ALBERT

Description: In this paper, we present the first multiyear time series of atmospheric ammonia (NH3) ground-based measurements in the Paris region (Créteil, 48.79∘ N, 2.44∘ E, France) retrieved with the midresolution “Observations of the Atmosphere by Solar absorption Infrared Spectroscopy” (OASIS) ground-based Fourier transform infrared solar observatory. Located in an urban region, OASIS has previously been used for monitoring air quality (tropospheric ozone and carbon monoxide) thanks to its specific column sensitivity across the whole troposphere down to the atmospheric boundary layer. A total of 4920 measurements of atmospheric total columns of ammonia have been obtained from 2009 to 2017, with uncertainties ranging from 20 % to 35 %, and have been compared with NH3 concentrations derived from the Infrared Atmospheric Sounding Interferometer (IASI). OASIS ground-based measurements show significant interannual and seasonal variabilities of atmospheric ammonia. NH3 total columns over the Paris megacity (12 million people) vary seasonally by 2 orders of magnitude from approximately 0.1×1016 molec. cm−2 in winter to 10×1016 molec. cm−2 for spring peaks, probably due to springtime spreading of fertilizers on surrounding croplands.

Description: Temperature, H2O, and O3 profiles, as well as CO2, N2O, CH4, chlorofluorocarbon-12 (CFC-12), and sea surface temperature (SST) scalar anomalies are computed using a clear subset of AIRS observations over ocean for the first 16 years of NASA's Earth-Observing Satellite (EOS) Aqua Atmospheric Infrared Sounder (AIRS) operation. The AIRS Level-1c radiances are averaged over 16 d and 40 equal-area zonal bins and then converted to brightness temperature anomalies. Geophysical anomalies are retrieved from the brightness temperature anomalies using a relatively standard optimal estimation approach. The CO2, N2O, CH4, and CFC-12 anomalies are derived by applying a vertically uniform multiplicative shift to each gas in order to obtain an estimate for the gas mixing ratio. The minor-gas anomalies are compared to the National Oceanic and Atmospheric Administration (NOAA) Earth System Research Laboratory (ESRL) in situ values and used to estimate the radiometric stability of the AIRS radiances. Similarly, the retrieved SST anomalies are compared to the SST values used in the ERA-Interim reanalysis and to NOAA's Optimum Interpolation SST (OISST) product. These intercomparisons strongly suggest that many AIRS channels are stable to better than 0.02 to 0.03 K per decade, well below climate trend levels, indicating that the AIRS blackbody is not drifting. However, detailed examination of the anomaly retrieval residuals (observed – computed) shows various small unphysical shifts that correspond to AIRS hardware events (shutdowns, etc.). Some examples are given highlighting how the AIRS radiance stability could be improved, especially for channels sensitive to N2O and CH4. The AIRS shortwave channels exhibit larger drifts that make them unsuitable for climate trending, and they are avoided in this work. The AIRS Level 2 surface temperature retrievals only use shortwave channels. We summarize how these shortwave drifts impacts recently published comparisons of AIRS surface temperature trends to other surface climatologies.

Description: Atmospheric mineral dust influences Earth's radiative budget, cloud formation, and lifetime; has adverse health effects; and affects air quality through the increase of regulatory PM10 concentrations, making its real-time quantification in the atmosphere of strategic importance. Only few near-real-time techniques can discriminate dust aerosol in PM10 samples and they are based on the dust chemical composition. The online determination of mineral dust using aerosol absorption photometers offers an interesting and competitive alternative but remains a difficult task to achieve. This is particularly challenging when dust is mixed with black carbon, which features a much higher mass absorption cross section. We build on previous work using filter photometers and present here for the first time a highly time-resolved online technique for quantification of mineral dust concentration by coupling a high-flow virtual impactor (VI) sampler that concentrates coarse particles with an aerosol absorption photometer (Aethalometer, model AE33). The absorption of concentrated dust particles is obtained by subtracting the absorption of the submicron (PM1) aerosol fraction from the absorption of the virtual impactor sample (VI-PM1 method). This real-time method for detecting desert dust was tested in the field for a period of 2 months (April and May 2016) at a regional background site of Cyprus, in the Eastern Mediterranean. Several intense desert mineral dust events were observed during the field campaign with dust concentration in PM10 up to 45 µg m−3. Mineral dust was present most of the time during the campaign with an average PM10 of about 8 µg m−3. Mineral dust absorption was most prominent at short wavelengths, yielding an average mass absorption cross section (MAC) of 0.24±0.01 m2 g−1 at 370 nm and an absorption Ångström exponent of 1.41±0.29. This MAC value can be used as a site-specific parameter for online determination of mineral dust concentration. The uncertainty of the proposed method is discussed by comparing and validating it with different methods.

Description: More than 300 non-dispersive infrared (NDIR) CO2 low-cost sensors labelled as LP8 were integrated into sensor units and evaluated for the purpose of long-term operation in the Carbosense CO2 sensor network in Switzerland. Prior to deployment, all sensors were calibrated in a pressure and climate chamber and in ambient conditions co-located with a reference instrument. To investigate their long-term performance and to test different data processing strategies, 18 sensors were deployed at five locations equipped with a reference instrument after calibration. Their accuracy during 19 to 25 months deployment was between 8 and 12 ppm. This level of accuracy requires careful sensor calibration prior to deployment, continuous monitoring of the sensors, efficient data filtering, and a procedure to correct drifts and jumps in the sensor signal during operation. High relative humidity (〉 ∼85 %) impairs the LP8 measurements, and corresponding data filtering results in a significant loss during humid conditions. The LP8 sensors are not suitable for the detection of small regional gradients and long-term trends. However, with careful data processing, the sensors are able to resolve CO2 changes and differences with a magnitude larger than about 30 ppm. Thereby, the sensor can resolve the site-specific CO2 signal at most locations in Switzerland. A low-power network (LPN) using LoRaWAN allowed for reliable data transmission with low energy consumption and proved to be a key element of the Carbosense low-cost sensor network.

Description: It is widely accepted that the atmospheric boundary layer is drastically under-sampled in the vertical dimension. In recent years, the commercial availability of ground-based remote sensors combined with the widespread use of small, weather-sensing uncrewed aerial systems (WxUAS) has opened up many opportunities to fill this measurement gap. In July 2018, the University of Oklahoma (OU) deployed a state-of-the-art WxUAS, dubbed the CopterSonde, and the Collaborative Lower Atmospheric Mobile Profiling System (CLAMPS) in the San Luis Valley in south-central Colorado. Additionally, these systems were deployed to the Kessler Atmospheric and Ecological Field Station (KAEFS) in October 2018. The colocation of these various systems provided ample opportunity to compare and contrast kinematic and thermodynamic observations from different methodologies of boundary layer profiling, namely WxUAS, remote sensing, and the traditional in situ radiosonde. In this study, temperature, dew point temperature, wind speed, and wind direction from these platforms are compared statistically with data from the two campaigns. Moreover, we present select instances from the dataset to highlight differences between the measurement techniques. This analysis highlights strengths and weaknesses of planetary boundary layer profiling and helps lay the groundwork for developing highly adaptable systems that integrate remote and in situ profiling techniques.

Description: An improved two-sphere integration (TSI) technique has been developed to quantify black carbon (BC) concentrations in the atmosphere and seasonal snow. The major advantage of this system is that it combines two distinct integrated spheres to reduce the scattering effect due to light-absorbing particles and thus provides accurate determinations of total light absorption from BC collected on Nuclepore filters. The TSI technique can be calibrated using a series of 15 filter samples of standard fullerene soot. This technique quantifies the mass of BC by separating the spectrally resolved total light absorption into BC and non-BC fractions. To assess the accuracy of the improved system, an empirical procedure for measuring BC concentrations with a two-step thermal–optical method is also applied. Laboratory results indicate that the BC concentrations determined using the TSI technique and theoretical calculations are well correlated (R2=0.99), whereas the thermal–optical method underestimates BC concentrations by 35 %–45 % compared to that measured by the TSI technique. Assessments of the two methods for atmospheric and snow samples revealed excellent agreement, with least-squares regression lines with slopes of 1.72 (r2=0.67) and 0.84 (r2=0.93), respectively. However, the TSI technique is more accurate in quantifications of BC concentrations in both the atmosphere and seasonal snow, with an overall lower uncertainty. Using the improved TSI technique, we find that light absorption at a wavelength of 550 nm due to BC plays a dominant role relative to non-BC light absorption in both the atmosphere (62.76 %–91.84 % of total light absorption) and seasonal snow (43.11 %–88.56 %) over northern China.

Description: Quantitative precipitation estimation with commercial microwave links (CMLs) is a technique developed to supplement weather radar and rain gauge observations. It is exploiting the relation between the attenuation of CML signal levels and the integrated rain rate along a CML path. The opportunistic nature of this method requires a sophisticated data processing using robust methods. In this study we focus on the processing step of rain event detection in the signal level time series of the CMLs, which we treat as a binary classification problem. This processing step is particularly challenging, because even when there is no rain, the signal level can show large fluctuations similar to that during rainy periods. False classifications can have a high impact on falsely estimated rainfall amounts. We analyze the performance of a convolutional neural network (CNN), which is trained to detect rainfall-specific attenuation patterns in CML signal levels, using data from 3904 CMLs in Germany. The CNN consists of a feature extraction and a classification part with, in total, 20 layers of neurons and 1.4×105 trainable parameters. With a structure inspired by the visual cortex of mammals, CNNs use local connections of neurons to recognize patterns independent of their location in the time series. We test the CNN's ability to recognize attenuation patterns from CMLs and time periods outside the training data. Our CNN is trained on 4 months of data from 800 randomly selected CMLs and validated on 2 different months of data, once for all CMLs and once for the 3104 CMLs not included in the training. No CMLs are excluded from the analysis. As a reference data set, we use the gauge-adjusted radar product RADOLAN-RW provided by the German meteorological service (DWD). The model predictions and the reference data are compared on an hourly basis. Model performance is compared to a state-of-the-art reference method, which uses the rolling standard deviation of the CML signal level time series as a detection criteria. Our results show that within the analyzed period of April to September 2018, the CNN generalizes well to the validation CMLs and time periods. A receiver operating characteristic (ROC) analysis shows that the CNN is outperforming the reference method, detecting on average 76 % of all rainy and 97 % of all nonrainy periods. From all periods with a reference rain rate larger than 0.6 mm h−1, more than 90 % was detected. We also show that the improved event detection leads to a significant reduction of falsely estimated rainfall by up to 51 %. At the same time, the quality of the correctly estimated rainfall is kept at the same level in regards to the Pearson correlation with the radar rainfall. In conclusion, we find that CNNs are a robust and promising tool to detect rainfall-induced attenuation patterns in CML signal levels from a large CML data set covering all of Germany.

Description: A new ion source (IS) utilizing vacuum ultraviolet (VUV) light is developed and characterized for use with iodide–chemical ionization mass spectrometers (I−-CIMS). The VUV-IS utilizes a compact krypton lamp that emits light at two wavelengths corresponding to energies of ∼10.030 and 10.641 eV. The VUV light photoionizes either methyl iodide (ionization potential, IP = 9.54 ± 0.02 eV) or benzene (IP = 9.24378 ± 0.00007 eV) to form cations and photoelectrons. The electrons react with methyl iodide to form I−, which serves as the reagent ion for the CIMS. The VUV-IS is characterized by measuring the sensitivity of a quadrupole CIMS (Q-CIMS) to formic acid, molecular chlorine, and nitryl chloride under a variety of flow and pressure conditions. The sensitivity of the Q-CIMS, with the VUV-IS, reached up to ∼700 Hz pptv−1, with detection limits of less than 1 pptv for a 1 min integration period. The reliability of the Q-CIMS with a VUV-IS is demonstrated with data from a month-long ground-based field campaign. The VUV-IS is further tested by operation on a high-resolution time-of-flight CIMS (TOF-CIMS). Sensitivities greater than 25 Hz pptv−1 were obtained for formic acid and molecular chlorine, which were similar to that obtained with a radioactive source. In addition, the mass spectra from sampling ambient air was cleaner with the VUV-IS on the TOF-CIMS compared to measurements using a radioactive source. These results demonstrate that the VUV lamp is a viable substitute for radioactive ion sources on I−-CIMS systems for most applications. In addition, initial tests demonstrate that the VUV-IS can be extended to other reagent ions by the use of VUV absorbers with low IPs to serve as a source of photoelectrons for high IP electron attachers, such as SF6-.

Description: The dynamic processing of aerosols in the atmosphere is difficult to mimic under laboratory conditions, particularly on a single-particle level with high spatial and chemical resolution. Our new microreactor system for X-ray microscopy facilitates observations under in situ conditions and extends the accessible parameter ranges of existing setups to very high humidities and low temperatures. With the parameter margins for pressure (180–1000 hPa), temperature (∼250 K to room temperature), and relative humidity (∼0 % to above 98 %), a wide range of tropospheric conditions is covered. Unique features are the mobile design and compact size that make the instrument applicable to different synchrotron facilities. Successful first experiments were conducted at two X-ray microscopes, MAXYMUS, located at beamline UE46 of the synchrotron BESSY II, and PolLux, located at beamline X07DA of the Swiss Light Source in the Paul Scherrer Institute. Here we present the design and analytical scope of the system, along with first results from hydration–dehydration experiments on ammonium sulfate and potassium sulfate particles and the tentative observation of water ice at low temperature and high relative humidity in a secondary organic aerosol particle from isoprene oxidation.

Description: In the last two decades, technological progress has not only seen improvements to the quality of atmospheric upper-air observations but also provided the opportunity to design and implement automated systems able to replace measurement procedures typically performed manually. Radiosoundings, which remain one of the primary data sources for weather and climate applications, are still largely performed around the world manually, although increasingly fully automated upper-air observations are used, from urban areas to the remotest locations, which minimize operating costs and challenges in performing radiosounding launches. This analysis presents a first step to demonstrating the reliability of the automatic radiosonde launchers (ARLs) provided by Vaisala, Meteomodem and Meisei. The metadata and datasets collected by a few existing ARLs operated by the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) certified or candidate sites (Sodankylä, Payerne, Trappes, Potenza) have been investigated and a comparative analysis of the technical performance (i.e. manual versus ARL) is reported. The performance of ARLs is evaluated as being similar or superior to those achieved with the traditional manual launches in terms of percentage of successful launches, balloon burst and ascent speed. For both temperature and relative humidity, the ground-check comparisons showed a negative bias of a few tenths of a degree and % RH, respectively. Two datasets of parallel soundings between manual and ARL-based measurements, using identical sonde models, provided by Sodankylä and Faa'a stations, showed mean differences between the ARL and manual launches smaller than ±0.2 K up to 10 hPa for the temperature profiles. For relative humidity, differences were smaller than 1 % RH for the Sodankylä dataset up to 300 hPa, while they were smaller than 0.7 % RH for Faa'a station. Finally, the observation-minus-background (O–B) mean and root mean square (rms) statistics for German RS92 and RS41 stations, which operate a mix of manual and ARL launch protocols, calculated using the European Centre for Medium-Range Weather Forecasts (ECMWF) forecast model, are very similar, although RS41 shows larger rms(O–B) differences for ARL stations, in particular for temperature and wind. A discussion of the potential next steps proposed by GRUAN community and other parties is provided, with the aim to lay the basis for the elaboration of a strategy to fully demonstrate the value of ARLs and guarantee that the provided products are traceable and suitable for the creation of GRUAN data products.