Nitrogen oxides (NOx = NO + NO2) in the atmosphere are often measured using instruments equipped with molybdenum converters. NO2 is catalytically converted to NO on a heated molybdenum surface and subsequently measured by chemiluminescence after reaction with ozone. The drawback of this technique is that other oxidized nitrogen compounds such as peroxyacetyl nitrate and nitric acid are also partly converted to NO. Thus such NO2 measurements are really surrogate NO2 measurements because the resultant values systematically overestimate the true value because of interferences of these compounds, especially when sampling photochemically aged air masses. However, molybdenum converters are widely used, and a dense network of surrogate NO2 measurements exists. As an alternative with far less interference, photolytic converters using ultraviolet light are nowadays applicable also for long‐term measurements. This work presents long‐term collocated NO2 measurements using molybdenum and photolytic converters at two rural sites in Switzerland. On a relative scale, the molybdenum converter instruments overestimate the NO2 concentrations most during spring/summer because of prevalent photochemistry. On a monthly basis, only 70–83% of the “surrogate” NO2 can be attributed to “real” NO2 at the non‐elevated site and even less (43–76%) at the elevated one. The observed interferences have to be taken into account for monitoring and regulatory issues and to be considered when using these data for ground‐truthing of satellite data or for validation of chemical transport models. Alternatively, an increased availability of artifact‐free data would also be beneficial for these issues.
Abstract.Results of continuous nitrogen oxide (NO), nitrogen dioxide (NO 2 ), peroxyacetyl nitrate (PAN) and total reactive nitrogen (NO y ) measurements along with seasonal field campaigns of nitric acid (HNO 3 ) and particulate nitrate (NO − 3 ) measurements are presented for a two-year period at the high-alpine research station Jungfraujoch (JFJ), 3580 m asl. The NO y mixing ratio and partitioning is shown to strongly depend on meteorological conditions. Knowledge of these meteorological transport processes allows discrimination between undisturbed (i.e. clean) and disturbed (i.e. influenced by regional pollution sources) free tropospheric (FT) conditions at the JFJ. Median NO y concentrations during undisturbed FT periods ranged from 350 pptv (winter, December to February) to 581 pptv (spring, March to May). PAN was found to be the dominant NO y species during spring and summer, whereas NO 2 was most abundant during autumn and winter. Particulate nitrate was found to contribute significantly to total NO y during thermally induced vertical transport. Föhn events, synoptical lifting (e.g. fronts) and thermally induced vertical transport resulted in mixing ratios up to 10 times higher at the JFJ compared to undisturbed FT conditions. Furthermore this meteorological variability of the NO y concentration and partitioning often dominated the seasonal variability. As a consequence the use of filters at the JFJ (and other mountainous sites) is crucial for the interpretation of data from such measurement sites. This study presents a further development of meteorological filters for the high-alpine site Jungfraujoch, which also could be modified and adapted to other mountainous measurement sites.
Published by Copernicus Publications on behalf of the European Geosciences Union. 458 A. J. M. Piters et al.: The CINDI campaign: design, execution and early resultsAbstract. 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-ofthe-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 CE-SAR 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 NO 2 , O 4 and HCHO with MAX-DOAS agree within 5 to 15 %, vertical profiles of NO 2 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 NO 2 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.
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 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 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 Cabauw 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 NO<sub>2</sub>, O<sub>4</sub> and HCHO with MAX-DOAS agree within 5 to 15%, vertical profiles of NO<sub>2</sub> derived from several independent instruments agree within 25%, and MAX-DOAS aerosol optical thickness agrees within 20–30% with AERONET data. For the in-situ NO<sub>2</sub> 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
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