Showing papers in "Atmospheric Measurement Techniques in 2016"

Community Air Sensor Network (CAIRSENSE) project: Evaluation of low-cost sensor performance in a suburban environment in the southeastern United States

Abstract: . Advances in air pollution sensor technology have enabled the development of small and low-cost systems to measure outdoor air pollution. The deployment of a large number of sensors across a small geographic area would have potential benefits to supplement traditional monitoring networks with additional geographic and temporal measurement resolution, if the data quality were sufficient. To understand the capability of emerging air sensor technology, the Community Air Sensor Network (CAIRSENSE) project deployed low-cost, continuous, and commercially available air pollution sensors at a regulatory air monitoring site and as a local sensor network over a surrounding ∼ 2 km area in the southeastern United States. Collocation of sensors measuring oxides of nitrogen, ozone, carbon monoxide, sulfur dioxide, and particles revealed highly variable performance, both in terms of comparison to a reference monitor as well as the degree to which multiple identical sensors produced the same signal. Multiple ozone, nitrogen dioxide, and carbon monoxide sensors revealed low to very high correlation with a reference monitor, with Pearson sample correlation coefficient (r) ranging from 0.39 to 0.97, −0.25 to 0.76, and −0.40 to 0.82, respectively. The only sulfur dioxide sensor tested revealed no correlation (r 0.5), step-wise multiple linear regression was performed to determine if ambient temperature, relative humidity (RH), or age of the sensor in number of sampling days could be used in a correction algorithm to improve the agreement. Maximum improvement in agreement with a reference, incorporating all factors, was observed for an NO2 sensor (multiple correlation coefficient R2adj-orig = 0.57, R2adj-final = 0.81); however, other sensors showed no apparent improvement in agreement. A four-node sensor network was successfully able to capture ozone (two nodes) and PM (four nodes) data for an 8-month period of time and show expected diurnal concentration patterns, as well as potential ozone titration due to nearby traffic emissions. Overall, this study demonstrates the performance of emerging air quality sensor technologies in a real-world setting; the variable agreement between sensors and reference monitors indicates that in situ testing of sensors against benchmark monitors should be a critical aspect of all field studies.

The on-orbit performance of the Orbiting Carbon Observatory-2 (OCO-2) instrument and its radiometrically calibrated products

Abstract: . The Orbiting Carbon Observatory-2 (OCO-2) carries and points a three-channel imaging grating spectrometer designed to collect high-resolution, co-boresighted spectra of reflected sunlight within the molecular oxygen (O2) A-band at 0.765 microns and the carbon dioxide (CO2) bands at 1.61 and 2.06 microns. These measurements are calibrated and then combined into soundings that are analyzed to retrieve spatially resolved estimates of the column-averaged CO2 dry-air mole fraction, XCO2. Variations of XCO2 in space and time are then analyzed in the context of the atmospheric transport to quantify surface sources and sinks of CO2. This is a particularly challenging remote-sensing observation because all but the largest emission sources and natural absorbers produce only small ( To meet its demanding measurement requirements, each OCO-2 spectrometer channel collects 24 spectra s−1 across a narrow ( 17 000), dynamic range (∼ 104), and sensitivity (continuum signal-to-noise ratio > 400). The OCO-2 instrument performance was extensively characterized and calibrated prior to launch. In general, the instrument has performed as expected during its first 18 months in orbit. However, ongoing calibration and science analysis activities have revealed a number of subtle radiometric and spectroscopic challenges that affect the yield and quality of the OCO-2 data products. These issues include increased numbers of bad pixels, transient artifacts introduced by cosmic rays, radiance discontinuities for spatially non-uniform scenes, a misunderstanding of the instrument polarization orientation, and time-dependent changes in the throughput of the oxygen A-band channel. Here, we describe the OCO-2 instrument, its data products, and its on-orbit performance. We then summarize calibration challenges encountered during its first 18 months in orbit and the methods used to mitigate their impact on the calibrated radiance spectra distributed to the science community.

Comparisons of the Orbiting Carbon Observatory-2 (OCO-2) X CO 2 measurements with TCCON

Abstract: NASA's Orbiting Carbon Observatory-2 (OCO-2) has been measuring carbon dioxide column-averaged dry-air mole fraction, X_(CO_2), in the Earth's atmosphere for over 2 years. In this paper, we describe the comparisons between the first major release of the OCO-2 retrieval algorithm (B7r) and X_(CO2) from OCO-2's primary ground-based validation network: the Total Carbon Column Observing Network (TCCON). The OCO-2 X_(CO_2) retrievals, after filtering and bias correction, agree well when aggregated around and coincident with TCCON data in nadir, glint, and target observation modes, with absolute median differences less than 0.4 ppm and RMS differences less than 1.5 ppm. After bias correction, residual biases remain. These biases appear to depend on latitude, surface properties, and scattering by aerosols. It is thus crucial to continue measurement comparisons with TCCON to monitor and evaluate the OCO-2 X_(CO_2) data quality throughout its mission.

The automated multiwavelength Raman polarization and water-vapor lidar Polly XT : the neXT generation

Abstract: . The atmospheric science community demands autonomous and quality-assured vertically resolved measurements of aerosol and cloud properties. For this purpose, a portable lidar called Polly was developed at TROPOS in 2003. The lidar system was continuously improved with gained experience from the EARLINET community, involvement in worldwide field campaigns, and international institute collaborations within the last 10 years. Here we present recent changes of the setup of the portable multiwavelength Raman and polarization lidar PollyXT and discuss the improved capabilities of the system by means of a case study. The latest system developments include an additional near-range receiver unit for Raman measurements of the backscatter and extinction coefficient down to 120 m above ground, a water-vapor channel, and channels for simultaneous measurements of the particle linear depolarization ratio at 355 and 532 nm. Quality improvements were achieved by systematically following the EARLINET guidelines and the international PollyNET quality assurance developments. A modified ship radar ensures measurements in agreement with air-traffic safety regulations and allows for 24∕7 monitoring of the atmospheric state with PollyXT.

The GOME-2 instrument on the Metop series of satellites: instrument design, calibration, and level 1 data processing – an overview

Abstract: . The Global Ozone Monitoring Experiment-2 (GOME-2) flies on the Metop series of satellites, the space component of the EUMETSAT Polar System. In this paper we will provide an overview of the instrument design, the on-ground calibration and characterization activities, in-flight calibration, and level 0 to 1 data processing. The current status of the level 1 data is presented and points of specific relevance to users are highlighted. Long-term level 1 data consistency is also discussed and plans for future work are outlined. The information contained in this paper summarizes a large number of technical reports and related documents containing information that is not currently available in the published literature. These reports and documents are however made available on the EUMETSAT web pages and readers requiring more details than can be provided in this overview paper will find appropriate references at relevant points in the text.

The Orbiting Carbon Observatory-2: first 18 months of science data products

Abstract: . The Orbiting Carbon Observatory-2 (OCO-2) is the first National Aeronautics and Space Administration (NASA) satellite designed to measure atmospheric carbon dioxide (CO2) with the accuracy, resolution, and coverage needed to quantify CO2 fluxes (sources and sinks) on regional scales. OCO-2 was successfully launched on 2 July 2014 and has gathered more than 2 years of observations. The v7/v7r operational data products from September 2014 to January 2016 are discussed here. On monthly timescales, 7 to 12 % of these measurements are sufficiently cloud and aerosol free to yield estimates of the column-averaged atmospheric CO2 dry air mole fraction, XCO2, that pass all quality tests. During the first year of operations, the observing strategy, instrument calibration, and retrieval algorithm were optimized to improve both the data yield and the accuracy of the products. With these changes, global maps of XCO2 derived from the OCO-2 data are revealing some of the most robust features of the atmospheric carbon cycle. This includes XCO2 enhancements co-located with intense fossil fuel emissions in eastern US and eastern China, which are most obvious between October and December, when the north–south XCO2 gradient is small. Enhanced XCO2 coincident with biomass burning in the Amazon, central Africa, and Indonesia is also evident in this season. In May and June, when the north–south XCO2 gradient is largest, these sources are less apparent in global maps. During this part of the year, OCO-2 maps show a more than 10 ppm reduction in XCO2 across the Northern Hemisphere, as photosynthesis by the land biosphere rapidly absorbs CO2. As the carbon cycle science community continues to analyze these OCO-2 data, information on regional-scale sources (emitters) and sinks (absorbers) which impart XCO2 changes on the order of 1 ppm, as well as far more subtle features, will emerge from this high-resolution global dataset.

New methods for the retrieval of chlorophyll red fluorescence from hyperspectral satellite instruments: simulations andapplication to GOME-2 and SCIAMACHY

Abstract: . Global satellite measurements of solar-induced fluorescence (SIF) from chlorophyll over land and ocean have proven useful for a number of different applications related to physiology, phenology, and productivity of plants and phytoplankton. Terrestrial chlorophyll fluorescence is emitted throughout the red and far-red spectrum, producing two broad peaks near 683 and 736 nm. From ocean surfaces, phytoplankton fluorescence emissions are entirely from the red region (683 nm peak). Studies using satellite-derived SIF over land have focused almost exclusively on measurements in the far red (wavelengths > 712 nm), since those are the most easily obtained with existing instrumentation. Here, we examine new ways to use existing hyperspectral satellite data sets to retrieve red SIF (wavelengths

Review of the state of the art and future prospects of the ground-based GNSS meteorology in Europe

Abstract: . Global navigation satellite systems (GNSSs) have revolutionised positioning, navigation, and timing, becoming a common part of our everyday life. Aside from these well-known civilian and commercial applications, GNSS is now an established atmospheric observing system, which can accurately sense water vapour, the most abundant greenhouse gas, accounting for 60–70 % of atmospheric warming. In Europe, the application of GNSS in meteorology started roughly two decades ago, and today it is a well-established field in both research and operation. This review covers the state of the art in GNSS meteorology in Europe. The advances in GNSS processing for derivation of tropospheric products, application of GNSS tropospheric products in operational weather prediction and application of GNSS tropospheric products for climate monitoring are discussed. The GNSS processing techniques and tropospheric products are reviewed. A summary of the use of the products for validation and impact studies with operational numerical weather prediction (NWP) models as well as very short weather prediction (nowcasting) case studies is given. Climate research with GNSSs is an emerging field of research, but the studies so far have been limited to comparison with climate models and derivation of trends. More than 15 years of GNSS meteorology in Europe has already achieved outstanding cooperation between the atmospheric and geodetic communities. It is now feasible to develop next-generation GNSS tropospheric products and applications that can enhance the quality of weather forecasts and climate monitoring. This work is carried out within COST Action ES1206 advanced global navigation satellite systems tropospheric products for monitoring severe weather events and climate (GNSS4SWEC, http://gnss4swec.knmi.nl ).

A surface reflectance scheme for retrieving aerosol optical depth over urbansurfaces in MODIS Dark Target retrieval algorithm

Abstract: . The MODerate resolution Imaging Spectroradiometer (MODIS) instruments, aboard the two Earth Observing System (EOS) satellites Terra and Aqua, provide aerosol information with nearly daily global coverage at moderate spatial resolution (10 and 3 km). Almost 15 years of aerosol data records are now available from MODIS that can be used for various climate and air-quality applications. However, the application of MODIS aerosol products for air-quality concerns is limited by a reduction in retrieval accuracy over urban surfaces. This is largely because the urban surface reflectance behaves differently than that assumed for natural surfaces. In this study, we address the inaccuracies produced by the MODIS Dark Target (MDT) algorithm aerosol optical depth (AOD) retrievals over urban areas and suggest improvements by modifying the surface reflectance scheme in the algorithm. By integrating MODIS Land Surface Reflectance and Land Cover Type information into the aerosol surface parameterization scheme for urban areas, much of the issues associated with the standard algorithm have been mitigated for our test region, the continental United States (CONUS). The new surface scheme takes into account the change in underlying surface type and is only applied for MODIS pixels with urban percentage (UP) larger than 20 %. Over the urban areas where the new scheme has been applied (UP > 20 %), the number of AOD retrievals falling within expected error (EE %) has increased by 20 %, and the strong positive bias against ground-based sun photometry has been eliminated. However, we note that the new retrieval introduces a small negative bias for AOD values less than 0.1 due to the ultra-sensitivity of the AOD retrieval to the surface parameterization under low atmospheric aerosol loadings. Global application of the new urban surface parameterization appears promising, but further research and analysis are required before global implementation.

Update on GOSAT TANSO-FTS performance, operations, and data products after more than 6 years in space

Abstract: . A data set containing more than 6 years (February 2009 to present) of radiance spectra for carbon dioxide (CO2) and methane (CH4) observations has been acquired by the Greenhouse gases Observing SATellite (GOSAT, available at http://data.gosat.nies.go.jp/GosatUserInterfaceGateway/guig/GuigPage/open.do ), nicknamed “Ibuki”, Thermal And Near infrared Sensor for carbon Observation Fourier Transform Spectrometer (TANSO-FTS). This paper provides updates on the performance of the satellite and TANSO-FTS sensor and describes important changes to the data product, which has recently been made available to users. With these changes the typical accuracy of retrieved column-averaged dry air mole fractions of CO2 and CH4 (XCO2 and XCH4, respectively) are 2 ppm or 0.5 % and 13 ppb or 0.7 %, respectively. Three major anomalies of the satellite system affecting TANSO-FTS are reported: a failure of one of the two solar paddles in May 2014, a switch to the secondary pointing system in January 2015, and most recently a cryocooler shutdown and restart in August 2015. The Level 1A (L1A) (raw interferogram) and the Level 1B (L1B) (radiance spectra) of version V201 described here have long-term uniform quality and provide consistent retrieval accuracy even after the satellite system anomalies. In addition, we discuss the unique observation abilities of GOSAT made possible by an agile pointing mechanism, which allows for optimization of global sampling patterns.

Structural uncertainty in air mass factor calculation for NO2 and HCHO satellite retrievals

Abstract: . Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (

Constraining the sensitivity of iodide adduct chemical ionization mass spectrometry to multifunctional organic molecules using the collision limit and thermodynamic stability of iodide ion adducts

Abstract: . The sensitivity of a chemical ionization mass spectrometer (ions formed per number density of analytes) is fundamentally limited by the collision frequency between reagent ions and analytes, known as the collision limit, the ion–molecule reaction time, and the transmission efficiency of product ions to the detector. We use the response of a time-of-flight chemical ionization mass spectrometer (ToF-CIMS) to N2O5, known to react with iodide at the collision limit, to constrain the combined effects of ion–molecule reaction time, which is strongly influenced by mixing and ion losses in the ion–molecule reaction drift tube. A mass spectrometric voltage scanning procedure elucidates the relative binding energies of the ion adducts, which influence the transmission efficiency of molecular ions through the electric fields within the vacuum chamber. Together, this information provides a critical constraint on the sensitivity of a ToF-CIMS towards a wide suite of routinely detected multifunctional organic molecules for which no calibration standards exist. We describe the scanning procedure and collision limit determination, and we show results from the application of these constraints to the measurement of organic aerosol composition at two different field locations.

Sulfur dioxide retrievals from TROPOMI onboard Sentinel-5 Precursor: algorithm theoretical basis

Abstract: . The TROPOspheric Monitoring Instrument (TROPOMI) onboard the Copernicus Sentinel-5 Precursor (S-5P) platform will measure ultraviolet earthshine radiances at high spectral and improved spatial resolution (pixel size of 7 km × 3.5 km at nadir) compared to its predecessors OMI and GOME-2. This paper presents the sulfur dioxide (SO2) vertical column retrieval algorithm implemented in the S-5P operational processor UPAS (Universal Processor for UV/VIS Atmospheric Spectrometers) and comprehensively describes its various retrieval steps. The spectral fitting is performed using the differential optical absorption spectroscopy (DOAS) method including multiple fitting windows to cope with the large range of atmospheric SO2 columns encountered. It is followed by a slant column background correction scheme to reduce possible biases or across-track-dependent artifacts in the data. The SO2 vertical columns are obtained by applying air mass factors (AMFs) calculated for a set of representative a priori profiles and accounting for various parameters influencing the retrieval sensitivity to SO2. Finally, the algorithm includes an error analysis module which is fully described here. We also discuss verification results (as part of the algorithm development) and future validation needs of the TROPOMI SO2 algorithm.

About the effects of polarising optics on lidar signals and the Δ90 calibration

Abstract: . This paper provides a model for assessing the effects of polarising optics on the signals of typical lidar systems, which is based on the description of the individual optical elements of the lidar and of the state of polarisation of the light by means of the Muller–Stokes formalism. General analytical equations are derived for the dependence of the lidar signals on polarisation parameters, for the linear depolarisation ratio, and for the signals of different polarisation calibration setups. The equations can also be used for the calculation of systematic errors caused by nonideal optical elements, their rotational misalignment, and by non-ideal laser polarisation. We present the description of the lidar signals including the polarisation calibration in a closed form, which can be applied for a large variety of lidar systems.

Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

Abstract: . Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 µm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60–91 %) achieved using this technique, together with low detection limits (0.8 µg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.

The uncertainty of the atmospheric integrated water vapour estimated from GNSS observations

Abstract: . Within the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) there is a need for an assessment of the uncertainty in the integrated water vapour (IWV) in the atmosphere estimated from ground-based global navigation satellite system (GNSS) observations. All relevant error sources in GNSS-derived IWV are therefore essential to be investigated. We present two approaches, a statistical and a theoretical analysis, for the assessment of the uncertainty of the IWV. The method is valuable for all applications of GNSS IWV data in atmospheric research and weather forecast. It will be implemented to the GNSS IWV data stream for GRUAN in order to assign a specific uncertainty to each data point. In addition, specific recommendations are made to GRUAN on hardware, software, and data processing practices to minimise the IWV uncertainty. By combining the uncertainties associated with the input variables in the estimations of the IWV, we calculated the IWV uncertainties for several GRUAN sites with different weather conditions. The results show a similar relative importance of all uncertainty contributions where the uncertainties in the zenith total delay (ZTD) dominate the error budget of the IWV, contributing over 75 % of the total IWV uncertainty. The impact of the uncertainty associated with the conversion factor between the IWV and the zenith wet delay (ZWD) is proportional to the amount of water vapour and increases slightly for moist weather conditions. The GRUAN GNSS IWV uncertainty data will provide a quantified confidence to be used for the validation of other measurement techniques.

Ground-based assessment of the bias and long-term stability of 14 limb and occultation ozone profile data records

Abstract: The ozone profile records of a large number of limb and occultation satellite instruments are widely used to address several key questions in ozone research. Further progress in some domains depends on a more detailed understanding of these data sets, especially of their long-term stability and their mutual consistency. To this end, we make a systematic assessment of fourteen limb and occultation sounders that, together, provide more than three decades of global ozone profile measurements. In particular, we consider the latest operational Level-2 records by SAGE II, SAGE III, HALOE, UARS MLS, Aura MLS, POAM II, POAM III, OSIRIS, SMR, GOMOS, MIPAS, SCIAMACHY, ACE-FTS and MAESTRO. Central to our work is a harmonized and robust analysis of the comparisons against the ground-based ozonesonde and stratospheric ozone lidar networks. It allows us to investigate, from the ground up to the stratopause, the following main aspects of data quality: long-term stability, overall bias, and short-term variability, together with their dependence on geophysical parameters and profile representation. In addition, it permits us to quantify the overall consistency between the ozone profilers. Generally, we find that between 20–40 km, the satellite ozone measurement biases are smaller than ±5 %, the short-term variabilities are better than 5–12 % and the drifts are at most ±5 % decade−1 (and ±3 % decade−1 for a few records). The agreement with ground-based data degrades somewhat towards the stratopause and especially towards the tropopause, where natural variability and low ozone abundancies impede a more precise analysis. A few records deviate from the preceding general remarks, in part of the stratosphere; we identify biases of 10 % and more (POAM II and SCIAMACHY), markedly higher single-profile variability (SMR and SCIAMACHY), and significant long-term drifts (SCIAMACHY, OSIRIS, HALOE, and possibly GOMOS and SMR as well). Furthermore, we reflect on the repercussions of our findings for the construction, analysis and interpretation of merged data records. Most notably, the discrepancies between several recent ozone profile trend assessments can be mostly explained by instrumental drift. This clearly demonstrates the need for systematic comprehensive multi-instrument comparison analyses.

Recommendations for processing atmospheric attenuated backscatter profiles from Vaisala CL31 ceilometers

Abstract: . Ceilometer lidars are used for cloud base height detection, to probe aerosol layers in the atmosphere (e.g. detection of elevated layers of Saharan dust or volcanic ash), and to examine boundary layer dynamics. Sensor optics and acquisition algorithms can strongly influence the observed attenuated backscatter profiles; therefore, physical interpretation of the profiles requires careful application of corrections. This study addresses the widely deployed Vaisala CL31 ceilometer. Attenuated backscatter profiles are studied to evaluate the impact of both the hardware generation and firmware version. In response to this work and discussion within the CL31/TOPROF user community (TOPROF, European COST Action aiming to harmonise ground-based remote sensing networks across Europe), Vaisala released new firmware (versions 1.72 and 2.03) for the CL31 sensors. These firmware versions are tested against previous versions, showing that several artificial features introduced by the data processing have been removed. Hence, it is recommended to use this recent firmware for analysing attenuated backscatter profiles. To allow for consistent processing of historic data, correction procedures have been developed that account for artefacts detected in data collected with older firmware. Furthermore, a procedure is proposed to determine and account for the instrument-related background signal from electronic and optical components. This is necessary for using attenuated backscatter observations from any CL31 ceilometer. Recommendations are made for the processing of attenuated backscatter observed with Vaisala CL31 sensors, including the estimation of noise which is not provided in the standard CL31 output. After taking these aspects into account, attenuated backscatter profiles from Vaisala CL31 ceilometers are considered capable of providing valuable information for a range of applications including atmospheric boundary layer studies, detection of elevated aerosol layers, and model verification.

LOAC: a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles – Part 1: Principle of measurements and instrument evaluation

Abstract: The study of aerosols in the troposphere and in the stratosphere is of major importance both for climate and air quality studies. Among the numerous instruments available, optical aerosol particles counters (OPCs) provide the size distribution in diameter range from about 100 nm to a few tens of µm. Most of them are very sensitive to the nature of aerosols, and this can result in significant biases in the retrieved size distribution. We describe here a new versatile optical particle/sizer counter named LOAC (Light Optical Aerosol Counter), which is light and compact enough to perform measurements not only at the surface but under all kinds of balloons in the troposphere and in the stratosphere. LOAC is an original OPC performing observations at two scattering angles. The first one is around 12°, and is almost insensitive to the refractive index of the particles; the second one is around 60° and is strongly sensitive to the refractive index of the particles. By combining measurement at the two angles, it is possible to retrieve the size distribution between 0.2 and 100 µm and to estimate the nature of the dominant particles (droplets, carbonaceous, salts and mineral particles) when the aerosol is relatively homogeneous. This typology is based on calibration charts obtained in the laboratory. The uncertainty for total concentrations measurements is ±20% when concentrations are higher than 1 particle cm-3 (for a 10 min integration time). For lower concentrations, the uncertainty is up to about ±60% for concentrations smaller than 10-2 particle cm-3. Also, the uncertainties in size calibration are ±0.025 μm for particles smaller than 0.6 μm, 5% for particles in the 0.7-2 μm range, and 10% for particles greater than 2 μm. The measurement accuracy of submicronic particles could be reduced in a strongly turbid case when concentration of particles > 3 µm exceeds a few particles cm-3. Several campaigns of cross-comparison of LOAC with other particle counting instruments and remote sensing photometers have been conducted to validate both the size distribution derived by LOAC and the retrieved particle number density. The typology of the aerosols has been validated in well-defined conditions including urban pollution, desert dust episodes, sea spray, fog, and cloud. Comparison with reference aerosol mass monitoring instruments also shows that the LOAC measurements can be successfully converted to mass concentrations.

Carbon monoxide total column retrievals from TROPOMI shortwave infrared measurements

Abstract: . The Tropospheric Monitoring Instrument (TROPOMI) spectrometer is the single payload of the Copernicus Sentinel 5 Precursor (S5P) mission. It measures Earth radiance spectra in the shortwave infrared spectral range around 2.3 µm with a dedicated instrument module. These measurements provide carbon monoxide (CO) total column densities over land, which for clear sky conditions are highly sensitive to the tropospheric boundary layer. For cloudy atmospheres over land and ocean, the column sensitivity changes according to the light path through the atmosphere. In this study, we present the physics-based operational S5P algorithm to infer atmospheric CO columns satisfying the envisaged accuracy (

GOCI Yonsei Aerosol Retrieval (YAER) algorithm and validation during the DRAGON-NE Asia 2012 campaign

Abstract: . The Geostationary Ocean Color Imager (GOCI) onboard the Communication, Ocean, and Meteorological Satellite (COMS) is the first multi-channel ocean color imager in geostationary orbit. Hourly GOCI top-of-atmosphere radiance has been available for the retrieval of aerosol optical properties over East Asia since March 2011. This study presents improvements made to the GOCI Yonsei Aerosol Retrieval (YAER) algorithm together with validation results during the Distributed Regional Aerosol Gridded Observation Networks – Northeast Asia 2012 campaign (DRAGON-NE Asia 2012 campaign). The evaluation during the spring season over East Asia is important because of high aerosol concentrations and diverse types of Asian dust and haze. Optical properties of aerosol are retrieved from the GOCI YAER algorithm including aerosol optical depth (AOD) at 550 nm, fine-mode fraction (FMF) at 550 nm, single-scattering albedo (SSA) at 440 nm, Angstrom exponent (AE) between 440 and 860 nm, and aerosol type. The aerosol models are created based on a global analysis of the Aerosol Robotic Networks (AERONET) inversion data, and covers a broad range of size distribution and absorptivity, including nonspherical dust properties. The Cox–Munk ocean bidirectional reflectance distribution function (BRDF) model is used over ocean, and an improved minimum reflectance technique is used over land. Because turbid water is persistent over the Yellow Sea, the land algorithm is used for such cases. The aerosol products are evaluated against AERONET observations and MODIS Collection 6 aerosol products retrieved from Dark Target (DT) and Deep Blue (DB) algorithms during the DRAGON-NE Asia 2012 campaign conducted from March to May 2012. Comparison of AOD from GOCI and AERONET resulted in a Pearson correlation coefficient of 0.881 and a linear regression equation with GOCI AOD = 1.083 × AERONET AOD − 0.042. The correlation between GOCI and MODIS AODs is higher over ocean than land. GOCI AOD shows better agreement with MODIS DB than MODIS DT. The other GOCI YAER products (AE, FMF, and SSA) show lower correlation with AERONET than AOD, but still show some skills for qualitative use.

Consistent evaluation of ACOS-GOSAT, BESD-SCIAMACHY, CarbonTracker, and MACC through comparisons to TCCON

Abstract: . Consistent validation of satellite CO2 estimates is a prerequisite for using multiple satellite CO2 measurements for joint flux inversion, and for establishing an accurate long-term atmospheric CO2 data record. Harmonizing satellite CO2 measurements is particularly important since the differences in instruments, observing geometries, sampling strategies, etc. imbue different measurement characteristics in the various satellite CO2 data products. We focus on validating model and satellite observation attributes that impact flux estimates and CO2 assimilation, including accurate error estimates, correlated and random errors, overall biases, biases by season and latitude, the impact of coincidence criteria, validation of seasonal cycle phase and amplitude, yearly growth, and daily variability. We evaluate dry-air mole fraction (XCO2) for Greenhouse gases Observing SATellite (GOSAT) (Atmospheric CO2 Observations from Space, ACOS b3.5) and SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) (Bremen Optimal Estimation DOAS, BESD v2.00.08) as well as the CarbonTracker (CT2013b) simulated CO2 mole fraction fields and the Monitoring Atmospheric Composition and Climate (MACC) CO2 inversion system (v13.1) and compare these to Total Carbon Column Observing Network (TCCON) observations (GGG2012/2014). We find standard deviations of 0.9, 0.9, 1.7, and 2.1 ppm vs. TCCON for CT2013b, MACC, GOSAT, and SCIAMACHY, respectively, with the single observation errors 1.9 and 0.9 times the predicted errors for GOSAT and SCIAMACHY, respectively. We quantify how satellite error drops with data averaging by interpreting according to error2 = a2 + b2/n (with n being the number of observations averaged, a the systematic (correlated) errors, and b the random (uncorrelated) errors). a and b are estimated by satellites, coincidence criteria, and hemisphere. Biases at individual stations have year-to-year variability of ∼ 0.3 ppm, with biases larger than the TCCON-predicted bias uncertainty of 0.4 ppm at many stations. We find that GOSAT and CT2013b underpredict the seasonal cycle amplitude in the Northern Hemisphere (NH) between 46 and 53° N, MACC overpredicts between 26 and 37° N, and CT2013b underpredicts the seasonal cycle amplitude in the Southern Hemisphere (SH). The seasonal cycle phase indicates whether a data set or model lags another data set in time. We find that the GOSAT measurements improve the seasonal cycle phase substantially over the prior while SCIAMACHY measurements improve the phase significantly for just two of seven sites. The models reproduce the measured seasonal cycle phase well except for at Lauder_125HR (CT2013b) and Darwin (MACC). We compare the variability within 1 day between TCCON and models in JJA; there is correlation between 0.2 and 0.8 in the NH, with models showing 10–50 % the variability of TCCON at different stations and CT2013b showing more variability than MACC. This paper highlights findings that provide inputs to estimate flux errors in model assimilations, and places where models and satellites need further investigation, e.g., the SH for models and 45–67° N for GOSAT and CT2013b.

A broadband cavity enhanced absorption spectrometer for aircraft measurements of glyoxal, methylglyoxal, nitrous acid, nitrogen dioxide, and water vapor

Abstract: . We describe a two-channel broadband cavity enhanced absorption spectrometer (BBCEAS) for aircraft measurements of glyoxal (CHOCHO), methylglyoxal (CH3COCHO), nitrous acid (HONO), nitrogen dioxide (NO2), and water (H2O). The instrument spans 361–389 and 438–468 nm, using two light-emitting diodes (LEDs) and a single grating spectrometer with a charge-coupled device (CCD) detector. Robust performance is achieved using a custom optical mounting system, high-power LEDs with electronic on/off modulation, high-reflectivity cavity mirrors, and materials that minimize analyte surface losses. We have successfully deployed this instrument during two aircraft and two ground-based field campaigns to date. The demonstrated precision (2σ) for retrievals of CHOCHO, HONO and NO2 are 34, 350, and 80 parts per trillion (pptv) in 5 s. The accuracy is 5.8, 9.0, and 5.0 %, limited mainly by the available absorption cross sections.

Statistical framework for estimating GNSS bias

Abstract: . We present a statistical framework for estimating global navigation satellite system (GNSS) non-ionospheric differential time delay bias. The biases are estimated by examining differences of measured line-integrated electron densities (total electron content: TEC) that are scaled to equivalent vertical integrated densities. The spatiotemporal variability, instrumentation-dependent errors, and errors due to inaccurate ionospheric altitude profile assumptions are modeled as structure functions. These structure functions determine how the TEC differences are weighted in the linear least-squares minimization procedure, which is used to produce the bias estimates. A method for automatic detection and removal of outlier measurements that do not fit into a model of receiver bias is also described. The same statistical framework can be used for a single receiver station, but it also scales to a large global network of receivers. In addition to the Global Positioning System (GPS), the method is also applicable to other dual-frequency GNSS systems, such as GLONASS (Globalnaya Navigazionnaya Sputnikovaya Sistema). The use of the framework is demonstrated in practice through several examples. A specific implementation of the methods presented here is used to compute GPS receiver biases for measurements in the MIT Haystack Madrigal distributed database system. Results of the new algorithm are compared with the current MIT Haystack Observatory MAPGPS (MIT Automated Processing of GPS) bias determination algorithm. The new method is found to produce estimates of receiver bias that have reduced day-to-day variability and more consistent coincident vertical TEC values.

The operational methane retrieval algorithm for TROPOMI

Abstract: . This work presents the operational methane retrieval algorithm for the Sentinel 5 Precursor (S5P) satellite and its performance tested on realistic ensembles of simulated measurements. The target product is the column-averaged dry air volume mixing ratio of methane (XCH4), which will be retrieved simultaneously with scattering properties of the atmosphere. The algorithm attempts to fit spectra observed by the shortwave and near-infrared channels of the TROPOspheric Monitoring Instrument (TROPOMI) spectrometer aboard S5P. The sensitivity of the retrieval performance to atmospheric scattering properties, atmospheric input data and instrument calibration errors is evaluated. In addition, we investigate the effect of inhomogeneous slit illumination on the instrument spectral response function. Finally, we discuss the cloud filters to be used operationally and as backup. We show that the required accuracy and precision of

Lidar-Radiometer Inversion Code (LIRIC) for the retrieval of vertical aerosol properties from combined lidar/radiometer data: development and distribution in EARLINET

Abstract: . This paper presents a detailed description of LIRIC (LIdar-Radiometer Inversion Code) algorithm for simultaneous processing of coincident lidar and radiometric (sun photometric) observations for the retrieval of the aerosol concentration vertical profiles. As the lidar/radiometric input data we use measurements from European Aerosol Research Lidar Network (EARLINET) lidars and collocated sun-photometers of Aerosol Robotic Network (AERONET). The LIRIC data processing provides sequential inversion of the combined lidar and radiometric data. The algorithm starts with the estimations of column-integrated aerosol parameters from radiometric measurements followed by the retrieval of height dependent concentrations of fine and coarse aerosols from lidar signals using integrated column characteristics of aerosol layer as a priori constraints. The use of polarized lidar observations allows us to discriminate between spherical and non-spherical particles of the coarse aerosol mode. The LIRIC software package was implemented and tested at a number of EARLINET stations. Intercomparison of the LIRIC-based aerosol retrievals was performed for the observations by seven EARLINET lidars in Leipzig, Germany on 25 May 2009. We found close agreement between the aerosol parameters derived from different lidars that supports high robustness of the LIRIC algorithm. The sensitivity of the retrieval results to the possible reduction of the available observation data is also discussed.

Characterization of the mass-dependent transmission efficiency of a CIMS

Abstract: . Knowledge about mass discrimination effects in a chemical ionization mass spectrometer (CIMS) is crucial for quantifying, e.g., the recently discovered extremely low volatile organic compounds (ELVOCs) and other compounds for which no calibration standard exists so far. Here, we present a simple way of estimating mass discrimination effects of a nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer. Characterization of the mass discrimination is achieved by adding different perfluorinated acids to the mass spectrometer in amounts sufficient to deplete the primary ions significantly. The relative transmission efficiency can then be determined by comparing the decrease of signals from the primary ions and the increase of signals from the perfluorinated acids at higher masses. This method is in use already for PTR-MS; however, its application to a CI-APi-TOF brings additional difficulties, namely clustering and fragmentation of the measured compounds, which can be treated with statistical analysis of the measured data, leading to self-consistent results. We also compare this method to a transmission estimation obtained with a setup using an electrospray ion source, a high-resolution differential mobility analyzer and an electrometer, which estimates the transmission of the instrument without the CI source. Both methods give different transmission curves, indicating non-negligible mass discrimination effects of the CI source. The absolute transmission of the instrument without the CI source was estimated with the HR-DMA method to plateau between the m∕z range of 127 and 568 Th at around 1.5 %; however, for the CI source included, the depletion method showed a steady increase in relative transmission efficiency from the m∕z range of the primary ion (mainly at 62 Th) to around 550 Th by a factor of around 5. The main advantages of the depletion method are that the instrument is used in the same operation mode as during standard measurements and no knowledge of the absolute amount of the measured substance is necessary, which results in a simple setup.

Chamber catalogues of optical and fluorescent signatures distinguishbioaerosol classes

Abstract: . Rapid bioaerosol characterization has immediate applications in the military, environmental and public health sectors. Recent technological advances have facilitated single-particle detection of fluorescent aerosol in near real time; this leverages controlled ultraviolet exposures with single or multiple wavelengths, followed by the characterization of associated fluorescence. This type of ultraviolet induced fluorescence has been used to detect airborne microorganisms and their fragments in laboratory studies, and it has been extended to field studies that implicate bioaerosol to compose a substantial fraction of supermicron atmospheric particles. To enhance the information yield that new-generation fluorescence instruments can provide, we report the compilation of a referential aerobiological catalogue including more than 50 pure cultures of common airborne bacteria, fungi and pollens, recovered at water activity equilibrium in a mesoscale chamber (1 m3). This catalogue juxtaposes intrinsic optical properties and select bandwidths of fluorescence emissions, which manifest to clearly distinguish between major classes of airborne microbes and pollens.

Orbiting Carbon Observatory-2 (OCO-2) cloud screening algorithms: validation against collocated MODIS and CALIOP data

Abstract: . The objective of the National Aeronautics and Space Administration's (NASA) Orbiting Carbon Observatory-2 (OCO-2) mission is to retrieve the column-averaged carbon dioxide (CO2) dry air mole fraction (XCO2) from satellite measurements of reflected sunlight in the near-infrared. These estimates can be biased by clouds and aerosols, i.e., contamination, within the instrument's field of view. Screening of the most contaminated soundings minimizes unnecessary calls to the computationally expensive Level 2 (L2) XCO2 retrieval algorithm. Hence, robust cloud screening methods have been an important focus of the OCO-2 algorithm development team. Two distinct, computationally inexpensive cloud screening algorithms have been developed for this application. The A-Band Preprocessor (ABP) retrieves the surface pressure using measurements in the 0.76 µm O2 A band, neglecting scattering by clouds and aerosols, which introduce photon path-length differences that can cause large deviations between the expected and retrieved surface pressure. The Iterative Maximum A Posteriori (IMAP) Differential Optical Absorption Spectroscopy (DOAS) Preprocessor (IDP) retrieves independent estimates of the CO2 and H2O column abundances using observations taken at 1.61 µm (weak CO2 band) and 2.06 µm (strong CO2 band), while neglecting atmospheric scattering. The CO2 and H2O column abundances retrieved in these two spectral regions differ significantly in the presence of cloud and scattering aerosols. The combination of these two algorithms, which are sensitive to different features in the spectra, provides the basis for cloud screening of the OCO-2 data set. To validate the OCO-2 cloud screening approach, collocated measurements from NASA's Moderate Resolution Imaging Spectrometer (MODIS), aboard the Aqua platform, were compared to results from the two OCO-2 cloud screening algorithms. With tuning of algorithmic threshold parameters that allows for processing of ≃ 20–25 % of all OCO-2 soundings, agreement between the OCO-2 and MODIS cloud screening methods is found to be ≃ 85 % over four 16-day orbit repeat cycles in both the winter (December) and spring (April–May) for OCO-2 nadir-land, glint-land and glint-water observations. No major, systematic, spatial or temporal dependencies were found, although slight differences in the seasonal data sets do exist and validation is more problematic with increasing solar zenith angle and when surfaces are covered in snow and ice and have complex topography. To further analyze the performance of the cloud screening algorithms, an initial comparison of OCO-2 observations was made to collocated measurements from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). These comparisons highlight the strength of the OCO-2 cloud screening algorithms in identifying high, thin clouds but suggest some difficulty in identifying some clouds near the surface, even when the optical thicknesses are greater than 1.

New-generation NASA Aura Ozone Monitoring Instrument (OMI) volcanic SO 2 dataset: algorithm description, initial results, and continuation with the Suomi-NPP Ozone Mapping and Profiler Suite (OMPS)

Abstract: . Since the fall of 2004, the Ozone Monitoring Instrument (OMI) has been providing global monitoring of volcanic SO2 emissions, helping to understand their climate impacts and to mitigate aviation hazards. Here we introduce a new-generation OMI volcanic SO2 dataset based on a principal component analysis (PCA) retrieval technique. To reduce retrieval noise and artifacts as seen in the current operational linear fit (LF) algorithm, the new algorithm, OMSO2VOLCANO, uses characteristic features extracted directly from OMI radiances in the spectral fitting, thereby helping to minimize interferences from various geophysical processes (e.g., O3 absorption) and measurement details (e.g., wavelength shift). To solve the problem of low bias for large SO2 total columns in the LF product, the OMSO2VOLCANO algorithm employs a table lookup approach to estimate SO2 Jacobians (i.e., the instrument sensitivity to a perturbation in the SO2 column amount) and iteratively adjusts the spectral fitting window to exclude shorter wavelengths where the SO2 absorption signals are saturated. To first order, the effects of clouds and aerosols are accounted for using a simple Lambertian equivalent reflectivity approach. As with the LF algorithm, OMSO2VOLCANO provides total column retrievals based on a set of predefined SO2 profiles from the lower troposphere to the lower stratosphere, including a new profile peaked at 13 km for plumes in the upper troposphere. Examples given in this study indicate that the new dataset shows significant improvement over the LF product, with at least 50 % reduction in retrieval noise over the remote Pacific. For large eruptions such as Kasatochi in 2008 (∼ 1700 kt total SO2) and Sierra Negra in 2005 (> 1100 DU maximum SO2), OMSO2VOLCANO generally agrees well with other algorithms that also utilize the full spectral content of satellite measurements, while the LF algorithm tends to underestimate SO2. We also demonstrate that, despite the coarser spatial and spectral resolution of the Suomi National Polar-orbiting Partnership (Suomi-NPP) Ozone Mapping and Profiler Suite (OMPS) instrument, application of the new PCA algorithm to OMPS data produces highly consistent retrievals between OMI and OMPS. The new PCA algorithm is therefore capable of continuing the volcanic SO2 data record well into the future using current and future hyperspectral UV satellite instruments.