio and backscatter ratio above Germany. Two missions on 3 and 4 November 2010 were selected to derive the water vapour mixing ratio inside cirrus clouds from the lidar instrument. A good agreement was found with in situ observations performed on a second research aircraft flying below HALO. ECMWF analysis temperature data are used to derive relative humidity fields with respect to ice (RHi) inside and outside of cirrus clouds from the lidar water vapour observations. The RHi variability is dominated by small-scale fluctuations in the water vapour fields while the temperature variation has a minor impact. The most frequent in-cloud RHi value from lidar observations is 98%. The RHi variance is smaller inside the cirrus than outside of the cloud. 2-D histograms of relative humidity and backscatter ratio show significant differences for in-cloud and out-of-cloud situations for two different cirrus cloud regimes. Combined with accurate temperature measurements, the lidar observations have a great potential for detailed statistical cirrus cloud and related humidity studies.

Airborne measurements of solar spectral radiance reflected by cirrus are performed with the HALO-Solar Radiation (HALO-SR) instrument onboard the High Altitude and Long Range Research Aircraft (HALO) in November 2010. The data are used to quantify the influence of surface albedo variability on the retrieval of cirrus optical thickness and crystal effective radius. The applied retrieval of cirrus optical properties is based on a standard two-wavelength approach utilizing measured and simulated reflected radiance in the visible and near-infrared spectral region. Frequency distributions of the surface albedos from Moderate resolution Imaging Spectroradiometer (MODIS) satellite observations are used to compile surface-albedo-dependent lookup tables of reflected radiance. For each assumed surface albedo the cirrus optical thickness and effective crystal radius are retrieved as a function of the assumed surface albedo. The results for the cirrus optical thickness are compared to measurements from the High Spectral Resolution Lidar (HSRL). The uncertainty in cirrus optical thickness due to local variability of surface albedo in the specific case study investigated here is below 0.1 and thus less than that caused by the measurement uncertainty of both instruments. It is concluded that for the retrieval of cirrus optical thickness the surface albedo variability is negligible. However, for the retrieval of crystal effective radius, the surface albedo variability is of major importance, introducing uncertainties up to 50%. Furthermore, the influence of the bidirectional reflectance distribution function (BRDF) on the retrieval of crystal effective radius was investigated and quantified with uncertainties below 10%, which ranges below the uncertainty caused by the surface albedo variability. The comparison with the independent lidar data allowed for investigation of the role of the crystal shape in the retrieval. It is found that if assuming aggregate ice crystals, the HSRL observations fit best with the retrieved optical thickness from HALO-SR.

During four aircraft field experiments with the DLR research aircraft Falcon in 1998 (LACE), 2006 (SAMUM-1) and 2008 (SAMUM-2 and EUCAARI), airborne High Spectral Resolution Lidar (HSRL) and in situ measurements of aerosol microphysical and optical properties were performed. Altogether, the properties of six different aerosol types and aerosol mixtures – Saharan mineral dust, Saharan dust mixtures, Canadian biomass burning aerosol, African biomass burning mixture, anthropogenic pollution aerosol, and marine aerosol have been studied. On the basis of this extensive HSRL data set, we present an aerosol classification scheme which is also capable to identify mixtures of different aerosol types. We calculated mixing lines that allowed us to determine the contributing aerosol types. The aerosol classification scheme was supported by backward trajectory analysis and validated with in-situ measurements. Our results demonstrate that the developed aerosol mask is capable to identify complex stratifications with different aerosol types throughout the atmosphere.

Airborne high spectral resolution lidar observations over Europe during the EUCAARI-LONGREX field experiment in May 2008 are analysed with respect to the optical properties of continental pollution aerosol. Continental pollution aerosol is characterized by its depolarisation and lidar ratio. Over all, the measurements of the lidar ratio and the particle linear depolarization ratio of pollution aerosols provide a narrow range of values. Therefore, this data set allows for a distinct characterization of the aerosol type "pollution aerosol" and thus is valuable both to distinguish continental pollution aerosol from other aerosol types and to determine mixtures with other types of aerosols.

During the CIRCLE-2 experiment carried out over Western Europe in May 2007, combined in situ and remote sensing observations allowed to describe microphysical and optical properties near-top of an overshooting convective cloud (11 080 m/−58 °C). The airborne measurements were performed with the DLR Falcon aircraft specially equipped with a unique set of instruments for the extensive in situ cloud measurements of microphysical and optical properties (Polar Nephelometer, FSSP-300, Cloud Particle Imager and PMS 2-D-C) and nadir looking remote sensing observations (DLR WALES Lidar). Quasi-simultaneous space observations from MSG/SEVIRI, CALIPSO/CALIOP-WFC-IIR and CloudSat/CPR combined with airborne RASTA radar reflectivity from the French Falcon aircraft flying above the DLR Falcon depict very well convective cells which overshoot by up to 600 m the tropopause level. Unusual high values of the concentration of small ice particles, extinction, ice water content (up to 70 cm−3, 30 km−1 and 0.5 g m−3, respectively) are experienced. The mean effective diameter and the maximum particle size are 43 μm and about 300 μm, respectively. This very dense cloud causes a strong attenuation of the WALES and CALIOP lidar returns. The SEVIRI retrieved parameters confirm the occurrence of small ice crystals at the top of the convective cell. Smooth and featureless phase functions with asymmetry factors of 0.776 indicate fairly uniform optical properties. Due to small ice crystals the power-law relationship between ice water content (IWC) and radar reflectivity appears to be very different from those usually found in cirrus and anvil clouds. For a given equivalent reflectivity factor, IWCs are significantly larger for the overshooting cell than for the cirrus. Assuming the same prevalent microphysical properties over the depth of the overshooting cell, RASTA reflectivity profiles scaled into ice water content show that retrieved IWC up to 1 g m−3 may be observed near the cloud top. Extrapolating the relationship for stronger convective clouds with similar ice particles, IWC up to 5 g m−3 could be experienced with reflectivity factors no larger than about 20 dBZ. This means that for similar situations, indication of rather weak radar echo does not necessarily warn the occurrence of high ice water content carried by small ice crystals. All along the cloud penetration the shape of the ice crystals is dominated by chain-like aggregates of frozen droplets. Our results confirm previous observations that the chains of ice crystals are found in a continental deep convective systems which are known generally to generate intense electric fields causing efficient ice particle aggregation processes. Vigorous updrafts could lift supercooled droplets which are frozen extremely rapidly by homogeneous nucleation near the −37 °C level, producing therefore high concentrations of very small ice particles at upper altitudes. They are sufficient to deplete the water vapour and suppress further nucleation as confirmed by humidity measurements. These observations address scientific issues related to the microphysical properties and structure of deep convective clouds and confirm that particles smaller than 50 μm may control the radiative properties in convective-related clouds. These unusual observations may also provide some possible insights regarding engineering issues related to the failure of jet engines commonly used on commercial aircraft during flights through areas of high ice water content. However, large uncertainties of the measured and derived parameters limit our observations.

Methane is the third most important greenhouse gas in the atmosphere after water vapour and carbon dioxide. A major handicap to quantify the emissions at the Earth's surface in order to better understand biosphere-atmosphere exchange processes and potential climate feedbacks is the lack of accurate and global observations of methane. Space-based integrated path differential absorption (IPDA) lidar has potential to fill this gap, and a Methane Remote Lidar Mission (MERLIN) on a small satellite in polar orbit was proposed by DLR and CNES in the frame of a German-French climate monitoring initiative. System simulations are used to identify key performance parameters and to find an advantageous instrument configuration, given the environmental, technological, and budget constraints. The sensitivity studies use representative averages of the atmospheric and surface state to estimate the measurement precision, i.e. the random uncertainty due to instrument noise. Key performance parameters for MERLIN are average laser power, telescope size, orbit height, surface reflectance, and detector noise. A modest-size lidar instrument with 0.45 W average laser power and 0.55 m telescope diameter on a 506 km orbit could provide 50-km averaged methane column measurement along the sub-satellite track with a precision of about 1% over vegetation. The use of a methane absorption trough at 1.65 μm improves the near-surface measurement sensitivity and vastly relaxes the wavelength stability requirement that was identified as one of the major technological risks in the pre-phase A studies for A-SCOPE, a space-based IPDA lidar for carbon dioxide at the European Space Agency. Minimal humidity and temperature sensitivity at this wavelength position will enable accurate measurements in tropical wetlands, key regions with largely uncertain methane emissions. In contrast to actual passive remote sensors, measurements in Polar Regions will be possible and biases due to aerosol layers and thin ice clouds will be minimised.

In the tropics, deep convection is the major source of uncertainty in water vapor transport to the upper troposphere and into the stratosphere. Although accurate measurements in this region would be of first order importance to better understand the processes that govern stratospheric water vapor concentrations and trends in the context of a changing climate, they are sparse because of instrumental shortcomings and observational challenges. Therefore, the Falcon research aircraft of the Deutsches Zentrum für Luft- und Raumfahrt (DLR) flew a zenith-viewing water vapor differential absorption lidar (DIAL) during the Tropical Convection, Cirrus and Nitrogen Oxides Experiment (TROCCINOX) in 2004 and 2005 in Brazil. The measurements were performed alternatively on three water vapor absorption lines of different strength around 940 nm. These are the first aircraft DIAL measurements in the tropical upper troposphere and in the mid-latitudes lower stratosphere. Sensitivity analyses reveal an accuracy of 5% between altitudes of 8 and 16 km. This is confirmed by intercomparisons with the Fast In-situ Stratospheric Hygrometer (FISH) and the Fluorescent Advanced Stratospheric Hygrometer (FLASH) onboard the Russian M-55 Geophysica research aircraft during five coordinated flights. The average relative differences between FISH and DIAL amount to −3%±8% and between FLASH and DIAL to −8%±14%, negative meaning DIAL is more humid. The average distance between the probed air masses was 129 km. The DIAL is found to have no altitude- or latitude-dependent bias. A comparison with the balloon ascent of a laser absorption spectrometer gives an average difference of 0%±19% at a distance of 75 km. Six tropical DIAL under-flights of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT reveal a mean difference of −8%±49% at an average distance of 315 km. While the comparison with MIPAS is somewhat less significant due to poorer comparison conditions, the agreement with the in-situ hygrometers provides evidence of the excellent quality of FISH, FLASH and DIAL. Most DIAL profiles exhibit a smooth exponential decrease of water vapor mixing ratio in the tropical upper troposphere to lower stratosphere transition. The hygropause with a minimum mixing ratio of 2.5 µmol/mol is found between 15 and 17 km. A high-resolution (2 km horizontal, 0.2 km vertical) DIAL cross section through the anvil outflow of tropical convection shows that the ambient humidity is increased by a factor of three across 100 km.

Mechanisms by which subvisible cirrus clouds (SVCs) might contribute to dehydration close to the tropical tropopause are not well understood. Recently Ultrathin Tropical Tropopause Clouds (UTTCs) with optical depths around 10-4 have been detected in the western Indian ocean. These clouds cover thousands of square kilometers as 200-300 m thick distinct and homogeneous layer just below the tropical tropopause. In their condensed phase UTTCs contain only 1-5% of the total water, and essentially no nitric acid. A new cloud stabilization mechanism is required to explain this small fraction of the condensed water content in the clouds and their small vertical thickness. This work suggests a mechanism, which forces the particles into a thin layer, based on upwelling of the air of some mm/s to balance the ice particles, supersaturation with respect to ice above and subsaturation below the UTTC. In situ measurements suggest that these requirements are fulfilled. The basic physical properties of this mechanism are explored by means of a single particle model. Comprehensive 1-D cloud simulations demonstrate this stabilization mechanism to be robust against rapid temperature fluctuations of +/- 0.5 K. However, rapid warming (Delta T > 2 K) leads to evaporation of the UTTC, while rapid cooling (Delta T < -2 K) leads to destabilization of the particles with the potential for significant dehydration below the cloud

Subvisible cirrus clouds (SVCs) may contribute to dehydration close to the tropical tropopause. The higher and colder SVCs and the larger their ice crystals, the more likely they represent the last efficient point of contact of the gas phase with the ice phase and, hence, the last dehydrating step, before the air enters the stratosphere. The first simultaneous in situ and remote sensing measurements of SVCs were taken during the APE-THESEO campaign in the western Indian ocean in February/March 1999. The observed clouds, termed Ultrathin Tropical Tropopause Clouds (UTTCs), belong to the geometrically and optically thinnest large-scale clouds in the Earth's atmosphere. Individual UTTCs may exist for many hours as an only 200--300 m thick cloud layer just a few hundred meters below the tropical cold point tropopause, covering up to 105 km2. With temperatures as low as 181 K these clouds are prime representatives for defining the water mixing ratio of air entering the lower stratosphere.