Intercomparison of in situ water vapor balloon-borne measurements from Pico-SDLA H₂O and FLASH-B in the tropical UTLS

In this paper we compare water vapor mixing ratio measurements from two quasi-parallel flights of the Pico-SDLA H2O and FLASH-B hygrometers. The measurements were made on 10 February 2013 and 13 March 2012, respectively, in the tropics near Bauru, Sao Paulo St., Brazil during an intense convective period. Both flights were performed as part of a French scientific project, TRO-Pico, to study the impact of the deep-convection overshoot on the water budget. Only a few instruments that permit the frequent sounding of stratospheric water vapor can be flown within a small volume weather balloons. Technical difficulties preclude the accurate measurement of stratospheric water vapor with conventional in situ techniques. The instruments described here are simple and lightweight, which permits their low-cost deployment by non-specialists aboard a small weather balloon. We obtain mixing ratio retrievals which agree above the cold-point tropopause to within 1.9 and 0.5 % for the first and second flights, respectively. This level of agreement for measured stratospheric water mixing ratio is among the best ever reported in the literature. Because both instruments show similar profiles within their combined uncertainties, we conclude that the Pico-SDLA H2O and FLASH-B datasets are mutually consistent.

The airborne mass spectrometer AIMS – Part 2: Measurements of trace gases with stratospheric or tropospheric origin in the UTLS

Understanding the role of climate-sensitive trace gas variabilities in the upper troposphere and lower stratosphere region (UTLS) and their impact on its radiative budget requires accurate measurements. The composition of the UTLS is governed by transport and chemistry of stratospheric and tropospheric constituents, such as chlorine, nitrogen oxide and sulphur components. The Airborne chemical Ionization Mass Spectrometer AIMS has been developed to accurately measure a set of these constituents on aircraft by means of chemical ionization. Here we present a setup using chemical ionization with SF5− reagent ions for the simultaneous measurement of trace gas concentrations in the pptv to ppmv (10−12 to 10−6 mol mol−1) range of HCl, HNO3 and SO2 with in-flight and online calibration called AIMS-TG. Part 1 of this paper (Kaufmann et al., 2015) reports on the UTLS water vapour measurements with the AIMS-H2O configuration. The instrument can be flexibly switched between two configurations depending on the scientific objective of the mission. For AIMS-TG, a custom-made gas discharge ion source has been developed generating a characteristic ionization scheme. HNO3 and HCl are routinely calibrated in-flight using permeation devices, SO2 is permanently calibrated during flight adding an isotopically labelled 34SO2 standard. In addition, we report on trace gas measurements of HONO which is sensitive to the reaction with SF5−. The detection limit for the various trace gases is in the low ten pptv range at a 1 s time resolution with an overall uncertainty of the measurement in the order of 20 %. AIMS has been integrated and successfully operated on the DLR research aircraft Falcon and HALO. Exemplarily, measurements conducted during the TACTS/ESMVal mission with HALO in 2012 are presented, focusing on a classification of tropospheric and stratospheric influences in the UTLS region. Comparison of AIMS measurements with other measurement techniques allow to draw a comprehensive picture of the sulphur, chlorine and reactive nitrogen oxide budget in the UTLS. The combination of the trace gases measured with AIMS exhibit the potential to gain a better understanding of the trace gas origin and variability at and near the tropopause.

The airborne mass spectrometer AIMS – Part 1: AIMS-H₂O for UTLS water vapor measurements

In the upper troposphere and lower stratosphere (UTLS), the accurate quantification of low water vapor concentrations has presented a significant measurement challenge. The instrumental uncertainties are passed on to estimates of H2O transport, cloud formation and the H2O role in the UTLS energy budget and resulting effects on surface temperatures. To address the uncertainty in UTLS H2O determination, the airborne mass spectrometer AIMS-H2O, with in-flight calibration, has been developed for fast and accurate airborne water vapor measurements. We present the new setup to measure water vapor by direct ionization of ambient air. Air is sampled via a backward facing inlet that includes a bypass flow to assure short residence times (< 0.2 s) in the inlet line, which allows the instrument to achieve a time resolution of ∼ 4 Hz. From the main inlet flow, a smaller flow is extracted into the novel pressure-controlled gas discharge ion source of the mass spectrometer. The air is directed through the gas discharge region where water molecules react to form hydronium ion clusters, H3O+(H2O)n (n= 0, 1, 2), in a complex reaction scheme similar to the reactions in the D-region of the ionosphere. These ions are counted to quantify the ambient water vapor mixing ratio. The instrument is calibrated during flight using a new calibration source based on the catalytic reaction of H2 and O2 on a Pt surface to generate a calibration standard with well defined and stable H2O mixing ratios. In order to increase data quality over a range of mixing ratios, two data evaluation methods are presented for lower and higher H2O mixing ratios respectively, using either only the H3O+(H2O) ions or the ratio of all water vapor dependent ions to the total ion current. Altogether, a range of water vapor mixing ratios from 1 to 500 ppmv (mole ratio, 10−6 mol mol−1) can be covered with an accuracy between 7 and 15 %. AIMS-H2O was deployed on two DLR research aircraft, the Falcon during CONCERT (Contrail and Cirrus Experiment) in 2011, and HALO during ML-CIRRUS (Mid-Latitude Cirrus) in 2014. The comparison of AIMS-H2O with the SHARC tunable diode laser hygrometer during ML-CIRRUS shows a very good overall agreement between both instruments for the entire campaign.

An automatic precipitation phase distinction algorithm for optical disdrometer data over the global ocean

The lack of high quality in situ surface precipitation data over the global ocean so far limits the capability to validate satellite precipitation retrievals. The first systematic ship-based surface precipitation dataset OceanRAIN (Ocean Rainfall And Ice-phase precipitation measurement Network) aims at providing a comprehensive statistical basis of in situ precipitation reference data from optical disdrometers at 1 min resolution deployed on various research vessels (RVs). Deriving the precipitation rate for rain and snow requires a priori knowledge of the precipitation phase (PP). Therefore, we present an automatic PP distinction algorithm using available data based on more than four years of atmospheric measurements onboard RV Polarstern that covers all climatic regions of the Atlantic Ocean. A time-consuming manual PP distinction within the OceanRAIN post-processing serves as reference, mainly based on 3 hourly present weather information from a human observer. For automation, we find that the combination of air temperature, relative humidity and 99th percentile of the particle diameter predicts best the PP with respect to the manually determined PP. Excluding mixed-phase, this variable combination reaches an accuracy of 91 % when compared to the manually determined PP for about 149 000 min of precipitation from RV Polarstern. Including mixed-phase (165 000 min), 81.2 % accuracy are reached with a slight snow overprediction bias of 0.93 for two independent PP distributions. In that respect, a method using two independent PP distributions outperforms a method based on only one PP distribution. The new statistical automatic PP distinction method significantly speeds up the data post-processing within OceanRAIN while introducing an objective PP probability for each PP at 1 min resolution.

Quality assessment of solar UV irradiance measured with array spectroradiometers

The reliable quantification of ultraviolet (UV) radiation at the Earth's surface requires accurate measurements of spectral global solar UV irradiance in order to determine the UV exposure to human skin and to understand long-term trends in this parameter. Array spectroradiometers are small, light, robust and cost effective instruments and are increasingly used for spectral irradiance measurements. Within the European EMRP-ENV03 project "Solar UV", new devices, guidelines, and characterization methods have been developed to improve solar UV measurements with array spectroradiometers and support to the end-user community has been provided. In order to assess the quality of 14 end-user array spectroradiometers, a solar UV intercomparison was held on the measurement platform of the World Radiation Center (PMOD/WRC) in Davos, Switzerland, from 10 to 17 July 2014. The results of the intercomparison revealed that array spectroradiometers, currently used for solar UV measurements, show a large variation in the quality of their solar UV measurements. Most of the instruments overestimate the erythema weighted UV index – in particular at low solar zenith angles – due to stray light contribution in the UV-B range. The spectral analysis of global solar UV irradiance further supported the finding that the uncertainties in the UV-B range are very large due to stray light contribution in this wavelength range. In summary, the UV index may be detected by some commercially available array spectroradiometer within 5 % compared to the world reference spectroradiometer, if well characterized and calibrated, but only for a limited range or solar zenith angle. Generally, the tested instruments are not yet suitable for solar UV measurements for the entire range between 290 to 400 nm under all atmospheric conditions.

Consistency and quality assessment of the Metop-A/IASI and Metop-B/IASI operational trace gas products (O₃, CO, N₂O, CH₄ and CO₂) in the Subtropical North Atlantic

This paper presents the tools and methodology for performing a routine comprehensive monitoring of consistency and quality of IASI (Infrared Atmospheric Sounding Interferometer) trace gas Level 2 (L2) products (O3, CO, N2O, CH4 and CO2) generated at EUMETSAT (European Organisation for the Exploitation of Meteorological Satellites) using ground-based observations at the Izaña Atmospheric Observatory (IZO, Tenerife). As a demonstration the period 2010–2014 was analysed, covering the version 5 of the IASI L2 processor. Firstly, we assess the consistency between the total column (TC) observations from the IASI sensors on-board the EUMETSAT Metop-A and Metop-B meteorological satellites (IASI-A and IASI-B, respectively) in the subtropical North Atlantic region during the first two years of IASI-B operations (2012–2014). By analysing different time scales, we probe the daily and annual consistency of the variability observed by IASI-A and IASI-B and, thereby, assess the suitability of IASI-B for continuation of the IASI-A time series. The continuous inter-comparison of both IASI sensors also offers important diagnostics for identifying inconsistencies between the data records and for documenting their temporal stability. Once the consistency of IASI sensors is documented we estimate the overall accuracy of all the IASI trace gas TC products by comparing to coincident ground-based Fourier Transform Infrared Spectrometer (FTS) measurements performed at IZO from 2010 to 2014. The IASI L2 products reproduce the ground-based FTS observations well at the longest temporal scales, i.e., annual cycles and long-term trends for all the trace gases considered (Pearson correlation coefficient, R, larger than 0.95 and 0.75 for long-term trends and annual cycles, respectively) with the exception of CO2. For CO2 acceptable agreement is only achieved for long-term trends (R~0.70). The differences observed between IASI and FTS observations can be in part attributed to the different vertical sensitivities of the two remote sensing instruments and also to the degree of maturity of the IASI products: O3 and CO are pre-operational, while N2O, CH4 and CO2 are, for the period covered by this study, aspirational products only and are not considered mature. Regarding shorter timescales (single or daily measurements), only the O3 product seems to be show good sensitivity to actual atmospheric variations (R~0.80), while the CO product is only moderately sensitive (R~0.50). For the remainder of the trace gases, further improvements would be required to capture the day-to-day real atmospheric variability.

Organic and inorganic decomposition products from the thermal desorption of atmospheric particles

Atmospheric aerosol composition is often analyzed using thermal desorption techniques to evaporate samples and deliver organic or inorganic molecules to various designs of detectors for identification and quantification. The organic aerosol (OA) fraction is composed of thousands of individual compounds, some with nitrogen- and sulfur-containing functionality, and often contains oligomeric material, much of which may be susceptible to decomposition upon heating. Here we analyze thermal decomposition products as measured by a thermal desorption aerosol gas chromatograph (TAG) capable of separating thermal decomposition products from thermally stable molecules. The TAG impacts particles onto a collection and thermal desorption (CTD) cell, and upon completion of sample collection, heats and transfers the sample in a helium flow up to 310 °C. Desorbed molecules are refocused at the head of a GC column that is held at 45 °C and any volatile decomposition products pass directly through the column and into an electron impact quadrupole mass spectrometer (MS). Analysis of the sample introduction (thermal decomposition) period reveals contributions of NO+ (m/z 30), NO2+ (m/z 46), SO+ (m/z 48), and SO2+ (m/z 64), derived from either inorganic or organic particle-phase nitrate and sulfate. CO2+ (m/z 44) makes up a major component of the decomposition signal, along with smaller contributions from other organic components that vary with the type of aerosol contributing to the signal (e.g., m/z 53, 82 observed here for isoprene-derived secondary OA). All of these ions are important for ambient aerosol analyzed with the aerosol mass spectrometer (AMS), suggesting similarity of the thermal desorption processes in both instruments. Ambient observations of these decomposition products compared to organic, nitrate, and sulfate mass concentrations measured by an AMS reveal good correlation, with improved correlations for OA when compared to the AMS oxygenated OA (OOA) component. TAG signal found in the traditional compound elution time period reveals higher correlations with AMS hydrocarbon-like OA (HOA) combined with the fraction of OOA that is less oxygenated. Potential to quantify nitrate and sulfate aerosol mass concentrations using the TAG system is explored through analysis of ammonium sulfate and ammonium nitrate standards. While chemical standards display a linear response in the TAG system, re-desorptions of the CTD cell following ambient sample analysis shows some signal carryover on sulfate and organics, and new desorption methods should be developed to improve throughput. Future standards should be composed of complex organic/inorganic mixtures, similar to what is found in the atmosphere, and perhaps will more accurately account for any aerosol mixture effects on compositional quantification.

Thermodynamic correction of particle concentrations measured by underwing probes on fast flying aircraft

Particle concentration measurements with underwing probes on aircraft are impacted by air compression upstream of the instrument body as a function of flight velocity. In particular for fast-flying aircraft the necessity arises to account for compression of the air sample volume. Hence, a correction procedure is needed to invert measured particle number concentrations to ambient conditions that is commonly applicable for different instruments to gain comparable results. In the compression region where the detection of particles occurs (i.e. under factual measurement conditions), pressure and temperature of the air sample are increased compared to ambient (undisturbed) conditions in certain distance away from the aircraft. Conventional procedures for scaling the measured number densities to ambient conditions presume that the particle penetration speed through the instruments' detection area equals the aircraft speed (True Air Speed, TAS). However, particle imaging instruments equipped with pitot-tubes measuring the Probe Air Speed (PAS) of each underwing probe reveal PAS values systematically below those of the TAS. We conclude that the deviation between PAS and TAS is mainly caused by the compression of the probed air sample. From measurements during two missions in 2014 with the German Gulfstream G-550 (HALO – High Altitude LOng range) research aircraft we develop a procedure to correct the measured particle concentration to ambient conditions using a thermodynamic approach. With the provided equation the corresponding concentration correction factor ξ is applicable to the high frequency measurements of each underwing probe which is equipped with its own air speed sensor (e.g. a pitot-tube). ξ-values of 1 to 0.85 are calculated for air speeds (i.e. TAS) between 60 and 260 m s−1. From HALO data it is found that ξ does not significantly vary between the different deployed instruments. Thus, for the current HALO underwing probe configuration a parameterisation of ξ as a function of TAS is provided for instances if PAS measurements are lacking. The ξ-correction yields higher ambient particle concentration by about 15–25 % compared to conventional procedures – an improvement which can be considered as significant for many research applications. The calculated ξ-values are specifically related to the considered HALO underwing probe arrangement and may differ for other aircraft or instrument geometries. Moreover, the ξ-correction may not cover all impacts originating from high flight velocities and from interferences between the instruments and, e.g., the aircraft wings and/or fuselage. Consequently, it is important that PAS (as a function of TAS) is individually measured by each probe deployed underneath the wings of a fast-flying aircraft.

OCRA radiometric cloud fractions for GOME-2 on MetOp-A/B

This paper describes an approach for cloud parameter retrieval (radiometric cloud fraction estimation) using the polarization measurements of the Global Ozone Monitoring Experiment-2 (GOME-2) on-board the MetOp-A/B satellites. The core component of the Optical Cloud Recognition Algorithm (OCRA) is the calculation of monthly cloud-free reflectances for a global grid (resolution of 0.2° in longitude and 0.2° in latitude) and to derive radiometric cloud fractions. These cloud fractions will serve as a priori information for the retrieval of cloud top height (CTH), cloud top pressure (CTP), cloud top albedo (CTA) and cloud optical thickness (COT) with the Retrieval Of Cloud Information using Neural Networks (ROCINN) algorithm. This approach is already being implemented operationally for the GOME/ERS-2 and SCIAMACHY/ENVISAT sensors and here we present version 3.0 of the OCRA algorithm applied to the GOME-2 sensors. Based on more than six years of GOME-2A data (February 2007–June 2013), reflectances are calculated for &amp;approx; 35 000 orbits. For each measurement a degradation correction as well as a viewing angle dependent and latitude dependent correction is applied. In addition, an empirical correction scheme is introduced in order to remove the effect of oceanic sun glint. A comparison of the GOME-2A/B OCRA cloud fractions with co-located AVHRR geometrical cloud fractions shows a general good agreement with a mean difference of −0.15±0.20. From operational point of view, an advantage of the OCRA algorithm is its extremely fast computational time and its straightforward transferability to similar sensors like OMI (Ozone Monitoring Instrument), TROPOMI (TROPOspheric Monitoring Instrument) on Sentinel 5 Precursor, as well as Sentinel 4 and Sentinel 5. In conclusion, it is shown that a robust, accurate and fast radiometric cloud fraction estimation for GOME-2 can be achieved with OCRA by using the polarization measurement devices (PMDs).

The Aerosol Limb Imager: acousto-optic imaging of limb scattered sunlight for stratospheric aerosol profiling

The Aerosol Limb Imager (ALI) is an optical remote sensing instrument designed to image scattered sunlight from the atmospheric limb. These measurements are used to retrieve spatially resolved information of the stratospheric aerosol distribution, including spectral extinction coefficient and particle size. Here we present the design, development and test results of an ALI prototype instrument. The long term goal of this work is the eventual realization of ALI on a satellite platform in low earth orbit, where it can provide high spatial resolution observations, both in the vertical and cross-track. The instrument design uses a large aperture Acousto-Optic Tunable Filter (AOTF) to image the sunlit stratospheric limb in a selectable narrow wavelength band ranging from the visible to the near infrared. The ALI prototype was tested on a stratospheric balloon flight from the Canadian Space Agency (CSA) launch facility in Timmins, Canada, in September 2014. Preliminary analysis of the hyperspectral images indicate that the radiance measurements are of high quality, and we have used these to retrieve vertical profiles of stratospheric aerosol extinction coefficient from 650–1000 nm, along with one moment of the particle size distribution. Those preliminary results are promising and development of a satellite prototype of ALI within the Canadian Space Agency is ongoing.