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The COVID-19 pandemic created an extreme natural experiment in which sudden changes in human behavior and economic activity resulted in significant declines in nitrogen oxide (NOx) emissions, immediately after strict lockdowns were imposed. Here we examined the impact of multiple waves and response phases of the pandemic on nitrogen dioxide (NO2) dynamics and the role of meteorology in shaping relative contributions from different emission sectors to NO2 pollution in post-pandemic New York City. Long term (> 3.5 years), high frequency measurements from a network of ground-based Pandora spectrometers were combined with TROPOMI satellite retrievals, meteorological data, mobility trends, and atmospheric transport model simulations to quantify changes in NO2 across the New York metropolitan area. The stringent lockdown measures after the first pandemic wave resulted in a decline in top-down NOx emissions by approx. 30 % on top of long-term trends, in agreement with sector-specific changes in NOx emissions. Ground-based measurements showed a sudden drop in total column NO2 in spring 2020, by up to 36 % in Manhattan and 19 %–29 % in Queens, New Jersey (NJ), and Connecticut (CT), and a clear weakening (by 16 %) of the typical weekly NO2 cycle. Extending our analysis to more than a year after the initial lockdown captured a gradual recovery in NO2 across the NY/NJ/CT tri-state area in summer and fall 2020, as social restrictions eased, followed by a second decline in NO2 coincident with the second wave of the pandemic and resurgence of lockdown measures in winter 2021. Meteorology was not found to have a strong NO2 biassing effect in New York City after the first pandemic wave. Winds, however, were favorable for low NO2 conditions in Manhattan during the second wave of the pandemic, resulting in larger column NO2 declines than expected based on changes in transportation emissions alone. Meteorology played a key role in shaping the relative contributions from different emission sectors to NO2 pollution in the city, with low-speed (

The COVID-19 pandemic created an extreme natural experiment in which sudden changes in human behavior and economic activity resulted in significant declines in nitrogen oxide (NO(x)) emissions, immediately after strict lockdowns were imposed. Here we examined the impact of multiple waves and response phases of the pandemic on nitrogen dioxide (NO(2)) dynamics and the role of meteorology in shaping relative contributions from different emission sectors to NO(2) pollution in post-pandemic New York City. Long term (> 3.5 years), high frequency measurements from a network of ground-based Pandora spectrometers were combined with TROPOMI satellite retrievals, meteorological data, mobility trends, and atmospheric transport model simulations to quantify changes in NO(2) across the New York metropolitan area. The stringent lockdown measures after the first pandemic wave resulted in a decline in top-down NO(x) emissions by approx. 30% on top of long-term trends, in agreement with sector-specific changes in NO(x) emissions. Ground-based measurements showed a sudden drop in total column NO(2) in spring 2020, by up to 36% in Manhattan and 19%–29% in Queens, New Jersey (NJ), and Connecticut (CT), and a clear weakening (by 16%) of the typical weekly NO(2) cycle. Extending our analysis to more than a year after the initial lockdown captured a gradual recovery in NO(2) across the NY/NJ/CT tri-state area in summer and fall 2020, as social restrictions eased, followed by a second decline in NO(2) coincident with the second wave of the pandemic and resurgence of lockdown measures in winter 2021. Meteorology was not found to have a strong NO(2) biassing effect in New York City after the first pandemic wave. Winds, however, were favorable for low NO(2) conditions in Manhattan during the second wave of the pandemic, resulting in larger column NO(2) declines than expected based on changes in transportation emissions alone. Meteorology played a key role in shaping the relative contributions from different emission sectors to NO with low-speed (< 5 ms(−1)) SW-SE winds enhancing contributions from the high-emitting power-generation sector in NJ and Queens and driving particularly high NO(2) pollution episodes in Manhattan, even during – and despite – the stringent early lockdowns. These results have important implications for air quality management in New York City, and highlight the value of high resolution NO(2) measurements in assessing the effects of rapid meteorological changes on air quality conditions and the effectiveness of sector-specific NO(x) emission control strategies.

Nitrogen oxides ( NO x ≡ NO + NO 2 ) in the NOx -limited upper troposphere (UT) are long-lived and so have a large influence on the oxidizing capacity of the troposphere and formation of the greenhouse gas ozone. Models misrepresent NOx in the UT, and observations to address deficiencies in models are sparse. Here we obtain a year of near-global seasonal mean mixing ratios of NO2 in the UT (450–180 hPa) at 1 ∘ × 1 ∘ by applying cloud-slicing to partial columns of NO2 from TROPOMI. This follows refinement of the cloud-slicing algorithm with synthetic partial columns from the GEOS-Chem chemical transport model. TROPOMI, prior to cloud-slicing, is corrected for a 13 % underestimate in stratospheric NO2 variance and a 50 % overestimate in free-tropospheric NO2 determined by comparison to Pandora total columns at high-altitude free-tropospheric sites at Mauna Loa, Izana, and Altzomoni and MAX-DOAS and Pandora tropospheric columns at Izana. Two cloud-sliced seasonal mean UT NO2 products for June 2019 to May 2020 are retrieved from corrected TROPOMI total columns using distinct TROPOMI cloud products that assume clouds are reflective boundaries (FRESCO-S) or water droplet layers (ROCINN-CAL). TROPOMI UT NO2 typically ranges from 20–30 pptv over remote oceans to >80 pptv over locations with intense seasonal lightning. Spatial coverage is mostly in the tropics and subtropics with FRESCO-S and extends to the midlatitudes and polar regions with ROCINN-CAL, due to its greater abundance of optically thick clouds and wider cloud-top altitude range. TROPOMI UT NO2 seasonal means are spatially consistent ( R=0.6 –0.8) with an existing coarser spatial resolution (5 ∘ latitude × 8 ∘ longitude) UT NO2 product from the Ozone Monitoring Instrument (OMI). UT NO2 from TROPOMI is 12–26 pptv more than that from OMI due to increase in NO2 with altitude from the OMI pressure ceiling (280 hPa) to that for TROPOMI (180 hPa), but possibly also due to altitude differences in TROPOMI and OMI cloud products and NO2 retrieval algorithms. The TROPOMI UT NO2 product offers potential to evaluate and improve representation of UT NOx in models and supplement aircraft observations that are sporadic and susceptible to large biases in the UT.

Multi-axis differential optical absorption spectroscopy (MAX-DOAS) and direct sun NO2 vertical column network data are used to investigate the accuracy of tropospheric NO2 column measurements of the GOME-2 instrument on the MetOp-A satellite platform and the OMI instrument on Aura. The study is based on 23 MAX-DOAS and 16 direct sun instruments at stations distributed worldwide. A method to quantify and correct for horizontal dilution effects in heterogeneous NO2 field conditions is proposed. After systematic application of this correction to urban sites, satellite measurements are found to present smaller biases compared to ground-based reference data in almost all cases. We investigate the seasonal dependence of the validation results as well as the impact of using different approaches to select satellite ground pixels in coincidence with ground-based data. In optimal comparison conditions (satellite pixels containing the station) the median bias between satellite tropospheric NO2 column measurements and the ensemble of MAX-DOAS and direct sun measurements is found to be significant and equal to −34 % for GOME-2A and −24 % for OMI. These biases are further reduced to −24 % and −18 % respectively, after application of the dilution correction. Comparisons with the QA4ECV satellite product for both GOME-2A and OMI are also performed, showing less scatter but also a slightly larger median tropospheric NO2 column bias with respect to the ensemble of MAX-DOAS and direct sun measurements.

While solar eclipses are known to greatly diminish the visible radiation reaching the surface of the Earth, less is known about the magnitude of the impact. We explore both the observed and modeled levels of change in surface radiation during the eclipse of 2017. We deployed a pyranometer and Pandora spectrometer instrument to Casper, Wyoming, and Columbia, Missouri, to measure surface broadband shortwave (SW) flux and atmospheric properties during the 21 August 2017 solar eclipse event. We performed detailed radiative transfer simulations to understand the role of clouds in spectral and broadband solar radiation transfer in the Earth's atmosphere for the normal (non-eclipse) spectrum and red-shift solar spectra for eclipse conditions. The theoretical calculations showed that the non-eclipse-to-eclipse surface flux ratio depends strongly on the obscuration of the solar disk and slightly on the cloud optical depth. These findings allowed us to estimate what the surface broadband SW flux would be for hypothetical non-eclipse conditions from observations during the eclipse and further to quantify the impact of the eclipse on the surface broadband SW radiation budget. We found that the eclipse caused local reductions of time-averaged surface flux of about 379 W m−2 (50 %) and 329 W m−2 (46 %) during the ∼3 h course of the eclipse at the Casper and Columbia sites, respectively. We estimated that the Moon's shadow caused a reduction of approximately 7 %–8 % in global average surface broadband SW radiation. The eclipse has a smaller impact on the absolute value of surface flux reduction for cloudy conditions than a clear atmosphere; the impact decreases with the increase in cloud optical depth. However, the relative time-averaged reduction of local surface SW flux during a solar eclipse is approximately 45 %, and it is not sensitive to cloud optical depth. The reduction of global average SW flux relative to climatology is proportional to the non-eclipse and eclipse flux difference in the penumbra area and depends on cloud optical depth in the Moon's shadow and geolocation due to the change in solar zenith angle. We also discuss the influence of cloud inhomogeneity on the observed SW flux. Our results not only quantify the reduction of the surface solar radiation budget, but also advance the understanding of broadband SW radiative transfer under solar eclipse conditions.

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97∘ N, 4.93∘ E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques.

Decades of air quality improvements have substantially reduced the motor vehicle emissions of volatile organic compounds (VOCs). Today, volatile chemical products (VCPs) are responsible for half of the petrochemical VOCs emitted in major urban areas. We show that VCP emissions are ubiquitous in US and European cities and scale with population density. We report significant VCP emissions for New York City (NYC), including a monoterpene flux of 14.7 to 24.4 kg ⋅ d(−1) ⋅ km(−2) from fragranced VCPs and other anthropogenic sources, which is comparable to that of a summertime forest. Photochemical modeling of an extreme heat event, with ozone well in excess of US standards, illustrates the significant impact of VCPs on air quality. In the most populated regions of NYC, ozone was sensitive to anthropogenic VOCs (AVOCs), even in the presence of biogenic sources. Within this VOC-sensitive regime, AVOCs contributed upwards of ∼20 ppb to maximum 8-h average ozone. VCPs accounted for more than 50% of this total AVOC contribution. Emissions from fragranced VCPs, including personal care and cleaning products, account for at least 50% of the ozone attributed to VCPs. We show that model simulations of ozone depend foremost on the magnitude of VCP emissions and that the addition of oxygenated VCP chemistry impacts simulations of key atmospheric oxidation products. NYC is a case study for developed megacities, and the impacts of VCPs on local ozone are likely similar for other major urban regions across North America or Europe.

Near-surface air quality (AQ) observations over coastal waters are scarce, a situation that limits our capacity to monitor pollution events at land-water interfaces. Satellite measurements of total column (TC) nitrogen dioxide (NO2) observations are a useful proxy for combustion sources but the once daily snapshots available from most sensors are insufficient for tracking the diurnal evolution and transport of pollution. Ground-based remote sensors like the Pandora Spectrometer Instrument (PSI) that have been developed to verify space-based total column NO2 and other trace gases are being tested for routine use as certified AQ monitors. The KORUS-OC (Korea-United States Ocean Color) cruise aboard the R/V Onnuri in May-June 2016 represented an opportunity to study AQ near the South Korean coast, a region affected by both local/regional and long-distance pollution sources. Using PSI data in direct-sun mode and in situ sensors for shipboard ozone, CO and NO2, we explore, for the first time, relationships between TC NO2 and surface AQ in this coastal region. Three case studies illustrate the value of the PSI as well as complexities in the surface-column NO2 relationship caused by varying meteorological conditions. Case Study 1 (25-26 May 2016) exhibited a high correlation of surface NO2 to TC NO2 measured by both PSI and Aura's Ozone Monitoring Instrument (OMI) but two other cases displayed poor relationships between in situ and TC NO2 due to decoupling of pollution layers from the surface. With suitable interpretation the PSI TC NO2 measurement demonstrates good potential for working with upcoming geostationary satellites to advance diurnal tracking of pollution.

NASA deployed the GeoTASO airborne UV–visible spectrometer in May–June 2017 to produce high-resolution (approximately 250 m×250 m) gapless NO2 datasets over the western shore of Lake Michigan and over the Los Angeles Basin. The results collected show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO2 observations (r2=0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and spatial heterogeneity that may be observed differently by the sunward-viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO (Tropospheric Emissions: Monitoring Pollution), TROPOMI (TROPOspheric Monitoring Instrument), and OMI (Ozone Monitoring Instrument), the agreement with Pandora measurements degraded, particularly for the most polluted columns as localized large pollution enhancements observed by Pandora and GeoTASO are spatially averaged with nearby less-polluted locations within the larger area representative of the satellite spatial resolutions (aircraft-to-Pandora slope: TEMPO scale =0.88; TROPOMI scale =0.77; OMI scale =0.57). In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well at least up to pollution scales of 30×1015 molecules cm−2. Two publicly available OMI tropospheric NO2 retrievals are found to be biased low with respect to these Pandora observations. However, the agreement improves when higher-resolution a priori inputs are used for the tropospheric air mass factor calculation (NASA V3 standard product slope =0.18 and Berkeley High Resolution product slope =0.30). Overall, this work explores best practices for satellite validation strategies with Pandora direct-sun observations by showing the sensitivity to product spatial resolution and demonstrating how the high-spatial-resolution NO2 data retrieved from airborne spectrometers, such as GeoTASO, can be used with high-temporal-resolution ground-based column observations to evaluate the influence of spatial heterogeneity on validation results.

Retrievals of total column NO2 (TCNO2) are compared for 14 sites from the Ozone Measuring Instrument (OMI using OMNO2-NASA v3.1) on the AURA satellite and from multiple ground-based PANDORA spectrometer instruments making direct-sun measurements. While OMI accurately provides the daily global distribution of retrieved TCNO2, OMI almost always underestimates the local amount of TCNO2 by 50 % to 100 % in polluted areas, while occasionally the daily OMI value exceeds that measured by PANDORA at very clean sites. Compared to local ground-based or aircraft measurements, OMI cannot resolve spatially variable TCNO2 pollution within a city or urban areas, which makes it less suitable for air quality assessments related to human health. In addition to systematic underestimates in polluted areas, OMI's selected 13:30 Equator crossing time polar orbit causes it to miss the frequently much higher values of TCNO2 that occur before or after the OMI overpass time. Six discussed Northern Hemisphere PANDORA sites have multi-year data records (Busan, Seoul, Washington DC, Waterflow, New Mexico, Boulder, Colorado, and Mauna Loa), and one site in the Southern Hemisphere (Buenos Aires, Argentina). The first four of these sites and Buenos Aires frequently have high TCNO2 (TCNO2 > 0.5 DU). Eight additional sites have shorter-term data records in the US and South Korea. One of these is a 1-year data record from a highly polluted site at City College in New York City with pollution levels comparable to Seoul, South Korea. OMI-estimated air mass factor, surface reflectivity, and the OMI 24 km × 13 km FOV (field of view) are three factors that can cause OMI to underestimate TCNO2. Because of the local inhomogeneity of NOx emissions, the large OMI FOV is the most likely factor for consistent underestimates when comparing OMI TCNO2 to retrievals from the small PANDORA effective FOV (measured in m2) calculated from the solar diameter of 0.5∘.

The worldwide operating Pandonia Global Network (PGN) is measuring atmospheric trace gases at high temporal resolution with the purpose of air quality monitoring and satellite validation. It is an activity carried out jointly by NASA and ESA as part of their “Joint Program Planning Group Subgroup” on calibration and validation and field activities, with additional collaboration from other institutions, most notably a strongly growing participation of the US Environmental Protection Agency (EPA). The more than 50 official PGN instruments are homogeneously calibrated and their data are centrally processed in real-time. Since 2019, total NO2 column amounts from the PGN are uploaded daily to the ESA Atmospheric Validation Data Centre (EVDC), where they are used for operational validation of Sentinel 5P (S5P) retrievals. During 2020, a new processor version 1.8 has been developed, which produces improved total NO2 column amounts and also the following new PGN products: total columns of O3, SO2 and HCHO based on direct sun observations and tropospheric columns, surface concentrations and tropospheric profiles of NO2 and HCHO based on sky observations. In this presentation we show some first examples of comparisons of the new PGN products with S5P data. Compared to the total NO2 columns from the previous processor version 1.7, the 1.8 data use better estimations for the effective NO2 temperature and the air mass factor. The effect of this improvement on the comparison with S5P retrievals is shown for some remote and high-altitude PGN sites. The new PGN total O3 column algorithm also retrieves the effective O3 temperature, which is a rather unique feature for ground-based direct sun retrievals. This allows us to analyze whether potential differences to satellite O3 columns might be influenced by the O3 temperature. Including the O3 temperature in the spectral fitting has also allowed the retrieval of accurate total SO2 columns. This PGN data product is of particular interest for satellite validation, as ground-based total SO2 column amounts are hardly measured by other instrumentation. An initial comparison of the PGN SO2 columns with S5P retrievals at selected PGN sites around the world is shown. PGN total HCHO columns from direct sun measurements are now possible for those PGN instruments, where the hardware parts made of Delrin, which outgasses HCHO, have been replaced by Nylon pieces. An initial comparison to HCHO retrievals from S5P is shown for locations with these upgraded instruments. Another new feature in the 1.8 PGN data is that they come with comprehensive uncertainty estimations, separated in the output files as independent, structured, common and total uncertainty.

Nitrogen oxides (NOx ≡ NO + NO2) in the NOx-limited upper troposphere (UT) are long-lived and so have a large influence on the oxidizing capacity of the troposphere and formation of the greenhouse gas ozone. Models misrepresent NOx in the UT and observations to address deficiencies in models are sparse. Here we obtain a year of near-global seasonal mean mixing ratios of NO2 in the UT (450–180 hPa) at 1 ° x 1° by applying cloud-slicing to partial columns of NO2 from TROPOMI. This follows refinement of the cloud-slicing algorithm with synthetic partial columns from the GEOS-Chem chemical transport model. We find that synthetic cloud-sliced UT NO2 are spatially consistent (R = 0.64) with UT NO2 calculated across the same cloud pressure range and scenes as are cloud-sliced (“true” UT NO2), but the cloud-sliced UT NO2 is 11–22 % more than the "true" all-sky seasonal mean. The largest contributors to differences between synthetic cloud-sliced and “true” UT NO2 are target resolution of the cloud-sliced product and uniformity of overlying stratospheric NO2. TROPOMI, prior to cloud-slicing, is corrected for a 13 % underestimate in stratospheric NO2 variance and a 50 % overestimate in free tropospheric NO2 determined by comparison to Pandora total columns at high-altitude sites in Mauna Loa, Izaña and Altzomoni, and MAX-DOAS and Pandora tropospheric columns at Izaña. Two cloud-sliced seasonal mean UT NO2 products for June 2019 to May 2020 are retrieved from corrected TROPOMI total columns using distinct TROPOMI cloud products that assume clouds are reflective boundaries (FRESCO-S) or water droplet layers (ROCINN-CAL). TROPOMI UT NO2 typically ranges from 20-30 pptv over remote oceans to > 80 pptv over locations with intense seasonal lightning. Spatial coverage is mostly in the tropics and subtropics with FRESCO-S and extends to the midlatitudes and polar regions with ROCINN-CAL, due to its greater abundance of optically thick clouds and wider cloud top altitude range. TROPOMI UT NO2 seasonal means are spatially consistent (R = 0.6–0.8) with an existing coarser spatial resolution (5° latitude x 8° longitude) UT NO2 product from the Ozone Monitoring Instrument (OMI). UT NO2 from TROPOMI is 12–26 pptv more than that from OMI due to increase in NO2 with altitude from the OMI pressure ceiling (280 hPa) to that for TROPOMI (180 hPa), but possibly also systematic altitude differences between the TROPOMI and OMI cloud products. The TROPOMI UT NO2 product offers potential to evaluate and improve representation of UT NOx in models and supplement aircraft observations that are sporadic and susceptible to large biases in the UT.

Near-surface air quality (AQ) observations over coastal waters are scarce, a situation that limits our capacity to monitor pollution events at land-water interfaces. Satellite measurements of total column (TC) nitrogen dioxide (NO(2)) observations are a useful proxy for combustion sources but the once daily snapshots available from most sensors are insufficient for tracking the diurnal evolution and transport of pollution. Ground-based remote sensors like the Pandora Spectrometer Instrument (PSI) that have been developed to verify space-based total column NO(2) and other trace gases are being tested for routine use as certified AQ monitors. The KORUS-OC (Korea-United States Ocean Color) cruise aboard the R/V Onnuri in May-June 2016 represented an opportunity to study AQ near the South Korean coast, a region affected by both local/regional and long-distance pollution sources. Using PSI data in direct-sun mode and in situ sensors for shipboard ozone, CO and NO(2), we explore, for the first time, relationships between TC NO(2) and surface AQ in this coastal region. Three case studies illustrate the value of the PSI as well as complexities in the surface-column NO(2) relationship caused by varying meteorological conditions. Case Study 1 (25-26 May 2016) exhibited a high correlation of surface NO(2) to TC NO(2) measured by both PSI and Aura’s Ozone Monitoring Instrument (OMI) but two other cases displayed poor relationships between in situ and TC NO(2) due to decoupling of pollution layers from the surface. With suitable interpretation the PSI TC NO(2) measurement demonstrates good potential for working with upcoming geostationary satellites to advance diurnal tracking of pollution.

MAX-DOAS and direct sun NO2 vertical column network data are used to investigate the accuracy of tropospheric NO2 column measurements of the GOME-2 instrument on the MetOP-A satellite platform and the OMI instrument on Aura. The study is based on 23 MAX-DOAS and 16 direct sun instruments at stations distributed worldwide. A method to quantify and correct for horizontal dilution effects in heterogeneous NO2 field conditions is proposed. After systematic application of this correction to urban sites, satellite measurements are found to present smaller biases compared to ground-based reference data in almost all cases. We investigate the seasonal dependence of the validation results, as well as the impact of using different approaches to select satellite ground pixels in coincidence with ground-based data. In optimal comparison conditions (satellite pixels containing the station) the median bias between satellite tropospheric NO2 column measurements and the ensemble of MAX-DOAS and direct sun measurements is found to be significant and equal to −36 % for GOME-2A and −20 % for OMI. These biases are further reduced to −24 % and −8 % respectively, after application of the dilution correction. Comparisons with the QA4ECV satellite product for both GOME-2A and OMI is also performed, showing less scatter but also a slightly larger median tropospheric NO2 column bias with respect to the ensemble of MAX-DOAS and direct sun measurements.

The Pandonia Global Network (PGN) is a worldwide operating network of passive remote sensing spectrometer systems named “Pandora”. PGN is measuring atmospheric trace gases at high temporal resolution with the purpose of air quality monitoring and satellite validation. PGN is an activity carried out jointly by NASA, through the Pandora project at Goddard Space Flight Center, and ESA, through the Austrian contractor LuftBlick, as part of their Joint Program Planning Group Subgroup on calibration and validation and field activities. Many of the more than 50 actual PGN instruments are directly owned by NASA or ESA, another part belongs to other collaborating governmental and academic institutions. A major objective of the PGN is to support the validation and verification of more than a dozen low-earth orbit and geostationary orbit based UV-visible sensors, most notably Sentinel 5P, TEMPO, GEMS and Sentinel 4. PGN instruments are homogeneously calibrated and their data are centrally processed in real-time. Starting in June 2019, the PGN team has made more and more network locations “official PGN sites”, which means all required technical and logistical steps for this purpose have been performed. At the end of 2019 there are 18 such official network sites, where quality assured data are uploaded daily to EVDC (ESA Atmospheric Validation Data Centre), where they are used for operational validation of Sentinel 5P retrievals (see e.g. http://mpc-vdaf-server.tropomi.eu/no2/no2-offl-pandora). The current official PGN data products are total vertical column amounts of NO2 and O3 from direct sun observations. Research data products include total vertical columns amounts of SO2 and HCHO from direct sun observations as well as surface concentrations, tropospheric columns amounts, and vertical profiles for NO2 and HCHO from sky observations. These named research products are planned to become official over the course of the year 2020.

Ten wavelength channels of calibrated radiance image data from the sunlit Earth are obtained every 65 min during Northern Hemisphere summer from the EPIC (Earth Polychromatic Imaging Camera) instrument on the DSCOVR (Deep Space Climate Observatory) satellite located near the Earth–Sun Lagrange 1 point (L1), about 1.5 million km from the Earth. The L1 location permitted seven observations of the Moon's shadow on the Earth for about 3 h during the 21 August 2017 eclipse. Two of the observations were timed to coincide with totality over Casper, Wyoming, and Columbia, Missouri. Since the solar irradiances within five channels (λi = 388, 443, 551, 680, and 780 nm) are not strongly absorbed in the atmosphere, they can be used for characterizing the eclipse reduction in reflected radiances for the Earth's sunlit face containing the eclipse shadow. Five channels (λi = 317.5, 325, 340, 688, and 764 nm) that are partially absorbed in the atmosphere give consistent reductions compared to the non-absorbed channels. This indicates that cloud reflectivities dominate the 317.5–780 nm radiances reflected back to space from the sunlit Earth's disk with a significant contribution from Rayleigh scattering for the shorter wavelengths. An estimated reduction of 10 % was obtained for spectrally integrated radiance (387 to 781 nm) reflected from the sunlit Earth towards L1 for two sets of observations on 21 August 2017, while the shadow was in the vicinity of Casper, Wyoming (42.8666° N, 106.3131° W; centered on 17:44:50 UTC), and Columbia, Missouri (38.9517° N, 92.3341° W; centered on 18:14:50 UTC). In contrast, when non-eclipse days (20 and 23 August) are compared for each wavelength channel, the change in reflected light is much smaller (less than 1 % for 443 nm compared to 9 % (Casper) and 8 % (Columbia) during the eclipse). Also measured was the ratio REN(λi) of reflected radiance on adjacent non-eclipse days divided by radiances centered in the eclipse totality region with the same geometry for all 10 wavelength channels. The measured REN(443 nm) was smaller for Columbia (169) than for Casper (935), because Columbia had more cloud cover than Casper. REN(λi) forms a useful test of a 3-D radiative transfer models for an eclipse in the presence of optically thin clouds. Specific values measured at Casper with thin clouds are REN(340 nm) = 475, REN(388 nm) = 3500, REN(443 nm) = 935, REN(551 nm) = 5455, REN(680 nm) = 220, and REN(780 nm) = 395. Some of the variability is caused by changing cloud amounts within the moving region of totality during the 2.7 min needed to measure all 10 wavelength channels.

Aerosol optical thickness (tau(aer))) is a fundamental parameter for analyzing aerosol loading and associated radiative effects. Tau(aer) can constrain many inversion algorithms using passive/active sensor measurements to retrieve other aerosol properties and/or the abundance of trace gases. In the next wave of spectroradiometric observations from geostationary platforms, we envision that a strategically distributed network of robust, well-calibrated ground-based spectroradiometers will comprehensively complement spaceborne measurements in spectral and temporal domains. Spectral tau(aer) can be accurately obtained from direct-Sun measurements based on the Langley calibration method, which allows for the analysis of distinct spectral features of the calibration results. In this study, we present a spectral tau(aer) retrieval algorithm for an in-house developed, field deployable spectroradiometer instrument covering wavelengths from ultraviolet to near infrared (UV-Vis-NIR). The spectral total optical thickness obtained from the Langley calibration method is partitioned into molecular and particulate components by utilizing a least-squares method. The resulting high temporal-resolution tau(aer) and Angstrom Exponent can be used effectively for cloud screening. The new algorithm was applied to months-long measurements acquired from the rooftop at NASA Goddard Space Flight Center's Building 33. The retrieved tau(aer) demonstrated excellent agreement with those from well-calibrated Aerosol Robotic Network (AERONET) sunphotometers at all overlapping wavelengths (correlation coefficients higher than 0.98). In addition, empirical stray light corrections considerably improved tau(aer) retrievals at short wavelengths in the UV. The continuous spectrum of tau(aer) from UV-Vis-NIR spectroradiometers is expected to provide more informative constraints for retrieval of additional aerosol properties such as refractive indices, size, and bulk vertical distribution.

Vertical column density (VCD) of nitrogen dioxide was measured using Pandora spectrometers at six sites on the Korean Peninsula during the Megacity Air Pollution Studies-Seoul (MAPS-Seoul) campaign from May to June 2015. To estimate the tropospheric nitrogen dioxide VCD, the stratospheric nitrogen dioxide VCD from the Ozone Monitoring Instrument (OMI) was subtracted from the total nitrogen dioxide VCD from Pandora. European Centre for Medium-Range Weather Forecasts (ECMWF) reanalysis wind data was used to analyze variations in tropospheric nitrogen dioxide VCD caused by wind patterns at each site. The Yonsei/SEO site was found to have the largest tropospheric nitrogen dioxide VCD (1.49 DU on average) from a statistical analysis of hourly tropospheric nitrogen dioxide VCD measurements. At rural sites, remarkably low nitrogen dioxide VCDs were observed. However, a wind field analysis showed that trans-boundary transport and emissions from domestic sources lead to an increase in tropospheric nitrogen dioxide VCD at NIER/BYI and KMA/AMY, respectively. At urban sites, high nitrogen dioxide VCD values were observed under conditions of low wind speed, which were influenced by local urban emissions. Tropospheric nitrogen dioxide VCD at HUFS/Yongin increases under conditions of significant transport from urban area of Seoul according to a correlation analysis that considers the transport time lag. Significant diurnal variations were found at urban sites during the MAPS Seoul campaign, but not at rural sites, indicating that it is associated with diurnal patterns of nitrogen dioxide emissions from dense traffic.

While solar eclipses are known to greatly diminish the visible radiation reaching the surface of the Earth, less is known about the magnitude of the impact. We explore both the observed and modelled level of change in surface radiation during the eclipse of 2017. We deployed a pyranometer and Pandora spectrometer instrument to Casper, Wyoming and Columbia, Missouri to measure surface broadband shortwave (SW) flux and atmospheric properties during the 21 August 2017 solar eclipse event. We performed detailed radiative transfer simulations to understand the role of clouds in spectral and broadband solar radiation transfer in the Earth’s atmosphere for the normal (non-eclipse) spectrum and red-shift solar spectra for eclipse conditions. The theoretical calculations showed that the non-eclipse-to-eclipse surface flux ratio depends strongly on the obscuration of solar disk and slightly on cloud optical depth. These findings allowed us to estimate what the surface broadband SW flux would be for non-eclipse conditions from observations during the eclipse and further to quantify the impact of the eclipse on the surface broadband SW radiation budget. We found that the eclipse caused local reductions of time-averaged surface flux of about 379 W m−2 (50 %) and 329 W m−2 (46 %) during the ∼3 hours course of the eclipse at the Casper and Columbia sites, respectively. We estimated that the Moon’s shadow caused a reduction of approximately 7–8 % in global average surface broadband SW radiation. The eclipse has a smaller impact on surface flux reduction for cloudy conditions than a clear atmosphere; the impact decreases with the increase of cloud optical depth. However, the relative time-averaged reduction of local surface SW flux during a solar eclipse is approximately 45 % and it is not sensitive to cloud optical depth. The reduction of global average SW flux relative to climatology is proportional to the non-eclipse and eclipse flux difference in the penumbra area and depends on cloud optical depth in the Moon’s shadow and geolocation due to the change of solar zenith angle. We also discuss the influence of cloud inhomogeneity on the observed SW flux. Our results not only quantify the reduction of the surface solar radiation budget but also advance the understanding of broadband SW radiative transfer under solar eclipse conditions.

NASA deployed an airborne UV/Visible spectrometer, GeoTASO, in May–June 2017 to produce high resolution (approximately 250 × 250 m), gapless NO2 datasets over the western shore of Lake Michigan and over the Los Angeles Basin. Results show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO2 observations (r2 = 0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and also spatial heterogeneity that may be observed differently by the sunward viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO, TROPOMI, and OMI, the agreement with Pandora measurements is degraded as localized polluted plumes observed by Pandora are spatially averaged over larger areas (aircraft-to-Pandora slope: TEMPO scale = 0.88; TROPOMI scale = 0.77; OMI scale = 0.57). This behavior suggests that satellite products are representative of individual Pandora observations up to a certain pollution scale that depends on satellite spatial resolution. In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well up to pollution scales of 30 x 1015 molecules cm−2. Two publicly available OMI tropospheric NO2 retrievals are both found to be biased low with respect to Pandora observations (NASA V3 Standard Product slope = 0.18 and Berkeley High Resolution Product slope = 0.30). However, the agreement improves when higher resolution a priori inputs are used for the tropospheric air mass factor calculation. Overall, this work explores best practices for satellite validation strategies by showing the sensitivity to product spatial resolution and demonstrates how the high spatial resolution NO2 data retrieved from airborne spectrometers, such as GeoTASO, can be used with high temporal resolution surface observations to evaluate the influence of spatial heterogeneity on validation results.

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 days during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, The Netherlands (51.97° N, 4.93° E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were to characterise and better understand the differences between a large number of Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, to discuss the performance of the various types of instruments and to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen dimer (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region and NO2 in an additional (smaller) wavelength range in the visible. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in an unprecedented set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the reference, and the RMS error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the measurement performance of all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques.

Accurately capturing the evolution of episodic stratosphere-to-troposphere transport is critical due to the potential impacts on both climate and air quality. Until now, investigating associated spatiotemporal gradients in total column ozone (TCO) has primarily been the task of observations from polar-orbiting satellites as well as high-resolution models. We explore how a network of five ground-based Pandora spectrometer systems can be utilized in a similar fashion. The passage of a strong mid-latitude cyclone in March 2018 and its associated stratospheric intrusion is used as a case demonstrating the ability of networked Pandora observations to contextualize these regions of transport across space and time. Results show that the high temporal resolution of Pandora observations and the networked approach were able to resolve increases in TCO associated with stratosphere-to-troposphere transport and to capture the spatial context of the chosen episode. The use of networked Pandora observations shows promise for additional transport studies and for supporting future geostationary atmospheric composition satellite missions and modeling efforts.

Coastal environments are highly dynamic, and are characterized by short-term, local-scale variability in atmospheric and oceanic processes. Yet, high-frequency measurements of atmospheric composition, and particularly nitrogen dioxide (NO2) and ozone (O3) dynamics, are scarce over the ocean, introducing uncertainties in satellite retrievals of coastal ocean biogeochemistry and ecology. Combining measurements from different platforms, the Korea-US Ocean Color and Air Quality field campaign provided a unique opportunity to capture, for the first time, the strong spatial dynamics and diurnal variability in total column (TC) NO2 and O3 over the coastal waters of South Korea. Measurements were conducted using a shipboard Pandora Spectrometer Instrument specifically designed to collect accurate, high-frequency observations from a research vessel, and were combined with ground-based observations at coastal land sites, synoptic satellite imagery, and air-mass trajectory simulations to assess source contributions to atmospheric pollution over the coastal ocean. TCO3 showed only small (

The KORUS-AQ field study conducted during May–June 2016 offered the first opportunity to evaluate direct-sun observations of formaldehyde (HCHO) total column densities with improved Pandora spectrometer instruments. The measurements highlighted in this work were conducted both in the Seoul megacity area at the Olympic Park site (latitude: 37.5232° N, longitude: 127.1260° E, 26 m a.s.l.) and at a nearby rural site downwind of the city at the Mount Taehwa Research Forest site (latitude: 37.3123° N, longitude: 127.3106° E, 160 m a.s.l.). Evaluation of these measurements was made possible by concurrent ground-based in situ observations of HCHO at both sites as well as overflight by the NASA DC-8 research aircraft. The flights provided in situ measurements of HCHO to characterize its vertical distribution in the lower troposphere (0–5 km). Diurnal variation in HCHO total column densities followed the same pattern at both sites, with the minimum daily values typically observed between 6:00–7:00 local time, gradually increasing to a maximum between 13:00 and 17:00 before decreasing into the evening. Pandora vertical column densities were compared with those derived from the DC-8 HCHO in-situ measured profiles augmented with in-situ surface concentrations below the lowest altitude of the DC-8 in proximity to the ground sites. A comparison between 49 column densities measured by Pandora versus aircraft integrated in-situ data showed that Pandora values were larger by 16 % (intercept = 0.22 DU, R2 = 0.68). Pandora HCHO columns were also compared with columns calculated from the surface in-situ measurements over Olympic Park by assuming a well-mixed lower atmosphere up to a ceilometer measured mixed-layer height (MLH) and various assumptions about the small residual HCHO amounts in the free troposphere up to the tropopause. The best comparison (slope = 1.03 ± 0.03, intercept = 0.29 ± 0.02 DU and R2 of 0.78 ± 0.02) was achieved assuming equal mixing within ceilometer measured MLH combined with an exponential profile shape. These results suggest that diurnal changes in HCHO surface concentrations can be reasonably estimated from the Pandora total column and information on the mixed-layer height. More work is needed to understand the bias in the intercept and the slope relative to columns derived from the in-situ aircraft and surface measurements.

Ten wavelength channels of calibrated radiance image data from the Sunlit Earth are obtained every 65 minutes during Northern Hemisphere summer from the DSCOVR/EPIC instrument located near the Earth-Sun Lagrange-1 point (L 1 ), 1.5 million km from the Earth. The L 1 location permitted seven observations of the Moon’s shadow on the Earth for about 3 hours during the 21 August 2017 eclipse. Two of the observations were timed to be over Casper, Wyoming and Columbia, Missouri. Since, the solar irradiances within 5 channels (λ i = 388, 443, 551, 680, and 780 nm) are not strongly absorbed in the atmosphere, they can be used for characterizing eclipse reduction in reflected radiances for the sunlit face of the Earth containing the eclipse shadow. Five channels (λ i = 317.5, 325, 340, 688, and 764 nm) that are partially absorbed in the atmosphere give consistent reductions compared to the non-absorbed channels. This indicates that cloud reflectivities dominate the 317.5 to 780 nm radiances reflected back to space from the sunlit Earth’s disk with a strong contribution from Rayleigh scattering for the shorter wavelengths. A reduction of 9.7 ± 1.7 % in the radiance (387 to 781 nm) reflected from the Earth towards L 1 was obtained for the set of observations on 21 August 2017, while the shadow was in the vicinity of Casper, Wyoming (42.8666° N, 106.3131° W, centered on 17:44:50 UTC). In contrast, when successive non-eclipse days are compared for each wavelength channel, the change in reflected light is much smaller (less than 1 % for 443 nm compared to 9 % during the eclipse). Also measured was the spatially averaged ratio R EN (λ i ) > of reflected radiance within the eclipse totality region to radiances for the same geometry on adjacent non-eclipse days for all 10 wavelength channels. The measured R EN (443 nm) > was smaller for Columbia (35) than for Casper (122), because Columbia had more cloud cover than Casper. R EN (λ i ) forms a useful test of 3-D radiative transfer models for an eclipse in the presence of optically thin clouds. A previously published clear-sky model (Emde and Mayer, 2007) shows results for a nearly overhead eclipse had R EN (340 nm)=1.7 x 10 4 compared to the maximum measured non-averaged R EN (340) at Casper of 515 ± 27 with optically thin clouds under similar geometrical conditions.

Urban nearshore regions are characterized by strong variability in atmospheric composition, associated with anthropogenic emissions and meteorological processes that influence the circulation and accumulation of atmospheric pollutants at the land-water interface. If not adequately corrected in satellite retrievals of ocean color, this atmospheric variability can impose a false impression of diurnal and seasonal changes in nearshore water quality and biogeochemical processes. Consideration of these errors is important for measurements from polar orbiting ocean color sensors but becomes critical for geostationary satellite missions having the capability for higher frequency and higher spatial resolution observations of coastal ocean dynamics. We examined variability in atmospheric NO2 over urban nearshore environments in the Eastern US, Europe, and Korea, using a new network of ground-based Pandora spectrometers and Aura-OMI satellite observations. Our measurements in the US and in Europe revealed clear diurnal and day-of-the-week patterns in total column NO2 (TCNO2), temporal changes as large as 0.8 DU within 4 h, and spatial variability as large as 0.7 DU within an area often covered by just a single OMI pixel. TCNO2 gradients were considerably stronger over the coastal cities of Korea. With a coarse resolution and an overpass at around 13:30 local time, OMI cannot detect this strong variability in NO2, missing pollution peaks from industrial and rush hour activities. Observations were combined with air quality model simulations and radiative transfer calculations to estimate the impact of atmospheric NO2 variability on satellite retrievals of coastal ocean remote sensing reflectance and biogeochemical variables (i.e., chlorophyll and CDOM).

Total columnar water vapor (CWV), nitrogen dioxide (NO2), and ozone (O3) are derived from a newly developed, hyperspectral airborne Sun-sky spectrometer (4STAR) for the first time during the two intensive phases of the Two-Column Aerosol Project (TCAP) in summer 2012 and winter 2013 aboard the DOE G-1 aircraft. We compare results with coincident measurements. We find 0.045 g/cm2 (4.2%) negative bias and 0.28 g/cm2 (26.3%) root-mean-square difference (RMSD) in water vapor layer comparison with an in situ hygrometer and an overall RMSD of 1.28 g/m3 (38%) water vapor amount in profile by profile comparisons, with differences distributed evenly around zero. RMSD for O3 columns average to 3%, with a 1% negative bias for 4STAR compared with the Ozone Measuring Instrument along aircraft flight tracks for 14 flights during both TCAP phases. Ground-based comparisons with Pandora spectrometers at the Goddard Space Flight Center, Greenbelt, Maryland, showed excellent agreement between the instruments for both O3 (1% RMSD and 0.1% bias) and NO2 (17.5% RMSD and −8% bias). We apply clustering analysis of the retrieved products as a case study during the TCAP summer campaign to identify variations in atmospheric composition of elevated pollution layers and demonstrate that combined total column measurements of trace gas and aerosols can be used to define different pollution layer sources, by comparing our results with trajectory analysis and in situ airborne miniSPLAT (single-particle mass spectrometer) measurements. Our analysis represents a first step in linking sparse but intense in situ measurements from suborbital campaigns with total column observations from space.

Total-column nitrogen dioxide (NO2) data collected by a ground-based sun-tracking spectrometer system (Pandora) and an photolytic-converter-based in-situ instrument collocated at NASA’s Langley Research Center in Hampton, Virginia were analyzed to study the relationship between total-column and surface NO2 measurements. The measurements span more than a year and cover all seasons. Surface mixing ratios are estimated via application of a planetary boundary-layer (PBL) height correction factor. This PBL correction factor effectively corrects for boundary-layer variability throughout the day, and accounts for up to ≈75 % of the variability between the NO2 data sets. Previous studies have made monthly and seasonal comparisons of column/surface data, which has shown generally good agreement over these long average times. In the current analysis comparisons of column densities averaged over 90 s and 1 h are made. Applicability of this technique to sulfur dioxide (SO2) is briefly explored. The SO2 correlation is improved by excluding conditions where surface levels are considered background. The analysis is extended to data from the July 2011 DISCOVER-AQ mission over the greater Baltimore, MD area to examine the method’s performance in more-polluted urban conditions where NO2 concentrations are typically much higher.

Spatial and temporal dynamics in trace gas pollutants were examined over a major urban estuarine ecosystem, using a new network of ground-based Pandora spectrometers deployed at strategic locations along the Washington-Baltimore corridor and the Chesapeake Bay. Total column ozone (TCO3) and nitrogen dioxide (TCNO2) were measured during NASA’s DISCOVER-AQ and GeoCAPE-CBODAQ campaigns in July 2011. The Pandora network provided high-resolution information on air-quality variability, local pollution conditions, large-scale meteorological influences, and interdependencies of ozone and its major precursor, NO2. Measurements were used to compare with air-quality model simulations (CMAQ), evaluate Aura-OMI satellite retrievals, and assess advantages and limitations of space-based observations under a range of conditions. During the campaign, TCNO2 varied by an order of magnitude, both spatially and temporally. Although fairly constant in rural regions, TCNO2 showed clear diurnal and weekly patterns in polluted urban areas caused by changes in near-surface emissions. With a coarse resolution and an overpass at around 13:30 local time, OMI cannot detect this strong variability in NO2, missing pollution peaks from industrial and rush hour activities. Not as highly variable as NO2, TCO3 was mostly affected by large-scale meteorological patterns as observed by OMI. A clear weekly cycle in TCO3, with minima over the weekend, was due to a combination of weekly weather patterns and changes in near-surface NOx emissions. A Pandora instrument intercomparison under the same conditions at GSFC showed excellent agreement, within ±4.8DU for TCO3 and ±0.07DU for TCNO2 with no air-mass-factor dependence, suggesting that observed variability during the campaign was real.

We present intercomparison results for formaldehyde (HCHO) slant column measurements performed during the Cabauw Intercomparison campaign of Nitrogen Dioxide measuring Instruments (CINDI) that took place in Cabauw, the Netherlands, in summer 2009. During two months, nine atmospheric research groups simultaneously operated MAX-DOAS (MultiAXis Differential Optical Absorption Spectroscopy) instruments of various designs to record UV-visible spectra of scattered sunlight at different elevation angles that were analysed using common retrieval settings. The resulting HCHO data set was found to be highly consistent, the mean difference between instruments generally not exceeding 15% or 7.5 × 1015 molec cm−2, for all viewing elevation angles. Furthermore, a sensitivity analysis was performed to investigate the uncertainties in the HCHO slant column retrieval when varying key input parameters such as the molecular absorption cross sections, correction terms for the Ring effect or the width and position of the fitting interval. This study led to the identification of potentially important sources of errors associated with cross-correlation effects involving the Ring effect, O4, HCHO and BrO cross sections and the DOAS closure polynomial. As a result, a set of updated recommendations was formulated for HCHO slant column retrieval in the 336.5–359 nm wavelength range. To conclude, an error budget is proposed which distinguishes between systematic and random uncertainties. The total systematic error is estimated to be of the order of 20% and is dominated by uncertainties in absorption cross sections and related spectral cross-correlation effects. For a typical integration time of one minute, random uncertainties range between 5 and 30%, depending on the noise level of individual instruments.

In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO2 from the ground for more than 11 days during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI), at Cabauw, NL (51.97° N, 4.93° E). All visible instruments used a common wavelength range and set of cross sections for the spectral analysis. Most of the instruments were of the multi-axis design with analysis by differential spectroscopy software (MAX-DOAS), whose non-zenith slant columns were compared by examining slopes of their least-squares straight line fits to mean values of a selection of instruments, after taking 30-min averages. Zenith slant columns near twilight were compared by fits to interpolated values of a reference instrument, then normalised by the mean of the slopes of the best instruments. For visible MAX-DOAS instruments, the means of the fitted slopes for NO2 and O4 of all except one instrument were within 10% of unity at almost all non-zenith elevations, and most were within 5%. Values for UV MAX-DOAS instruments were almost as good, being 12% and 7%, respectively. For visible instruments at zenith near twilight, the means of the fitted slopes of all instruments were within 5% of unity. This level of agreement is as good as that of previous intercomparisons, despite the site not being ideal for zenith twilight measurements. It bodes well for the future of measurements of tropospheric NO2, as previous intercomparisons were only for zenith instruments focussing on stratospheric NO2, with their longer heritage.

A comparison of retrieved total column ozone (TCO) amounts between the Pandora #34 spectrometer system and the Dobson #061 spectrophotometer from direct-sun observations was performed on the roof of the Boulder, Colorado, NOAA building. This paper, part of an ongoing study, covers a 1-year period starting on 17 December 2013. Both the standard Dobson and Pandora TCO retrievals required a correction, TCOcorr = TCO (1 + C(T)), using a monthly varying effective ozone temperature, TE, derived from a temperature and ozone profile climatology. The correction is used to remove a seasonal difference caused by using a fixed temperature in each retrieval algorithm. The respective corrections C(TE) are CPandora = 0.00333(TE-225) and CDobson = -0.0013(TE-226.7) per degree K. After the applied corrections removed most of the seasonal retrieval dependence on ozone temperature, TCO agreement between the instruments was within 1 % for clear-sky conditions. For clear-sky observations, both co-located instruments tracked the day-to-day variation in total column ozone amounts with a correlation of r2 = 0.97 and an average offset of 1.1 ± 5.8 DU. In addition, the Pandora TCO data showed 0.3 % annual average agreement with satellite overpass data from AURA/OMI (Ozone Monitoring Instrument) and 1 % annual average offset with Suomi-NPP/OMPS (Suomi National Polar-orbiting Partnership, the nadir viewing portion of the Ozone Mapper Profiler Suite).

Long-term measurements by the AERONET program of spectral aerosol optical depth, precipitable water, and derived Angstrom exponent were analyzed and compiled into an aerosol optical properties climatology. Quality assured monthly means are presented and described for 9 primary sites and 21 additional multiyear sites with distinct aerosol regimes representing tropical biomass burning, boreal forests, midlatitude humid climates, midlatitude dry climates, oceanic sites, desert sites, and background sites. Seasonal trends for each of these nine sites are discussed and climatic averages presented.

The new infrared radiometer (conveyable low-noise infrared radiometer for measurements of atmosphere and ground surface targets, or CLIMAT) is a highly sensitive field instrument designed to measure brightness temperatures or radiances in the infrared, from the ground level, or from an aircraft. It can be equipped with up to six channels in the 8–14-μm range. This instrument is characterized by its portability (total mass less than 5 kg), its self-sufficiency, and its automated operation. It can be operated either manually or automatically. The optical head of the instrument contains an objective lens and a condenser mounted according to the Kohler design, providing a uniform irradiation on the detector and a well-delimited field of view. The radiation is measured by a low-noise fast thermopile whose responsivity is slightly temperature dependent. The radiometric noise expressed as an equivalent brightness temperature is on the order of 50 mK for a 1-μm bandwidth at room temperature. The applicat...

An analysis is presented for both ground- and satellite-based retrievals of total column ozone and nitrogen dioxide levels from the Washington, D.C., and Baltimore, Maryland, metropolitan area during the NASA-sponsored July 2011 campaign of Deriving Information on Surface COnditions from Column and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ). Satellite retrievals of total column ozone and nitrogen dioxide from the Ozone Monitoring Instrument (OMI) on the Aura satellite are used, while Pandora spectrometers provide total column ozone and nitrogen dioxide amounts from the ground. We found that OMI and Pandora agree well (residuals within ±25 % for nitrogen dioxide, and ±4.5 % for ozone) for a majority of coincident observations during July 2011. Comparisons with surface nitrogen dioxide from a Teledyne API 200 EU NOx Analyzer showed nitrogen dioxide diurnal variability that was consistent with measurements by Pandora. However, the wide OMI field of view, clouds, and aerosols affected retrievals on certain days, resulting in differences between Pandora and OMI of up to ±65 % for total column nitrogen dioxide, and ±23 % for total column ozone. As expected, significant cloud cover (cloud fraction >0.2) was the most important parameter affecting comparisons of ozone retrievals; however, small, passing cumulus clouds that do not coincide with a high (>0.2) cloud fraction, or low aerosol layers which cause significant backscatter near the ground affected the comparisons of total column nitrogen dioxide retrievals. Our results will impact post-processing satellite retrieval algorithms and quality control procedures.

We present new, high precision, high temporal resolution measurements of total column ozone (TCO) amounts derived from ground-based direct-sun irradiance measurements using our recently deployed Pandora single-grating spectrometers. Pandora's small size and portability allow deployment at multiple sites within an urban air-shed and development of a ground-based monitoring network for studying small-scale atmospheric dynamics, spatial heterogeneities in trace gas distribution, local pollution conditions, photochemical processes and interdependencies of ozone and its major precursors. Results are shown for four mid- to high-latitude sites where different Pandora instruments were used. Comparisons with a well calibrated double-grating Brewer spectrometer over a period of more than a year in Greenbelt MD showed excellent agreement and a small bias of approximately 2 DU (or, 0.6%). This was constant with slant column ozone amount over the full range of observed solar zenith angles (15-80), indicating adequate Pandora stray light correction. A small (1-2%) seasonal difference was found, consistent with sensitivity studies showing that the Pandora spectral fitting TCO retrieval has a temperature dependence of 1% per 3K, with an underestimation in temperature (e.g., during summer) resulting in an underestimation of TCO. Pandora agreed well with Aura-OMI (Ozone Measuring Instrument) satellite data, with average residuals of

From June to July 2009 more than thirty different in-situ and remote sensing instruments from all over the world participated in the Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI). The campaign took place at KNMI's Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands. Its main objectives were to determine the accuracy of state-of-the-art ground-based measurement techniques for the detection of atmospheric nitrogen dioxide (both in-situ and remote sensing), and to investigate their usability in satellite data validation. The expected outcomes are recommendations regarding the operation and calibration of such instruments, retrieval settings, and observation strategies for the use in ground-based networks for air quality monitoring and satellite data validation. Twenty-four optical spectrometers participated in the campaign, of which twenty-one had the capability to scan different elevation angles consecutively, the so-called Multi-axis DOAS systems, thereby collecting vertical profile information, in particular for nitrogen dioxide and aerosol. Various in-situ samplers and lidar instruments simultaneously characterized the variability of atmospheric trace gases and the physical properties of aerosol particles. A large data set of continuous measurements of these atmospheric constituents has been collected under various meteorological conditions and air pollution levels. Together with the permanent measurement capability at the CESAR site characterizing the meteorological state of the atmosphere, the CINDI campaign provided a comprehensive observational data set of atmospheric constituents in a highly polluted region of the world during summertime. First detailed comparisons performed with the CINDI data show that slant column measurements of NO2, O4 and HCHO with MAX-DOAS agree within 5 to 15%, vertical profiles of NO2 derived from several independent instruments agree within 25% of one another, and MAX-DOAS aerosol optical thickness agrees within 20–30% with AERONET data. For the in-situ NO2 instrument using a molybdenum converter, a bias was found as large as 5 ppbv during day time, when compared to the other in-situ instruments using photolytic converters.