Articles | Volume 10, issue 10
Atmos. Meas. Tech., 10, 3719–3742, 2017
Atmos. Meas. Tech., 10, 3719–3742, 2017

Research article 12 Oct 2017

Research article | 12 Oct 2017

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

Yang Wang1,2, Steffen Beirle1, Francois Hendrick3, Andreas Hilboll4,5, Junli Jin6,7, Aleksandra A. Kyuberis8, Johannes Lampel9,1, Ang Li2, Yuhan Luo2, Lorenzo Lodi10, Jianzhong Ma6, Monica Navarro11, Ivan Ortega12, Enno Peters4, Oleg L. Polyansky10,8, Julia Remmers1, Andreas Richter4, Olga Puentedura11, Michel Van Roozendael3, André Seyler4, Jonathan Tennyson10, Rainer Volkamer12, Pinhua Xie2,13, Nikolai F. Zobov8, and Thomas Wagner1 Yang Wang et al.
  • 1Max Planck Institute for Chemistry, Mainz, Germany
  • 2Anhui Institute of Optics and Fine Mechanics, Key Laboratory of Environmental Optics and Technology, Chinese Academy of Sciences, Hefei, 230031, China
  • 3Belgian Institute for Space Aeronomy – BIRA-IASB, Brussels, Belgium
  • 4Institute of Environmental Physics, University of Bremen, Bremen, Germany
  • 5Center for Marine Environmental Sciences (MARUM), University of Bremen, Bremen, Germany
  • 6Chinese Academy of Meteorological Sciences, Beijing, China
  • 7CMA Meteorological Observation Centre, Beijing, China
  • 8Institute of Applied Physics, Russian Academy of Sciences, Nizhny Novgorod, Russia
  • 9Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
  • 10Department of Physics and Astronomy, University College London, Gower St, London, WC1E 6BT, UK
  • 11Area de Investigación e Instrumentación Atmosférica, INTA, Torrejón de Ardoz, Spain
  • 12Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA
  • 13CAS Center for Excellence in Urban Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China

Abstract. In order to promote the development of the passive DOAS technique the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) was held at the Max Planck Institute for Chemistry in Mainz, Germany, from June to October 2013. Here, we systematically compare the differential slant column densities (dSCDs) of nitrous acid (HONO) derived from measurements of seven different instruments. We also compare the tropospheric difference of SCDs (delta SCD) of HONO, namely the difference of the SCDs for the non-zenith observations and the zenith observation of the same elevation sequence. Different research groups analysed the spectra from their own instruments using their individual fit software. All the fit errors of HONO dSCDs from the instruments with cooled large-size detectors are mostly in the range of 0.1 to 0.3  ×  1015 molecules cm−2 for an integration time of 1 min. The fit error for the mini MAX-DOAS is around 0.7  ×  1015 molecules cm−2. Although the HONO delta SCDs are normally smaller than 6  ×  1015 molecules cm−2, consistent time series of HONO delta SCDs are retrieved from the measurements of different instruments. Both fits with a sequential Fraunhofer reference spectrum (FRS) and a daily noon FRS lead to similar consistency. Apart from the mini-MAX-DOAS, the systematic absolute differences of HONO delta SCDs between the instruments are smaller than 0.63  ×  1015 molecules cm−2. The correlation coefficients are higher than 0.7 and the slopes of linear regressions deviate from unity by less than 16 % for the elevation angle of 1°. The correlations decrease with an increase in elevation angle. All the participants also analysed synthetic spectra using the same baseline DOAS settings to evaluate the systematic errors of HONO results from their respective fit programs. In general the errors are smaller than 0.3  ×  1015 molecules cm−2, which is about half of the systematic difference between the real measurements.

The differences of HONO delta SCDs retrieved in the selected three spectral ranges 335–361, 335–373 and 335–390 nm are considerable (up to 0.57  ×  1015 molecules cm−2) for both real measurements and synthetic spectra. We performed sensitivity studies to quantify the dominant systematic error sources and to find a recommended DOAS setting in the three spectral ranges. The results show that water vapour absorption, temperature and wavelength dependence of O4 absorption, temperature dependence of Ring spectrum, and polynomial and intensity offset correction all together dominate the systematic errors. We recommend a fit range of 335–373 nm for HONO retrievals. In such fit range the overall systematic uncertainty is about 0.87  ×  1015 molecules cm−2, much smaller than those in the other two ranges. The typical random uncertainty is estimated to be about 0.16  ×  1015 molecules cm−2, which is only 25 % of the total systematic uncertainty for most of the instruments in the MAD-CAT campaign. In summary for most of the MAX-DOAS instruments for elevation angle below 5°, half daytime measurements (usually in the morning) of HONO delta SCD can be over the detection limit of 0.2  ×  1015 molecules cm−2 with an uncertainty of  ∼  0.9  ×  1015 molecules cm−2.

Short summary
Slant column densities of nitrous acid (HONO) derived from different MAX-DOAS instruments and retrieval software are systematically compared for the first time during the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) campaign held at MPIC in Mainz, Germany, from June to October 2013. Through the inter-comparisons and sensitivity studies we quantified the uncertainties in the DOAS fits of HONO from different sources and concluded a recommended setting.