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.

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.

Abstract. We present two Differential Optical Absorption Spectroscopy (DOAS) instruments built at RIVM: the RIVM DOAS and the miniDOAS. Both instruments provide virtually interference-free measurements of NH 3 concentrations in the atmosphere, since they measure over an open path, without suffering from inlet problems or interference problems by ammonium aerosols dissociating on tubes or filters. They measure concentrations up to at least 200 µg m −3 , have a fast response, low maintenance demands, and a high uptime. The RIVM DOAS has a high accuracy of typically 0.15 µg m −3 for ammonia for 5-min averages and over a total light path of 100 m. The miniDOAS has been developed for application in measurement networks such as the Dutch National Air Quality Monitoring Network (LML). Compared to the RIVM DOAS it has a similar accuracy, but is significantly reduced in size, costs, and handling complexity. The RIVM DOAS and miniDOAS results showed excellent agreement (R 2 = 0.996) during a field measurement campaign in Vredepeel, the Netherlands. This measurement site is located in an agricultural area and is characterized by highly variable, but on average high ammonia concentrations in the air. The RIVM-DOAS and miniDOAS results were compared to the results of the AMOR instrument, a continuous-flow wet denuder system, which is currently used in the LML. Averaged over longer time spans of typically a day, the (mini)DOAS and AMOR results agree reasonably well, although an offset of the AMOR values compared to the (mini)DOAS results exists. On short time scales, the (mini)DOAS shows a faster response and does not show the memory effects due to inlet tubing and transport of absorption fluids encountered by the AMOR. Due to its high accuracy, high uptime, low maintenance and its open path, the (mini)DOAS shows a good potential for flux measurements by using two (or more) systems in a gradient set-up and applying the aerodynamic gradient technique.

Abstract. Multiple Axis Differential Optical AbsorptionSpectroscopy (MAX-DOAS) instruments can measure from the ground the absorption by nitrogen dioxide (NO 2 ) of scattered sunlight seen in multiple viewing directions. This paper studies the potential of this technique to derive the vertical distribution of NO 2 in the troposphere. Such profile information is essential for detailed comparisons of MAX-DOAS retrievals with other measurement techniques for NO 2 , e.g. with a lidar or from space.The retrieval algorithm used is based on a pre-calculated look-up table and assumes homogeneous mixing of aerosols and NO 2 in layers extending from the surface to a variable height. Two retrieval models are compared: one including and one excluding an elevated NO 2 layer at a fixed altitude in the free troposphere. An ensemble technique is applied to derive retrieval uncertainties.Sensitivity studies demonstrate that NO 2 in the free troposphere can only be retrieved accurately if: (i) the retrieved boundary layer profiles for aerosols and NO 2 correspond to the real ones, (ii) if the right a-priori choice is made for the (average) height of free tropospheric NO 2 , and (iii) if all other error sources are very low. It is shown that retrieval models that are capable of accurate NO 2 retrievals in the free troposphere, i.e. models not constrained too much by a-priori assumptions, have as a major disadvantage that they will frequently find free tropospheric NO 2 , also when it is not present in reality. This is a consequence of the fact that NO 2 in the free troposphere is poorly constrained by the MAX-DOAS observations, especially for high aerosol optical thickness values in the boundary layer. Retrieval of free tropospheric NO 2 is therefore sensitive to a large number of error sources. For this reason it is advised to firmly constrain free tropospheric NO 2 in MAX-DOAS retrieval models used Correspondence to: T. Vlemmix (vlemmix@knmi.nl) for applications such as satellite validation. This effectively makes free tropospheric NO 2 a source of error for MAX-DOAS retrieval of NO 2 profiles in the boundary layer.A comparison was performed with independent data, based on MAX-DOAS observations done at the CINDI campaign, held in the Netherlands in 2009. Comparison with lidar partial tropospheric NO 2 columns showed a correlation of 0.78, and an average difference of 0.1× 10 15 molec cm −2 . The diurnal evolution of the NO 2 volume mixing ratio measured by in-situ monitors at the surface and averaged over five days with cloud-free mornings, compares well to the MAX-DOAS retrieval: a correlation was found of 0.94, and an average difference of 0.04 ppb.

Abstract. Methods for the determination of ship fuel sulphur content and NO x emission factors based on remote measurements have been compared in the harbour of Rotterdam and compared to direct stack emission measurements on the ferry Stena Hollandica. The methods were selected based on a review of the available literature on ship emission measurements. They were either optical (LIDAR, Differential Optical Absorption Spectroscopy (DOAS), UV camera), combined with model-based estimates of fuel consumption, or based on the so called "sniffer" principle, where SO 2 or NO x emission factors are determined from simultaneous measurement of the increase of CO 2 and SO 2 or NO x concentrations in the plume of the ship compared to the background. The measurements were performed from stations at land, from a boat and from a helicopter. Mobile measurement platforms were found to have important advantages compared to the land-based ones because they allow optimizing the sampling conditions and sampling from ships on the open sea. Although optical methods can provide reliable results it was found that at the state of the art level, the "sniffer" approach is the most convenient technique for determining both SO 2 and NO x emission factors remotely. The average random error on the determination of SO 2 emission factors comparing two identical instrumental set-ups was 6 %. However, it was found that apparently minor differences in the instrumental characteristics, such as response time, could cause significant differences between the emission factors determined. Direct stack measurements showed that about 14 % of the fuel sulphur content was not emitted as SO 2 . This was supported by the remote measurements and is in agreement with the results of other field studies.