Slant Column Research Articles

Intercomparison of Pandora stratospheric NO<sub>2</sub> slant column product with the NDACC-certified M07 spectrometer in Lauder, New Zealand

Abstract. In September 2014, a Pandora multi-spectral photometer operated by the SAGE-III project was sent to Lauder, New Zealand, to operate side-by-side with the National Institute of Water and Atmospheric Research's (NIWA) Network for Detection of Atmospheric Composition Change (NDACC) certified zenith slant column NO2 instrument to allow intercomparison between the two instruments and for evaluation of the Pandora unit as a potential SAGE-III validation tool for stratospheric NO2. This intercomparison spanned a full year, from September 2014 to September 2015. Both datasets were produced using their respective native algorithms using a common reference spectrum (i.e., 12:00 NZDT (UTC + 13) on 26 February 2015). Throughout the entire deployment period both instruments operated in a zenith-only observation configuration. Though conversion from slant column density (SCD) to vertical-column density is routine (by application of an air mass factor), we limit the current analysis to SCD only. This omission is beneficial in that it provides an intercomparison based on similar modes of operation for the two instruments and the retrieval algorithms as opposed to introducing an air mass factor dependence in the intercomparison as well. It was observed that the current hardware configurations and retrieval algorithms are in good agreement (R > 0.95). The detailed results of this investigation are presented herein.

MAX-DOAS measurements of HONO slant column densities during the MAD-CAT campaign: inter-comparison, sensitivity studies on spectral analysis settings, and error budget

Abstract. In order to promote the development of the passive DOAS technique the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) was held at the Max Planck Institute for Chemistry in Mainz, Germany, from June to October 2013. Here, we systematically compare the differential slant column densities (dSCDs) of nitrous acid (HONO) derived from measurements of seven different instruments. We also compare the tropospheric difference of SCDs (delta SCD) of HONO, namely the difference of the SCDs for the non-zenith observations and the zenith observation of the same elevation sequence. Different research groups analysed the spectra from their own instruments using their individual fit software. All the fit errors of HONO dSCDs from the instruments with cooled large-size detectors are mostly in the range of 0.1 to 0.3 × 1015 molecules cm−2 for an integration time of 1 min. The fit error for the mini MAX-DOAS is around 0.7 × 1015 molecules cm−2. Although the HONO delta SCDs are normally smaller than 6 × 1015 molecules cm−2, consistent time series of HONO delta SCDs are retrieved from the measurements of different instruments. Both fits with a sequential Fraunhofer reference spectrum (FRS) and a daily noon FRS lead to similar consistency. Apart from the mini-MAX-DOAS, the systematic absolute differences of HONO delta SCDs between the instruments are smaller than 0.63 × 1015 molecules cm−2. The correlation coefficients are higher than 0.7 and the slopes of linear regressions deviate from unity by less than 16 % for the elevation angle of 1°. The correlations decrease with an increase in elevation angle. All the participants also analysed synthetic spectra using the same baseline DOAS settings to evaluate the systematic errors of HONO results from their respective fit programs. In general the errors are smaller than 0.3 × 1015 molecules cm−2, which is about half of the systematic difference between the real measurements.The differences of HONO delta SCDs retrieved in the selected three spectral ranges 335–361, 335–373 and 335–390 nm are considerable (up to 0.57 × 1015 molecules cm−2) for both real measurements and synthetic spectra. We performed sensitivity studies to quantify the dominant systematic error sources and to find a recommended DOAS setting in the three spectral ranges. The results show that water vapour absorption, temperature and wavelength dependence of O4 absorption, temperature dependence of Ring spectrum, and polynomial and intensity offset correction all together dominate the systematic errors. We recommend a fit range of 335–373 nm for HONO retrievals. In such fit range the overall systematic uncertainty is about 0.87 × 1015 molecules cm−2, much smaller than those in the other two ranges. The typical random uncertainty is estimated to be about 0.16 × 1015 molecules cm−2, which is only 25 % of the total systematic uncertainty for most of the instruments in the MAD-CAT campaign. In summary for most of the MAX-DOAS instruments for elevation angle below 5°, half daytime measurements (usually in the morning) of HONO delta SCD can be over the detection limit of 0.2 × 1015 molecules cm−2 with an uncertainty of ∼ 0.9 × 1015 molecules cm−2.

OMI satellite observed formaldehyde column from 2006 to 2015 over Xishuangbanna, southwest China, and validation using ground based zenith-sky DOAS

Formaldehyde (HCHO) provides a proxy to reveal the isoprene and biogenic volatile organic compounds emission which plays important roles in atmospheric chemical process and climate change. The ground-based observation with zenith-sky DOAS is carried out in order to validate the HCHO columns from OMI. It has a good correlation of 0.71678 between the HCHO columns from two sources. Then we use the OMI HCHO columns from January 2006 to December 2015 to indicate the interannual variation and spatial distribution in Xishuangbanna. The HCHO concentration peaks appeared in March or April for each year significantly corresponding to the intensive fire counts at the same time, which illustrate that the high HCHO columns are strongly influenced by the biomass burning in spring. Temperature and precipitation are also the important influence factors in the seasonal variation when there is nearly no biomass burning. The spatial patterns over the past ten years strengthen the deduction from the temporal variation and show the relationship with land cover and land use, elevation and population density. It is concluded that the biogenic activity plays a role in controlling the background level of HCHO in Xishuangbanna, while biomass burning is the main driving force of high HCHO concentration. And forests are greater contributor to HCHO rather than rubber trees which cover over 20% of the land in the region. Moreover, uncertainties from HCHO slant column retrieval and AMFs calculation are discussed in detail.

The version 3 OMI NO<sub>2</sub> standard product

Abstract. We describe the new version 3.0 NASA Ozone Monitoring Instrument (OMI) standard nitrogen dioxide (NO2) products (SPv3). The products and documentation are publicly available from the NASA Goddard Earth Sciences Data and Information Services Center (https://disc.gsfc.nasa.gov/datasets/OMNO2_V003/summary/). The major improvements include (1) a new spectral fitting algorithm for NO2 slant column density (SCD) retrieval and (2) higher-resolution (1° latitude and 1.25° longitude) a priori NO2 and temperature profiles from the Global Modeling Initiative (GMI) chemistry–transport model with yearly varying emissions to calculate air mass factors (AMFs) required to convert SCDs into vertical column densities (VCDs). The new SCDs are systematically lower (by ∼ 10–40 %) than previous, version 2, estimates. Most of this reduction in SCDs is propagated into stratospheric VCDs. Tropospheric NO2 VCDs are also reduced over polluted areas, especially over western Europe, the eastern US, and eastern China. Initial evaluation over unpolluted areas shows that the new SPv3 products agree better with independent satellite- and ground-based Fourier transform infrared (FTIR) measurements. However, further evaluation of tropospheric VCDs is needed over polluted areas, where the increased spatial resolution and more refined AMF estimates may lead to better characterization of pollution hot spots.

The Effects of Aerosol on the Retrieval Accuracy of NO2 Slant Column Density

We investigate the effects of aerosol optical depth (AOD), single scattering albedo (SSA), aerosol peak height (APH), measurement geometry (solar zenith angle (SZA) and viewing zenith angle (VZA)), relative azimuth angle, and surface reflectance on the accuracy of NO2 slant column density using synthetic radiance. High AOD and APH are found to decrease NO2 SCD retrieval accuracy. In moderately polluted (5 × 1015 molecules cm−2 < NO2 vertical column density (VCD) < 2 × 1016 molecules cm−2) and clean regions (NO2 VCD < 5 × 1015 molecules cm−2), the correlation coefficient (R) between true NO2 SCDs and those retrieved is 0.88 and 0.79, respectively, and AOD and APH are about 0.1 and is 0 km, respectively. However, when AOD and APH are about 1.0 and 4 km, respectively, the R decreases to 0.84 and 0.53 in moderately polluted and clean regions, respectively. On the other hand, in heavily polluted regions (NO2 VCD > 2 × 1016 molecules cm−2), even high AOD and APH values are found to have a negligible effect on NO2 SCD precision. In high AOD and APH conditions in clean NO2 regions, the R between true NO2 SCDs and those retrieved increases from 0.53 to 0.58 via co-adding four pixels spatially, showing the improvement in accuracy of NO2 SCD retrieval. In addition, the high SZA and VZA are also found to decrease the accuracy of the NO2 SCD retrieval.

Plume Segmentation from UV Camera Images for SO2 Emission Rate Quantification on Cloud Days

We performed measurements of SO2 emissions with a high UV sensitive dual-camera optical system. Generally, in order to retrieve the two-dimensional SO2 emission rates of a source, e.g., the slant column density of a plume emitted by a stack, one needs to acquire four images with UV cameras: two images including the emitting stack at wavelengths with high and negligible absorption features (λon/off), and two additional images of the background intensity behind the plume, at the same wavelengths as before. However, the true background intensity behind a plume is impossible to obtain from a remote measurement site at rest, and thus, one needs to find a way to approximate the background intensity. Some authors have presented methods to estimate the background behind the plume from two emission images. However, those works are restricted to dealing with clear sky, or almost homogeneously illuminated days. The purpose of this work is to present a new approach using background images constructed from emission images by an automatic plume segmentation and interpolation procedure, in order to estimate the light intensity behind the plume. We compare the performance of the proposed approach with the four images method, which uses, as background, sky images acquired at a different viewing direction. The first step of the proposed approach involves the segmentation of the SO2 plume from the background. In clear sky days, we found similar results from both methods. However, when the illumination of the sky is non homogeneous, e.g., due to lateral sun illumination or clouds, there are appreciable differences between the results obtained by both methods. We present results obtained in a series of measurements of SO2 emissions performed on a cloudy day from a stack of an oil refinery in Montevideo City, Uruguay. The results obtained with the UV cameras were compared with scanning DOAS measurements, yielding a good agreement.

High-resolution airborne imaging DOAS measurements of NO<sub>2</sub> above Bucharest during AROMAT

Abstract. In this study we report on airborne imaging DOAS measurements of NO2 from two flights performed in Bucharest during the AROMAT campaign (Airborne ROmanian Measurements of Aerosols and Trace gases) in September 2014. These measurements were performed with the Airborne imaging Differential Optical Absorption Spectroscopy (DOAS) instrument for Measurements of Atmospheric Pollution (AirMAP) and provide nearly gapless maps of column densities of NO2 below the aircraft with a high spatial resolution of better than 100 m. The air mass factors, which are needed to convert the measured differential slant column densities (dSCDs) to vertical column densities (VCDs), have a strong dependence on the surface reflectance, which has to be accounted for in the retrieval. This is especially important for measurements above urban areas, where the surface properties vary strongly. As the instrument is not radiometrically calibrated, we have developed a method to derive the surface reflectance from intensities measured by AirMAP. This method is based on radiative transfer calculation with SCIATRAN and a reference area for which the surface reflectance is known. While surface properties are clearly apparent in the NO2 dSCD results, this effect is successfully corrected for in the VCD results. Furthermore, we investigate the influence of aerosols on the retrieval for a variety of aerosol profiles that were measured in the context of the AROMAT campaigns. The results of two research flights are presented, which reveal distinct horizontal distribution patterns and strong spatial gradients of NO2 across the city. Pollution levels range from background values in the outskirts located upwind of the city to about 4 × 1016 molec cm−2 in the polluted city center. Validation against two co-located mobile car-DOAS measurements yields good agreement between the datasets, with correlation coefficients of R = 0.94 and R = 0.85, respectively. Estimations on the NOx emission rate of Bucharest for the two flights yield emission rates of 15.1 ± 9.4 and 13.6 ± 8.4 mol s−1, respectively.

Mobile DOAS Observations of Tropospheric NO2 Using an UltraLight Trike and Flux Calculation

In this study, we report on airborne Differential Optical Absorption Spectroscopy (DOAS) observations of tropospheric NO2 using an Ultralight Trike (ULT) and associated flux calculations. The instrument onboard the ULT was developed for measuring the tropospheric NO2 Vertical Column Density (VCD) and it was operated for several days between 2011 and 2014, in the South-East of Romania. Collocated measurements were performed using a car-DOAS instrument. Most of the airborne and mobile ground-based measurements were performed close to an industrial platform located nearby Galati city (45.43° N, 28.03° E). We found a correlation of R = 0.71 between tropospheric NO2 VCDs deduced from airborne DOAS observations and mobile ground-based DOAS observations. We also present a comparison between stratospheric NO2 Slant Column Density (SCD) derived from the Dutch OMI NO2 (DOMINO) satellite data product and stratospheric SCDs obtained from ground and airborne measurements. The airborne DOAS observations performed on 13 August 2014 were used to quantify the NO2 flux originating from an industrial platform located nearby Galati city. Measurements during a flight above the industrial plume showed a maximum tropospheric NO2 VCD of (1.41 ± 0.27) × 1016 molecules/cm2 and an associated NO2 flux of (3.45 ± 0.89) × 10−3 kg/s.

Space-based observation of volcanic iodine monoxide

Abstract. Volcanic eruptions inject substantial amounts of halogens into the atmosphere. Chlorine and bromine oxides have frequently been observed in volcanic plumes from different instrumental platforms such as from ground, aircraft and satellites. The present study is the first observational evidence that iodine oxides are also emitted into the atmosphere during volcanic eruptions. Large column amounts of iodine monoxide, IO, are observed in satellite measurements following the major eruption of the Kasatochi volcano, Alaska, in 2008. The IO signal is detected in measurements made both by SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric CHartographY) on ENVISAT (Environmental Satellite) and GOME-2 (Global Ozone Monitoring Experiment-2) on MetOp-A (Meteorological Operational Satellite A). Following the eruption on 7 August 2008, strongly elevated levels of IO slant columns of more than 4 × 1013 molec cm−2 are retrieved along the volcanic plume trajectories for several days. The retrieved IO columns from the different instruments are consistent, and the spatial distribution of the IO plume is similar to that of bromine monoxide, BrO. Details in the spatial distribution, however, differ between IO, BrO and sulfur dioxide, SO2. The column amounts of IO are approximately 1 order of magnitude smaller than those of BrO. Using the GOME-2A observations, the total mass of IO in the volcanic plume injected into the atmosphere from the eruption of Kasatochi on 7 August 2008, is determined to be on the order of 10 Mg.

Improved OSIRIS NO<sub>2</sub> retrieval algorithm: description and validation

Abstract. A new retrieval algorithm for OSIRIS (Optical Spectrograph and Infrared Imager System) nitrogen dioxide (NO2) profiles is described and validated. The algorithm relies on spectral fitting to obtain slant column densities of NO2, followed by inversion using an algebraic reconstruction technique and the SaskTran spherical radiative transfer model (RTM) to obtain vertical profiles of local number density. The validation covers different latitudes (tropical to polar), years (2002–2012), all seasons (winter, spring, summer, and autumn), different concentrations of nitrogen dioxide (from denoxified polar vortex to polar summer), a range of solar zenith angles (68.6–90.5°), and altitudes between 10.5 and 39 km, thereby covering the full retrieval range of a typical OSIRIS NO2 profile. The use of a larger spectral fitting window than used in previous retrievals reduces retrieval uncertainties and the scatter in the retrieved profiles due to noisy radiances. Improvements are also demonstrated through the validation in terms of bias reduction at 15–17 km relative to the OSIRIS operational v3.0 algorithm. The diurnal variation of NO2 along the line of sight is included in a fully spherical multiple scattering RTM for the first time. Using this forward model with built-in photochemistry, the scatter of the differences relative to the correlative balloon NO2 profile data is reduced.

The MAX-DOAS network in Mexico City to measure atmospheric pollutants

An instrument based on the Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) technique was designed and constructed to measure scattered sunlight in the UV-visible region at different elevation angles. Slant column densities (SCDs) of specific gas absorbers such as nitrogen dioxide (NO2) and form-aldehyde (HCHO) are derived from the measured spectra. In this contribution, the technical characteristics and performance of the instruments, their deployment in a newly formed observational network within the metropolitan area of Mexico City, and some results of the retrieved NO2 and HCHO SCDs are presented. These measurements provide more insight on the vertical and spatial distribution of these key atmospheric pollutants and their temporal variability, which also serve as a basis for present and future satellite validation studies.

A new Differential Optical Absorption Spectroscopy instrument to study atmospheric chemistry from a high-altitude unmanned aircraft

Abstract. Observations of atmospheric trace gases in the tropical upper troposphere (UT), tropical tropopause layer (TTL), and lower stratosphere (LS) require dedicated measurement platforms and instrumentation. Here we present a new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument developed for NASA's Global Hawk (GH) unmanned aerial system and deployed during the Airborne Tropical TRopopause EXperiment (ATTREX). The mini-DOAS system is designed for automatic operation under unpressurized and unheated conditions at 14–18 km altitude, collecting scattered sunlight in three wavelength windows: UV (301–387 nm), visible (410–525 nm), and near infrared (900–1700 nm). A telescope scanning unit allows selection of a viewing angle around the limb, as well as real-time correction of the aircraft pitch. Due to the high altitude, solar reference spectra are measured using diffusors and direct sunlight. The DOAS approach allows retrieval of slant column densities (SCDs) of O3, O4, NO2, and BrO with relative errors similar to other aircraft DOAS systems. Radiative transfer considerations show that the retrieval of trace gas mixing ratios from the observed SCD based on O4 observations, the most common approach for DOAS measurements, is inadequate for high-altitude observations. This is due to the frequent presence of low-altitude clouds, which shift the sensitivity of the O4 SCD into the lower atmosphere and make it highly dependent on cloud coverage. A newly developed technique that constrains the radiative transfer by comparing in situ and DOAS O3 observations overcomes this issue. Extensive sensitivity calculations show that the novel O3-scaling technique allows the retrieval of BrO and NO2 mixing ratios at high accuracies of 0.5 and 15 ppt, respectively. The BrO and NO2 mixing ratios and vertical profiles observed during ATTREX thus provide new insights into ozone and halogen chemistry in the UT, TTL, and LS.

Investigating differences in DOAS retrieval codes using MAD-CAT campaign data

Abstract. The differential optical absorption spectroscopy (DOAS) method is a well-known remote sensing technique that is nowadays widely used for measurements of atmospheric trace gases, creating the need for harmonization and characterization efforts. In this study, an intercomparison exercise of DOAS retrieval codes from 17 international groups is presented, focusing on NO2 slant columns. The study is based on data collected by one instrument during the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, in summer 2013. As data from the same instrument are used by all groups, the results are free of biases due to instrumental differences, which is in contrast to previous intercomparison exercises.While in general an excellent correlation of NO2 slant columns between groups of > 99.98 % (noon reference fits) and > 99.2 % (sequential reference fits) for all elevation angles is found, differences between individual retrievals are as large as 8 % for NO2 slant columns and 100 % for rms residuals in small elevation angles above the horizon.Comprehensive sensitivity studies revealed that absolute slant column differences result predominantly from the choice of the reference spectrum while relative differences originate from the numerical approach for solving the DOAS equation as well as the treatment of the slit function. Furthermore, differences in the implementation of the intensity offset correction were found to produce disagreements for measurements close to sunrise (8–10 % for NO2, 80 % for rms residual). The largest effect of ≈ 8 % difference in NO2 was found to arise from the reference treatment; in particular for fits using a sequential reference. In terms of rms fit residual, the reference treatment has only a minor impact. In contrast, the wavelength calibration as well as the intensity offset correction were found to have the largest impact (up to 80 %) on rms residual while having only a minor impact on retrieved NO2 slant columns.

An exploratory study on the aerosol height retrieval from OMI measurements of the 477 nm O<sub>2</sub> − O<sub>2</sub> spectral band using a neural network approach

Abstract. This paper presents an exploratory study on the aerosol layer height (ALH) retrieval from the OMI 477 nm O2 − O2 spectral band. We have developed algorithms based on the multilayer perceptron (MLP) neural network (NN) approach and applied them to 3-year (2005–2007) OMI cloud-free scenes over north-east Asia, collocated with MODIS Aqua aerosol product. In addition to the importance of aerosol altitude for climate and air quality objectives, our long-term motivation is to evaluate the possibility of retrieving ALH for potential future improvements of trace gas retrievals (e.g. NO2, HCHO, SO2) from UV–visible air quality satellite measurements over scenes including high aerosol concentrations. This study presents a first step of this long-term objective and evaluates, from a statistic point of view, an ensemble of OMI ALH retrievals over a long time period of 3 years covering a large industrialized continental region. This ALH retrieval relies on the analysis of the O2 − O2 slant column density (SCD) and requires an accurate knowledge of the aerosol optical thickness, τ. Using MODIS Aqua τ(550 nm) as a prior information, absolute seasonal differences between the LIdar climatology of vertical Aerosol Structure for space-based lidar simulation (LIVAS) and average OMI ALH, over scenes with MODIS τ(550 nm) ≥ 1. 0, are in the range of 260–800 m (assuming single scattering albedo ω0 = 0. 95) and 180–310 m (assuming ω0 = 0. 9). OMI ALH retrievals depend on the assumed aerosol single scattering albedo (sensitivity up to 660 m) and the chosen surface albedo (variation less than 200 m between OMLER and MODIS black-sky albedo). Scenes with τ ≤ 0. 5 are expected to show too large biases due to the little impact of particles on the O2 − O2 SCD changes. In addition, NN algorithms also enable aerosol optical thickness retrieval by exploring the OMI reflectance in the continuum. Comparisons with collocated MODIS Aqua show agreements between −0. 02 ± 0. 45 and −0. 18 ± 0. 24, depending on the season. Improvements may be obtained from a better knowledge of the surface albedo and higher accuracy of the aerosol model. Following the previous work over ocean of Park et al.(2016), our study shows the first encouraging aerosol layer height retrieval results over land from satellite observations of the 477 nm O2 − O2 absorption spectral band.

Aerosol scattering effects on water vapor retrievals over the Los Angeles Basin

Abstract. In this study, we propose a novel approach to describe the scattering effects of atmospheric aerosols in a complex urban environment using water vapor (H2O) slant column measurements in the near infrared. This approach is demonstrated using measurements from the California Laboratory for Atmospheric Remote Sensing Fourier Transform Spectrometer on the top of Mt. Wilson, California, and a two-stream-exact single scattering (2S-ESS) radiative transfer (RT) model. From the spectral measurements, we retrieve H2O slant column density (SCD) using 15 different absorption bands between 4000 and 8000 cm−1. Due to the wavelength dependence of aerosol scattering, large variations in H2O SCD retrievals are observed as a function of wavelength. Moreover, the variations are found to be correlated with aerosol optical depths (AODs) measured at the AERONET-Caltech station. Simulation results from the RT model reproduce this correlation and show that the aerosol scattering effect is the primary contributor to the variations in the wavelength dependence of the H2O SCD retrievals. A significant linear correlation is also found between variations in H2O SCD retrievals from different bands and corresponding AOD data; this correlation is associated with the asymmetry parameter, which is a first-order measure of the aerosol scattering phase function. The evidence from both measurements and simulations suggests that wavelength-dependent aerosol scattering effects can be derived using H2O retrievals from multiple bands. This understanding of aerosol scattering effects on H2O retrievals suggests a promising way to quantify the effect of aerosol scattering on greenhouse gas retrievals and could potentially contribute towards reducing biases in greenhouse gas retrievals from space.

High‐resolution NO2 observations from the Airborne Compact Atmospheric Mapper: Retrieval and validation

AbstractNitrogen dioxide (NO2) is a short‐lived atmospheric pollutant that serves as an air quality indicator and is itself a health concern. The Airborne Compact Atmospheric Mapper (ACAM) was flown on board the NASA UC‐12 aircraft during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality Maryland field campaign in July 2011. The instrument collected hyperspectral remote sensing measurements in the 304–910 nm range, allowing daytime observations of several tropospheric pollutants, including nitrogen dioxide (NO2), at an unprecedented spatial resolution of 1.5 × 1.1 km2. Retrievals of slant column abundance are based on the differential optical absorption spectroscopy method. For the air mass factor computations needed to convert these retrievals to vertical column abundance, we include high‐resolution information for the surface reflectivity by using bidirectional reflectance distribution function data from the Moderate Resolution Imaging Spectroradiometer. We use high‐resolution simulated vertical distributions of NO2 from the Community Multiscale Air Quality and Global Modeling Initiative models to account for the temporal variation in atmospheric NO2 to retrieve middle and lower tropospheric NO2 columns (NO2 below the aircraft). We compare NO2 derived from ACAM measurements with in situ observations from NASA's P‐3B research aircraft, total column observations from the ground‐based Pandora spectrometers, and tropospheric column observations from the space‐based Ozone Monitoring Instrument. The high‐resolution ACAM measurements not only give new insights into our understanding of atmospheric composition and chemistry through observation of subsampling variability in typical satellite and model resolutions, but they also provide opportunities for testing algorithm improvements for forthcoming geostationary air quality missions.

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.

Improvements to the OMI O<sub>2</sub>–O<sub>2</sub> operational cloud algorithm and comparisons with ground-based radar–lidar observations

Abstract. The OMI (Ozone Monitoring Instrument on board NASA's Earth Observing System (EOS) Aura satellite) OMCLDO2 cloud product supports trace gas retrievals of for example ozone and nitrogen dioxide. The OMCLDO2 algorithm derives the effective cloud fraction and effective cloud pressure using a DOAS (differential optical absorption spectroscopy) fit of the O2–O2 absorption feature around 477 nm. A new version of the OMI OMCLDO2 cloud product is presented that contains several improvements, of which the introduction of a temperature correction on the O2–O2 slant columns and the updated look-up tables have the largest impact. Whereas the differences in the effective cloud fraction are on average limited to 0.01, the differences of the effective cloud pressure can be up to 200 hPa, especially at cloud fractions below 0.3. As expected, the temperature correction depends on latitude and season. The updated look-up tables have a systematic effect on the cloud pressure at low cloud fractions. The improvements at low cloud fractions are very important for the retrieval of trace gases in the lower troposphere, for example for nitrogen dioxide and formaldehyde. The cloud pressure retrievals of the improved algorithm are compared with ground-based radar–lidar observations for three sites at mid-latitudes. For low clouds that have a limited vertical extent the comparison yields good agreement. For higher clouds, which are vertically extensive and often contain several layers, the satellite retrievals give a lower cloud height. For high clouds, mixed results are obtained.

The AOTF-based NO<sub>2</sub> camera

Abstract. The abundance of NO2 in the boundary layer relates to air quality and pollution source monitoring. Observing the spatiotemporal distribution of NO2 above well-delimited (flue gas stacks, volcanoes, ships) or more extended sources (cities) allows for applications such as monitoring emission fluxes or studying the plume dynamic chemistry and its transport. So far, most attempts to map the NO2 field from the ground have been made with visible-light scanning grating spectrometers. Benefiting from a high retrieval accuracy, they only achieve a relatively low spatiotemporal resolution that hampers the detection of dynamic features. We present a new type of passive remote sensing instrument aiming at the measurement of the 2-D distributions of NO2 slant column densities (SCDs) with a high spatiotemporal resolution. The measurement principle has strong similarities with the popular filter-based SO2 camera as it relies on spectral images taken at wavelengths where the molecule absorption cross section is different. Contrary to the SO2 camera, the spectral selection is performed by an acousto-optical tunable filter (AOTF) capable of resolving the target molecule's spectral features. The NO2 camera capabilities are demonstrated by imaging the NO2 abundance in the plume of a coal-fired power plant. During this experiment, the 2-D distribution of the NO2 SCD was retrieved with a temporal resolution of 3 min and a spatial sampling of 50 cm (over a 250 × 250 m2 area). The detection limit was close to 5 × 1016 molecules cm−2, with a maximum detected SCD of 4 × 1017 molecules cm−2. Illustrating the added value of the NO2 camera measurements, the data reveal the dynamics of the NO to NO2 conversion in the early plume with an unprecedent resolution: from its release in the air, and for 100 m upwards, the observed NO2 plume concentration increased at a rate of 0.75–1.25 g s−1. In joint campaigns with SO2 cameras, the NO2 camera could also help in removing the bias introduced by the NO2 interference with the SO2 spectrum.

Effect of temperature-dependent cross sections on O4 slant column density estimation by a space-borne UV–visible hyperspectral sensor

The sensitivities of oxygen dimer (O4) slant column densities (SCDs) were examined by applying temperature-dependent O4 cross sections using the radiative transfer model (RTM) calculation with the linearized pseudo-spherical vector discrete ordinate radiative transfer model. For the sensitivity study, we used a newly developed cross section database in place of the database used in the operational algorithm. Newly investigated O4 cross section databases for 203 K and 293 K were used for the radiance simulation by interpolating temperature for each atmospheric layer based on the vertical profile of standard atmosphere in the RTM. The effect of the temperature-dependent cross sections was a significant O4 SCD increase of 8.3% with dependence on satellite and solar viewing geometries. Furthermore, the O4 SCD generally increased by an estimated 3.9% based on the observation geometries of the Ozone Monitoring Instrument. For the long-term comparison, the O4 SCD estimated from the temperature-dependent cross sections corrects 20% of the total underestimation of O4 SCD between the observation and simulation. Although the surface pressure variation and background aerosol effect also correct the O4 SCD discrepancy, the effect of temperature-dependent cross sections was more important than the effects of surface pressure variation and background aerosols. Therefore, temperature dependence of the cross section in the RTM calculation is essential for the accurate simulation of O4 SCD.