Abstract. Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of nitrous acid (HONO) and its precursor NO 2 (nitrogen dioxide) as well as aerosols have been performed daily in Beijing city centre (39.98 • N, 116.38 • E) from July 2008 to April 2009 and at the suburban site of Xianghe (39.75 • N, 116.96 • E) located ∼ 60 km east of Beijing from March 2010 to December 2012. This extensive dataset allowed for the first time the investigation of the seasonal cycle of HONO as well as its diurnal variation in and in the vicinity of a megacity. Our study was focused on the HONO and NO 2 near-surface concentrations (0-200 m layer) and total vertical column densities (VCDs) and also aerosol optical depths (AODs) and extinction coefficients retrieved by applying the Optimal Estimation Method to the MAX-DOAS observations. Monthly averaged HONO near-surface concentrations at local noon display a strong seasonal cycle with a maximum in late fall/winter (∼ 0.8 and 0.7 ppb at Beijing and Xianghe, respectively) and a minimum in summer (∼ 0.1 ppb at Beijing and 0.03 ppb at Xianghe). The seasonal cycles of HONO and NO 2 appear to be highly correlated, with correlation coefficients in the 0.7-0.9 and 0.5-0.8 ranges at Beijing and Xianghe, respectively. The stronger correlation of HONO with NO 2 and also with aerosols observed in Beijing suggests possibly larger role of NO 2 conversion into HONO in the Beijing city center than at Xianghe. The observed diurnal cycle of HONO near-surface concentration shows a maximum in the early morning (about 1 ppb at both sites) likely resulting from night-time accumulation, followed by a decrease to values of about 0.1-0.4 ppb around local noon. The HONO / NO 2 ratio shows a similar pattern with a maximum in the early morning (values up to 0.08) and a decrease to ∼ 0.01-0.02 around local noon. The seasonal and diurnal cycles of the HONO near-surface concentration are found to be similar in shape and in relative amplitude to the corresponding cycles of the HONO total VCD and are therefore likely driven mainly by the balance between HONO sources and the photolytic sink, whereas dilution effects appear to play only a minor role. The estimation of OH radical production from HONO and O 3 photolysis based on retrieved HONO near-surface concentrations and calculated photolysis rates indicate that in the 0-200 m altitude range, HONO is by far the largest source of OH radicals in winter as well as in the early morning at all seasons, while the contribution of O 3 dominates in summer from mid-morning until mid-afternoon.
We report on the retrieval of aerosol extinction profiles at four wavelengths from ground-based multi-axis differential absorption spectroscopy (MAXDOAS) measurements performed in Beijing, China. Measurements were made over a 10-month time period (June 2008 to April 2009) using a newly developed MAXDOAS instrument. A retrieval algorithm, based on an on-line implementation of the radiative transfer code LIDORT and the optimal estimation technique, has been designed to provide near real time information on aerosol extinction vertical profiles. The algorithm was applied to O<sub>4</sub> measurements at four wavelengths (360, 477, 577, and 630 nm). The total aerosol optical depths (AODs) calculated from the retrieved profiles exhibit higher values in spring and summer and lower values in autumn and winter. Comparison of the retrieved total AODs with values from a co-located CIMEL sunphotometer revealed a good correlation. The best results are obtained for the UV region with a correlation coefficient (<I>R</I>) of 0.91 and a slope of the linear regression fit of 1.1. At the longest wavelength, <I>R</I> drops down to 0.67 and the slope increases to 1.5. The results confirm that good quality O<sub>4</sub> slant column measurements are essential for the success of the retrievals. A method is presented to determine a correction factor to account for systematic errors. It is demonstrated that the algorithm is capable of reliably retrieving aerosol extinction profiles for a wide range of atmospheric conditions (total AODs at 360 nm ranging from about 0.1 to 3). The results open up new perspectives for the extension of the algorithm for the near real time retrieval of trace gas vertical profiles
Abstract. In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO 2 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 nonzenith 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 Correspondence to: H. K. Roscoe (h.roscoe@bas.ac.uk) 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 NO 2 and O 4 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 NO 2 , as previous intercomparisons were only for zenith instruments focussing on stratospheric NO 2 , with their longer heritage.Published by Copernicus Publications on behalf of the European Geosciences Union.
Environment (RIVM) NO 2 lidar. We show that NO 2 from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) compares well with in situ measurements. We show that different MAX-DOAS instruments, operating simultaneously during the campaign, give very similar results. We also provide unique information on the spatial homogeneity and the vertical and temporal variability of NO 2 , showing that during a number of days, the NO 2 columns derived from measurements in different directions varied significantly, which implies that, under polluted conditions, measurements in one single azimuth direction are not always representative for the averaged field that the satellite observes. In addition, we show that there is good agreement between tropospheric NO 2 from OMI and MAX-DOAS, and also between total NO 2 from OMI and directsun observations. Observations of the aerosol optical thickness (AOT) show that values derived with three ground-based instruments correspond well with each other, and with aerosol optical thicknesses observed by OMI.
[1] The Global Ozone Monitoring Instrument (GOME) was launched on European Space Agency's ERS-2 platform in April 1995. The GOME data processor (GDP) operational retrieval algorithm has generated total ozone columns since July 1995. In 2004 the GDP system was given a major upgrade to version 4.0, a new validation was performed, and the 10-year GOME level 1 data record was reprocessed. In two papers, we describe the GDP 4.0 retrieval algorithm and present an error budget and sensitivity analysis (paper 1) and validation of the GDP total ozone product and the overall accuracy of the entire GOME ozone record (paper 2). GDP 4.0 uses an optimized differential optical absorption spectroscopy (DOAS) algorithm, with air mass factor (AMF) conversions calculated using the radiative transfer code linearized discrete ordinate radiative transfer (LIDORT). AMF computation is based on the TOMS version 8 ozone profile climatology, classified by total column, and AMFs are adjusted iteratively to reflect the DOAS slant column result. GDP 4.0 has improved wavelength calibration and reference spectra and includes a new molecular Ring correction to deal with distortion of ozone absorption features due to inelastic rotational Raman scattering effects. Preprocessing for cloud parameter estimation in GDP 4.0 is done using two new cloud correction algorithms: OCRA and ROCINN. For clear and cloudy scenes the precision of the ozone column product is better than 2.4 and 3.3%, respectively, for solar zenith angles up to 80°. Comparisons with ground-based data are generally at the 1-1.5% level or better for all regions outside the poles.Citation: Van Roozendael, M., et al. (2006), Ten years of GOME/ERS-2 total ozone data-The new GOME data processor (GDP) version 4: 1. Algorithm description,
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