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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∘×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, 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 × 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. [ABSTRACT FROM AUTHOR]

Aerosol backscatter coefficients were calculated using multiwavelength aerosol extinction products from the SAGE II and III/ISS instruments (SAGE: Stratospheric Aerosol and Gas Experiment). The conversion methodology is presented, followed by an evaluation of the conversion algorithm's robustness. The SAGE-based backscatter products were compared to backscatter coefficients derived from ground-based lidar at three sites (Table Mountain Facility, Mauna Loa, and Observatoire de Haute-Provence). Further, the SAGE-derived lidar ratios were compared to values from previous balloon and theoretical studies. This evaluation includes the major eruption of Mt. Pinatubo in 1991, followed by the atmospherically quiescent period beginning in the late 1990s. Recommendations are made regarding the use of this method for evaluation of aerosol extinction profiles collected using the occultation method. [ABSTRACT FROM AUTHOR]

Retrievals of vertical profiles of key atmospheric gases provide a critical long-term record from ground-based Fourier transform infrared (FTIR) solar absorption measurements. However, the characterization of the retrieved vertical profile structure can be difficult to validate, especially for gases with large vertical gradients and spatial–temporal variability such as water vapor. In this work, we evaluate the accuracy of the most common water vapor isotope (H216O , hereafter WV) FTIR retrievals in the lower and upper troposphere–lower stratosphere. Coincident high-quality vertically resolved WV profile measurements obtained from 2010 to 2016 with balloon-borne NOAA frost point hygrometers (FPHs) are used as reference to evaluate the performance of the retrieved profiles at two sites: Boulder (BLD), Colorado, and at the mountaintop observatory of Mauna Loa (MLO), Hawaii. For a meaningful comparison, the spatial–temporal variability has been investigated. We present results of comparisons among FTIR retrievals with unsmoothed and smoothed FPH profiles to assess WV vertical gradients. Additionally, we evaluate the quantitative impact of different a priori profiles in the retrieval of WV. An orthogonal linear regression analysis shows the best correlation among tropospheric layers using ERA-Interim (ERA-I) a priori profiles and biases are lower for unsmoothed comparisons. In Boulder, we found a negative bias of 0.02±1.9 % (r=0.95) for the 1.5–3 km layer. A larger negative bias of 11.1±3.5 % (r=0.97) was found in the lower free troposphere layer of 3–5 km attributed to rapid vertical change of WV, which is not always captured by the retrievals. The bias improves in the 5–7.5 km layer (1.0±5.3 %, r=0.94). The bias remains at about 13 % for layers above 7.5 km but below 13.5 km. At MLO the spatial mismatch is significantly larger due to the launch of the sonde being farther from the FTIR location. Nevertheless, we estimate a negative bias of 5.9±4.6 % (r=0.93) for the 3.5–5.5 km layer and 9.9±3.7 % (r=0.93) for the 5.5–7.5 km layer, and we measure positive biases of 6.2±3.6 % (r=0.95) for the 7.5–10 km layer and 12.6 % and greater values above 10 km. The agreement for the first layer is significantly better at BLD because the air masses are similar for both FTIR and FPH. Furthermore, for the first time we study the influence of different WV a priori profiles in the retrieval of selected gas profiles. Using NDACC standard retrievals we present results for hydrogen cyanide (HCN), carbon monoxide (CO), and ethane (C2H6) by taking NOAA FPH profiles as the ground truth and evaluating the impact of other WV profiles. We show that the effect is minor for C2H6 (bias <0.5 % for all WV sources) among all vertical layers. However, for HCN we found significant biases between 6 % for layers close to the surface and 2 % for the upper troposphere depending on the WV profile source. The best results (reduced bias and precision and r values closer to unity) are always found for pre-retrieved WV. Therefore, we recommend first retrieving WV to use in subsequent retrieval of gases. [ABSTRACT FROM AUTHOR]

The near-infrared (NIR) part of the solar spectrum is of prime importance for solar physics and climatology, directly intervening in the Earth's radiation budget. Despite its major role, available solar spectral irradiance (SSI) NIR datasets, space-borne or ground-based, present discrepancies caused by instrumental or methodological reasons. We present new results obtained from the PYR-ILIOS SSI NIR ground-based campaign, which is a replication of the previous IRSPERAD campaign which took place in 2011 at the Izaña Atmospheric Observatory (IZO). We used the same instrument and primary calibration source of spectral irradiance. A new site was chosen for PYR-ILIOS: the Mauna Loa Observatory (MLO) in Hawaii (3397 m a.s.l.), approximately 1000 m higher than IZO. Relatively to IRSPERAD, the methodology of monitoring the traceability to the primary calibration source was improved. The results as well as a detailed error budget are presented. We demonstrate that the most recent results, from PYR-ILIOS and other space-borne and ground-based experiments, show an NIR SSI lower than the previous reference spectrum, ATLAS3, for wavelengths above 1.6µm. [ABSTRACT FROM AUTHOR]