Recalculation of 11‐year total ozone of Brewer spectrophotometer 115

Author name used in this publication: K. S. Lam2007-2008 > Academic research: refereed > Publication in refereed journalVersion of RecordPublishe

Improved retrieval of nitrogen dioxide (NO2) column densities by means of MKIV Brewer spectrophotometers

A new algorithm to retrieve nitrogen dioxide (NO2) column densities using MKIV ("Mark IV") Brewer spectrophotometers is described. The method includes several improvements, such as a more recent spectroscopic data set, the reduction of measurement noise, interference by other atmospheric species and instrumental settings, and a better determination of the zenith sky air mass factor. The technique was tested during an ad hoc calibration campaign at the high-altitude site of Izaña (Tenerife, Spain) and the results of the direct sun and zenith sky geometries were compared to those obtained by two reference instruments from the Network for the Detection of Atmospheric Composition Change (NDACC): a Fourier Transform Infrared Radiometer (FTIR) and an advanced visible spectrograph (RASAS-II) based on the differential optical absorption spectrometry (DOAS) technique

A calibration procedure which accounts for non-linearity in single-monochromator Brewer ozone spectrophotometer measurements

It is now known that single-monochromator Brewer spectrophotometer ozone and sulfur dioxide measurements suffer from non-linearity at large ozone slant column amounts due to the presence of instrumental stray light caused by scattering within the optics of the instrument. Because of the large gradient in the ozone absorption spectrum in the near-ultraviolet, the atmospheric spectra measured by the instrument possess a very large gradient in intensity in the 300 to 325&thinsp;nm wavelength region. This results in a significant sensitivity to stray light when there is more than 1000 Dobson units (DU) of ozone in the light path. As the light path (air mass) through ozone increases, the stray-light effect on the measurements also increases. The measurements can be of the order of 10&thinsp;%, low for an ozone column of 600&thinsp;DU and an air mass factor of 3 (1800&thinsp;DU slant column amount), which is an example of conditions that produce large slant column amounts. Primary calibrations for the Brewer instrument are carried out at Mauna Loa Observatory in Hawaii and Izana Observatory in Tenerife. They are done using the Langley plot method to extrapolate a set of measurements made under a constant ozone vertical column to an extraterrestrial calibration constant. Since the effects of a small non-linearity at moderate ozone paths may still be important, a better calibration procedure should account for the non-linearity of the instrument response. Studies involving the scanning of a laser source have been used to characterize the stray-light response of the Brewer (Fioletov et al., 2000), but until recently these data have not been used to elucidate the relationship between the stray-light response and the ozone measurement non-linearity. In a study done by Karppinen et al. (2015), a method for correcting stray light has been presented that uses an additive correction, which is determined via instrument slit characterization and a radiative transfer model simulation and is then applied to the single Brewer data (Karppinen et al., 2015). The European Brewer Network is also applying stray-light corrections, which includes an iterative process that results in correcting the single Brewer data to agree with double Brewer data (Rimmer et al., 2018; Redondas et al., 2018). The first model requires measurements of the slit function and the latter method relies on a calibrated instrument, such as a double Brewer, to characterize the instrument and to determine a correction for stray light. This paper presents a simple and practical method to correct for the effects of stray light, which includes a mathematical model of the instrument response and a non-linear retrieval approach that calculates the best values for the model parameters. The model can then be used in reverse to provide more accurate ozone values up to a defined maximum ozone slant path. The parameterization used was validated using an instrument physical model simulation. This model can be applied independently to any Brewer instrument and correct for the effects of stray light.</p

Performance of the ground-based total ozone network assessed using satellite data

Dobson and Brewer spectrophotometer and filter ozonometer data available from the World Ozone and Ultraviolet Data Centre (WOUDC) were compared with satellite total ozone measurements from TOMS (onboard Nimbus 7, Meteor 3, and Earth Probe satellites), OMI (AURA satellite) and GOME (ERS-2 satellite) instruments. Five characteristics of the difference with satellite data were calculated for each site and instrument type: the mean difference, the standard deviation of daily differences, the standard deviation of monthly differences, the amplitude of the seasonal component of the difference, and the range of annual values. All these characteristics were calculated for five 5-year-long bins and for each site separately for direct sun (DS) and zenith sky (ZS) ozone measurements. The main percentiles were estimated for the five characteristics of the difference and then used to establish criteria for “suspect” or “outlier” sites for each characteristic. About 61% of Dobson, 46% of Brewer, and 28% of filter stations located between 60°S and 60°N have no “suspect” or “outlier” characteristics. In nearly 90% of all cases, Dobson and Brewer sites demonstrated 5-year mean differences with satellites to be within ±3% (for DS observations). The seasonal median difference between all Brewer DS measurements at 25°–60°N and GOME and OMI overpasses remained within ±0.5% over a period of more than 10 years (...

Temperature dependence of the Brewer global UV measurements

Spectral measurements of global UV irradiance recorded by Brewer spectrophotometers can be significantly affected by instrument-specific optical and mechanical features. Thus, proper corrections are needed in order to reduce the associated uncertainties to within acceptable levels. The present study aims to contribute to the reduction of uncertainties originating from changes in the Brewer internal temperature, which affect the performance of the optical and electronic parts, and subsequently the response of the instrument. Until now, measurements of the irradiance from various types of lamps at different temperatures have been used to characterize the instruments' temperature dependence. The use of 50 W lamps was found to induce errors in the characterization due to changes in the transmissivity of the Teflon diffuser as it warms up by the heat of the lamp. In contrast, the use of 200 or 1000 W lamps is considered more appropriate because they are positioned at longer distances from the diffuser so that warming is negligible. Temperature gradients inside the instrument can cause mechanical stresses which can affect the instrument's optical characteristics. Therefore, during the temperature-dependence characterization procedure warming or cooling must be slow enough to minimize these effects. In this study, results of the temperature characterization of eight different Brewer spectrophotometers operating in Greece, Finland, Germany and Spain are presented. It was found that the instruments' response changes differently in different temperature regions due to different responses of the diffusers' transmittance. The temperature correction factors derived for the Brewer spectrophotometers operating at Thessaloniki, Greece, and Sodankylä, Finland, were evaluated and were found to remove the temperature dependence of the instruments' sensitivity.This article is based upon work from COST Action ES1207 “A European Brewer Network (EUBREWNET)”, supported by COST (European Cooperation in Science and Technology) and from the ENV59-ATMOZ (“Traceability for atmospheric total column ozone”) Joint Research Programme (JRP)

Validation of ACE and OSIRIS ozone and NO2 measurements using ground-based instruments at 80 degrees N

The Optical Spectrograph and Infra-Red Imager System (OSIRIS) and the Atmospheric Chemistry Experiment (ACE) have been taking measurements from space since 2001 and 2003, respectively. This paper presents intercomparisons between ozone and NO2 measured by the ACE and OSIRIS satellite instruments and by ground-based instruments at the Polar Environment Atmospheric Research Laboratory (PEARL), which is located at Eureka, Canada (80A degrees N, 86A degrees W) and is operated by the Canadian Network for the Detection of Atmospheric Change (CANDAC). The ground-based instruments included in this study are four zenith-sky differential optical absorption spectroscopy (DOAS) instruments, one Bruker Fourier transform infrared spectrometer (FTIR) and four Brewer spectrophotometers. Ozone total columns measured by the DOAS instruments were retrieved using new Network for the Detection of Atmospheric Composition Change (NDACC) guidelines and agree to within 3.2%. The DOAS ozone columns agree with the Brewer spectrophotometers with mean relative differences that are smaller than 1.5%. This suggests that for these instruments the new NDACC data guidelines were successful in producing a homogenous and accurate ozone dataset at 80A degrees N. Satellite 14-52 km ozone and 17-40 km NO2 partial columns within 500 km of PEARL were calculated for ACE-FTS Version 2.2 (v2.2) plus updates, ACE-FTS v3.0, ACE-MAESTRO (Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) v1.2 and OSIRIS SaskMART v5.0x ozone and Optimal Estimation v3.0 NO2 data products. The new ACE-FTS v3.0 and the validated ACE-FTS v2.2 partial columns are nearly identical, with mean relative differences of 0.0 +/- 0.2% and -0.2 +/- 0.1% for v2.2 minus v3.0 ozone and NO2, respectively. Ozone columns were constructed from 14-52 km satellite and 0-14 km ozonesonde partial columns and compared with the ground-based total column measurements. The satellite-plus-sonde measurements agree with the ground-based ozone total columns with mean relative differences of 0.1-7.3%. For NO2, partial columns from 17 km upward were scaled to noon using a photochemical model. Mean relative differences between OSIRIS, ACE-FTS and ground-based NO2 measurements do not exceed 20%. ACE-MAESTRO measures more NO2 than the other instruments, with mean relative differences of 25-52%. Seasonal variation in the differences between NO2 partial columns is observed, suggesting that there are systematic errors in the measurements and/or the photochemical model corrections. For ozone spring-time measurements, additional coincidence criteria based on stratospheric temperature and the location of the polar vortex were found to improve agreement between some of the instruments. For ACE-FTS v2.2 minus Bruker FTIR, the 2007-2009 spring-time mean relative difference improved from -5.0 +/- 0.4% to -3.1 +/- 0.8% with the dynamical selection criteria. This was the largest improvement, likely because both instruments measure direct sunlight and therefore have well-characterized lines-of-sight compared with scattered sunlight measurements. For NO2, the addition of a +/- 1A degrees latitude coincidence criterion improved spring-time intercomparison results, likely due to the sharp latitudinal gradient of NO2 during polar sunrise. The differences between satellite and ground-based measurements do not show any obvious trends over the missions, indicating that both the ACE and OSIRIS instruments continue to perform well

Properties of Sarychev sulphate aerosols over the Arctic

Aerosols from the Sarychev Peak volcano entered the Arctic region less than a week after the strongest SO2 eruption on June 15 and 16, 2009 and had, by the second week in July, spread out over the entire Arctic region. These predominantly stratospheric aerosols were determined to be sub-micron in size and inferred to be composed of sulphates produced from the condensation of SO2 gases emitted during the eruption. Average (500 nm) Sarychev-induced stratospheric optical depths over the Polar Environmental Atmospheric Research Laboratory (PEARL) at Eureka, Nunavut, Canada were found to be between 0.03 and 0.05 during the months of July and August, 2009. This estimate, derived from sunphotometry and integrated lidar backscatter profiles was consistent with averages derived from lidar estimates over Ny-Ålesund (Spitsbergen). The Sarychev SOD e-folding time at Eureka, deduced from lidar profiles, was found to be approximately 4 months relative to a regression start date of July 27. These profiles initially revealed the presence of multiple Sarychev plumes between the tropopause and about 17 km altitude. After about two months, the complex vertical plume structures had collapsed into fewer, more homogeneous plumes located near the tropopause. It was found that the noisy character of daytime backscatter returns induced an artifactual minimum in the temporal, pan-Arctic, CALIOP SOD response to Sarychev sulphates. A depolarization ratio discrimination criterion was used to separate the CALIOP stratospheric layer class into a low depolarization subclass which was more representative of Sarychev sulphates. Post-SAT (post Sarychev Arrival Time) retrievals of the fine mode effective radius (reff,f) and the logarithmic standard deviation for two Eureka sites and Thule, Greenland were all close to 0.25 μm and 1.6 respectively. The stratospheric analogue to the columnar reff,f average was estimated to be reff,f(+) = 0.29 μm for Eureka data. Stratospheric, Raman lidar retrievals at Ny-Ålesund, yielded a post-SAT average of reff,f(+) = 0.27 μm. These results are ~ 50% larger than the background stratospheric-aerosol value. They are also about a factor of two larger than modeling values used in recent publications or about a factor of five larger in terms of (per particle) backscatter cross section

Advanced NO2 retrieval technique for the Brewer spectrophotometer applied to the 20-year record in Rome, Italy

A re-evaluated data set of nitrogen dioxide (NO2) column densities over Rome for the years 1996 to 2017 is here presented. This long-term record is obtained from ground-based direct sun measurements with a MkIV Brewer spectrophotometer (serial number #067) and further reprocessed using a novel algorithm. Compared to the original Brewer algorithm, the new method includes updated NO2 absorption cross sections and Rayleigh scattering coefficients, and it accounts for additional atmospheric compounds and instrumental artefacts, such as the spectral transmittance of the filters, the alignment of the wavelength scale, and internal temperature. Moreover, long-term changes in the Brewer radiometric sensitivity are tracked using statistical methods for in-field calibration. The resulting series presents only a few (about 30) periods with missing data longer than 1 week and features NO2 retrievals for more than 6100ĝ€¯d, covering nearly 80ĝ€¯% of the considered 20-year period. The high quality of the data is demonstrated by two independent comparisons. In the first intensive campaign, Brewer #067 is compared against another Brewer (#066), recently calibrated at the Izaña Atmospheric Observatory through the Langley method and there compared to reference instrumentation from the Network for the Detection of Atmospheric Composition Change (NDACC). Data from this campaign show a highly significant Pearson's correlation coefficient of 0.90 between the two series of slant column densities (SCDs), slope 0.98 and offset 0.05ĝ€¯DU (Dobson units; 1.3×1015ĝ€¯molec.cm-2). The average bias between the vertical column densities is 0.03ĝ€¯DU (8.1×1014ĝ€¯molec.cm-2), well within the combined uncertainty of both instruments. Brewer #067 is also independently compared with new-generation instrumentation, a co-located Pandora spectrometer (#117), over a 1-year-long period (2016-2017) at Sapienza University of Rome, showing linear correlation indices above 0.96 between slant column densities, slope of 0.97, and offset of 0.02ĝ€¯DU (5.4×1014ĝ€¯molec.cm-2). The average bias between vertical column densities is negligible (-0.002ĝ€¯DU or -5.4×1013ĝ€¯molec.cm-2). This, incidentally, represents the first intercomparison of NO2 retrievals between a MkIV Brewer and a Pandora instrument. Owing to its accuracy and length, the Brewer data set collected in Rome can be useful for satellite calibration/validation exercises, comparison with photochemical models, and better aerosol optical depth estimates (NO2 optical depth climatology). In addition, it can be employed to identify long-term trends in NO2 column densities in a metropolitan environment, over two decades witnessing important changes in environmental policies, emission loads and composition, and the effect of a worldwide economic recession, to offer just a few examples. The method can be replicated on the more than 80 MkIV spectrophotometers operating worldwide in the frame of the international Brewer network. The NO2 data set described in this paper can be freely accessed at 10.5281/zenodo.4715219