Abstract. Variations of stable water isotopes in water vapourhave become measurable at a measurement frequency of about 1 Hz in recent years using novel laser spectroscopic techniques. This enables us to perform continuous measurements for process-based investigations of the atmospheric water cycle at the time scales relevant for synoptic and mesoscale meteorology. An important prerequisite for the interpretation of data from automated field measurements lasting for several weeks or months is a detailed knowledge about instrument properties and the sources of measurement uncertainty. We present here a comprehensive characterisation and comparison study of two commercial laser spectroscopic systems based on cavity ring-down spectroscopy (Picarro) and off-axis integrated cavity output spectroscopy (Los Gatos Research). The uncertainty components of the measurements were first assessed in laboratory experiments, focussing on the effects of (i) water vapour mixing ratio, (ii) measurement stability, (iii) uncertainties due to calibration and (iv) response times of the isotope measurements due to adsorption-desorption processes on the tubing and measurement cavity walls. Based on the experience from our laboratory experiments, we set up a one-week field campaign for comparing measurements of the ambient isotope signals from the two laser spectroscopic systems. The optimal calibration strategy determined for both instruments was applied as well as the correction functions for water vapour mixing ratio effects. The root mean square difference between the isotope signals from the two instruments during the field deployment was 2.3 ‰ for δ 2 H, 0.5 ‰ for δ 18 O and 3.1 ‰ for deuterium excess. These uncertainty estimates from field measurements compare well to those found in the laboratory experiments. The present quality of measurements from laser spectroscopic instruments combined with a calibration system opens new possibilities for investigating the atmospheric water cycle and the land-atmosphere moisture fluxes.

Uncertainty in radiative forcing caused by aerosol–cloud interactions is about twice as large as for CO2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly quantified state of aerosols in the pristine preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to help evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific, and Atlantic Oceans; length of ship track >33,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics [e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations], trace gases, and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, and back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset (https://zenodo.org/communities/spi-ace?page=1&size=20) provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport, and processing occurring over the pristine Southern Ocean.

Abstract. Studying the evaporation process and its link to the atmospheric circulation is central for a better understanding of the feedbacks between the surface water components and the atmosphere. In this study, we use 5 months of deuterium excess (d) measurements at the hourly to daily timescale from a cavity ring-down laser spectrometer to characterise the evaporation source of low-level continental water vapour at the long-term hydrometeorological monitoring site Rietholzbach in northeastern Switzerland. To reconstruct the phase change history of the air masses in which we measure the d signature and to diagnose its area of surface evaporation we apply a Lagrangian moisture source diagnostic. With the help of a correlation analysis we investigate the strength of the relation between d measurements and the moisture source conditions. Temporal episodes with a duration of a few days of strong anticorrelation between d and relative humidity as well as temperature are identified. The role of plant transpiration, the large-scale advection of remotely evaporated moisture, the local boundary layer dynamics at the measurement site and recent precipitation at the site of evaporation are discussed as reasons for the existence of these modes of strong anticorrelation between d and moisture source conditions. We show that the importance of continental moisture recycling and the contribution of plant transpiration to the continental evaporation flux may be deduced from the d-relative humidity relation at the seasonal timescale as well as for individual events. The methodology and uncertainties associated with these estimates of the transpiration fraction of evapotranspiration are presented and the proposed novel framework is applied to individual events from our data set. Over the whole analysis period (August to December 2011) a transpiration fraction of the evapotranspiration flux over the continental part of the moisture source region of 62 % is found albeit with a large event-to-event variability (0 % to 89 %) for continental Europe. During days of strong local moisture recycling a higher overall transpiration fraction of 76 % (varying between 65 % and 86 %) is found. These estimates are affected by uncertainties in the assumptions involved in our method as well as by parameter uncertainties. An average uncertainty of 11 % results from the strong dependency of the transpiration estimates on the choice of the non-equilibrium fractionation factor. Other uncertainty sources like the influence of boundary layer dynamics are probably large but more difficult to quantify. Nevertheless, such Lagrangian estimates of the transpiration part of continental evaporation could potentially be useful for the verification of model estimates of this important landatmosphere coupling parameter.

This study investigates the role of below‐cloud evaporation and evapotranspiration for the short‐term variability of stable isotopes in near‐surface water vapor and precipitation associated with central European cold fronts. To this end, a combination of observations with high temporal resolution and numerical sensitivity experiments with the isotope‐enabled regional weather prediction model COSMOiso is used. The representation of the interaction between rain droplets and ambient vapor below the cloud is fundamental for adequately simulating precipitation isotopes (δp) and total rainfall amount. Neglecting these effects leads to depletion biases of 20–40‰ in δp2H and 5–10‰ in δp18O and to an increase of 74% in rainfall amount. Isotope fractionation during soil evaporation is of primary importance for correctly simulating the variability of continental low‐level vapor δv2H and δv18O and particularly of the secondary isotope parameter deuterium excess (dv).

Abstract. Stable isotopes of water vapour are powerful indicators of meteorological processes on a broad range of scales, reflecting evaporation, condensation, and air mass mixing processes. With the recent advent of fast laser-based spectroscopic methods, it has become possible to measure the stable isotopic composition of atmospheric water vapour in situ at a high temporal resolution. Here we present results from such comprehensive airborne spectroscopic isotope measurements in water vapour over the western Mediterranean at a high spatial and temporal resolution. Measurements have been acquired by a customized Picarro L2130-i cavity-ring down spectrometer deployed onboard the Dornier 128 D-IBUF aircraft together with a meteorological flux measurement package during the HyMeX SOP1 (Hydrological cycle in Mediterranean Experiment special observation period 1) field campaign in Corsica, France, during September and October 2012. Taking into account memory effects of the air inlet pipe, the typical time resolution of the measurements was about 15-30 s, resulting in an average horizontal resolution of about 1-2 km. Cross-calibration of the water vapour measurements from all humidity sensors showed good agreement under most flight conditions but the most turbulent ones. In total 21 successful stable isotope flights with 59 flight hours have been performed. Our data provide quasi-climatological autumn average conditions and vertical profiles of the stable isotope parameters δD, δ 18 O, and d-excess during the study period. A d-excess minimum in the overall average profile is reached in the region of the boundary-layer top, possibly caused by precipitation evaporation. This minimum is bracketed by higher d-excess values near the surface caused by non-equilibrium fractionation, and a maximum above the boundary layer related to the increasing d-excess in very depleted and dry high-altitude air masses. Repeated flights along the same pattern reveal pronounced day-to-day variability due to changes in the large-scale circulation. During a period marked by a strong inversion at the top of the marine boundary layer, vertical gradients in stable isotopes reached up to 25.4 ‰ 100 m −1 for δD and 24.0 ‰ 100 m −1 for the dexcess.

Abstract. Global measurements of atmospheric water vapour isotopologues aid to better understand the hydrological cycle and improve global circulation models. This paper presents a new data set of vertical column densities of H2O and HDO retrieved from short-wave infrared (2.3 µm) reflectance measurements by the Tropospheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite. TROPOMI features daily global coverage with a spatial resolution of up to 7 km×7 km. The retrieval utilises a profile-scaling approach. The forward model neglects scattering, and strict cloud filtering is therefore necessary. For validation, recent ground-based water vapour isotopologue measurements by the Total Carbon Column Observing Network (TCCON) are employed. A comparison of TCCON δD with ground-based measurements by the Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) project for data prior to 2014 (where MUSICA data are available) shows a bias in TCCON δD estimates. As TCCON HDO is currently not validated, an overall correction of recent TCCON HDO data is derived based on this finding. The agreement between the corrected TCCON measurements and co-located TROPOMI observations is good with an average bias of (-0.2±3)×1021 molec cm−2 ((1.1±7.2) %) in H2O and (-2±7)×1017 molec cm−2 ((-1.1±7.3) %) in HDO, which corresponds to a mean bias of (-14±17) ‰ in a posteriori δD. The bias is lower at low- and mid-latitude stations and higher at high-latitude stations. The use of the data set is demonstrated with a case study of a blocking anticyclone in northwestern Europe in July 2018 using single-overpass data.

Abstract. Stable water isotopologues (SWIs) are useful tracers of moist diabatic processes in the atmospheric water cycle. They provide a framework to analyse moist processes on a range of timescales from large-scale moisture transport to cloud formation, precipitation and small-scale turbulent mixing. Laser spectrometric measurements on research vessels produce high-resolution time series of the variability of the water vapour isotopic composition in the marine boundary layer. In this study, we present a 5-month continuous time series of such ship-based measurements of δ2H and δ18O from the Antarctic Circumnavigation Expedition (ACE) in the Atlantic and the Southern Ocean in the time period from November 2016 to April 2017. We analyse the drivers of meridional SWI variations in the marine boundary layer across diverse climate zones in the Atlantic and Southern Ocean using Lagrangian moisture source diagnostics and relate vertical SWI differences to near-surface wind speed and ocean surface state. The median values of δ18O, δ2H and deuterium excess during ACE decrease continuously from low to high latitudes. These meridional SWI distributions reflect climatic conditions at the measurement and moisture source locations, such as air temperature, specific humidity and relative humidity with respect to sea surface temperature. The SWI variability at a given latitude is highest in the extratropics and polar regions with decreasing values equatorwards. This meridional distribution of SWI variability is explained by the variability in moisture source locations and its associated environmental conditions as well as transport processes. The westward-located moisture sources of water vapour in the extratropics are highly variable in extent and latitude due to the frequent passage of cyclones and thus widen the range of encountered SWI values in the marine boundary layer. Moisture loss during transport further contributes to the high SWI variability in the extratropics. In the subtropics and tropics, persistent anticyclones lead to well-confined narrow easterly moisture source regions, which is reflected in the weak SWI variability in these regions. Thus, the expected range of SWI signals at a given latitude strongly depends on the large-scale circulation. Furthermore, the ACE SWI time series recorded at 8.0 and 13.5 m above the ocean surface provide estimates of vertical SWI gradients in the lowermost marine boundary layer. On average, the vertical gradients with height found during ACE are -0.1‰m-1 for δ18O, -0.5‰m-1 for δ2H and 0.3 ‰ m−1 for deuterium excess. Careful calibration and post-processing of the SWI data and a detailed uncertainty analysis provide a solid basis for the presented gradients. Using sea spray concentrations and sea state conditions, we show that the vertical SWI gradients are particularly large during high wind speed conditions with increased contribution of sea spray evaporation or during low wind speed conditions due to weak vertical turbulent mixing. Although further SWI measurements at a higher vertical resolution are required to validate these findings, the simultaneous SWI measurements at several heights during ACE show the potential of SWIs as tracers for vertical mixing and sea spray evaporation in the lowermost marine boundary layer.

This paper presents an object-based, global climatology (1979–2014) of strong large-scale ocean evaporation (SLOE) and its associated climatic properties. SLOE is diagnosed using an “atmospheric moisture uptake efficiency” criterion related to the ratio of surface evaporation and integrated water vapor content in the near-surface atmosphere. The chosen Eulerian identification procedure focuses on events that strongly contribute to the available near-surface atmospheric humidity. SLOE is particularly frequent along the warm ocean western boundary currents, downstream of large continental areas, and at the sea ice edge in polar regions with frequent cold-air outbreaks. Furthermore, wind-driven SLOE occurs in regions with topographically enforced winds. On a global annual average, SLOE occurs only 6% of the time but explains 22% of total ocean evaporation. An analysis of the past history and fate of air parcels involved in cold season SLOE in the North Atlantic and south Indian Oceans shows that cold-air advection is the main mechanism that induces these events. Extratropical cyclones thereby play an important role in setting the necessary equatorward synoptic flow. Consequently, the interannual variability of SLOE associated with the North Atlantic Oscillation and the southern annular mode reveals a very high sensitivity of SLOE with respect to the location of the storm tracks. This study highlights the strong link between transient synoptic events and the spatiotemporal variability in ocean evaporation patterns, which cannot be deduced from thermodynamic steady-state and climate mean state considerations alone.