ICAD RELATED PUBLICATIONS
In situ measurement studies involving ICAD instruments
In situ measurement studies involving ICAD instruments
The spatial recording of the pollutant distribution of nitrogen dioxide (NO2) in an urban area can be realized by the new mobile ICAD measurement technology with limited costs and effort. Repeated measurements at different times are carried out on a fixed route, e.g. with a bicycle, in order to calculate a reliable mean distribution and an extrapolated annual mean value. The possibility of these measurements is illustrated using the example of a study in the city of Walldorf.
(Article in german.)
Ausgabe / Jahr: 3 / 2021
This report summarises the result of a project for high emitter heavy duty vehicle (HDV) detection in Denmark (17.9. – 01.10.2020) and followed police inspection of the HDV with high and suspicious emissions. The project is carried out as a collaboration between the Danish Road Traffic Authority, the Danish National Police and Airyx.
Proof of concept investigations for MANN+HUMMEL Filter Cube Installation at Stuttgart, Neckartor (German version). Experiments were conducted in 2019 with three hardware configurations, showing the effectiveness of fine dust filter setups as well as activated carbon filter elements on the respective immission levels.
What new applications are offered by a measuring device for nitrogen oxides developed at the Institute of Environmental Physics and now commercially available in the field of mobile immission and emission measurements under real conditions? The following article exemplifies some approaches to provide citizens and decision-makers with reliable and realistic measurement data in the short term, so that necessary and targeted measures for the reduction of air pollutants in cities can be taken.
This includes the mobile determination of the distribution of the legally regulated nitrogen dioxide (NO2), area-wide or in specific problem areas. Furthermore, real emission measurements by means of plume chasing enable the rapid and simple determination of the pollutant emissions of individual vehicles, e.g. buses and trucks. In Europe-wide studies, high nitrogen oxide (NOx) emissions have been identified on various vehicles, indicating to authorities systematically increased emissions, defective or potentially manipulated emission control systems.
(Article in german.)
Ausgabe / Jahr: 3 / 2019
Horbanski, M., Pöhler, D., Lampel, J., and Platt, U.: The ICAD (iterative cavity-enhanced DOAS) method, Atmos. Meas. Tech., 12, 3365–3381, https://doi.org/10.5194/amt-12-3365-2019, 2019.
Cavity-enhanced differential optical absorption spectroscopy (CE-DOAS or BB-CEAS DOAS) allows us to make in situ measurements while maintaining the kilometre-long light paths required by DOAS. This technique has been successfully used for several years to measure in situ atmospheric trace gases. A property of optical cavities is that in the presence of strong absorbers or scatterers the light path is reduced, in contrast to classical long-path DOAS measurements where the light path is fixed. Typical CE-DOAS or BB-CEAS evaluation schemes correct this effect using the measured total light intensity attenuation. This makes them sensitive to any variations in the light intensity not arising from the trace gas absorption. That means an important DOAS advantage, to be independent of total light intensity, is actually lost. In order to cope with this problem, the instrument setup would require a thorough stabilisation of the light source and a very rigid mechanical setup, which would make instrumentation more complex and error prone.
We present a new approach to cavity-enhanced (CE) DOAS based on an iterative algorithm (ICAD) which actually models the light path reduction from the derived absorbers in the optical resonator. It allows a sensitive and robust data analysis that does not depend on the total light intensity, allowing a simpler and more compact instrument setup. The algorithm is discussed and simulated measurements demonstrate its sensitivity and robustness. Furthermore, a new ICAD NO2 instrument is presented. It takes advantage of the advanced data evaluation to build a compact (50 cm cavity) and lightweight instrument (<10 kg) with low power consumption (25 W) for sensitive measurements of NO2 with a detection limit of 0.02 ppbv at an averaging time of 7 min. The instrument is characterised with a NO2 calibration source and good long-term stability is demonstrated in a comparison with a commercial chemiluminescence detector. As a new application of ICAD we show measurements on an automobile platform to investigate the two-dimensional NO2 distribution in an urban area. The instrument is so robust that even strong vibrations do not lead to any measurement problems.
Passive remote sensing measurement studies involving SKYSPEC instruments or data analysis methods
Tirpitz, J.-L., Frieß, U., Spurr, R., and Platt, U.: Enhancing MAX-DOAS atmospheric state retrievals by multispectral polarimetry – studies using synthetic data, Atmos. Meas. Tech., 15, 2077–2098, https://doi.org/10.5194/amt-15-2077-2022, 2022.
Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) is a widely used measurement technique for the remote detection of atmospheric aerosol and trace gases. The technique relies on the analysis of ultra-violet and visible radiation spectra of scattered sunlight (skylight) to obtain information on different atmospheric parameters. From an appropriate set of spectra recorded under different viewing directions (typically a group of observations at different elevation angles) the retrieval of aerosol and trace gas vertical distributions is achieved through numerical inversion methods.
It is well known that the polarisation state of skylight is particularly sensitive to atmospheric aerosol content as well as aerosol properties and that polarimetric measurements could therefore provide additional information for MAX-DOAS profile retrievals; however, such measurements have not yet been used for this purpose. To address this issue, we have developed the RAPSODI (Retrieval of Atmospheric Parameters from Spectroscopic Observations using DOAS Instruments) algorithm. In contrast to existing MAX-DOAS algorithms, it can process polarimetric information, and it can retrieve simultaneously profiles of aerosols and various trace gases at multiple wavelengths in a single retrieval step; a further advantage is that it contains a Mie scattering model, allowing for the retrieval of aerosol microphysical properties. The forward-model component in RAPSODI is based on a linearised vector radiative transfer model with Jacobian facilities, and we have used this model to create a database of synthetic measurements in order to carry out sensitivity analyses aimed at assessing the potential of polarimetric MAX-DOAS observations. We find that multispectral polarimetry significantly enhances the sensitivity, particularly to aerosol-related quantities. Assuming typical viewing geometries, the degrees of freedom for signal (DOFS) increase by about 50 % and 70 % for aerosol vertical distributions and aerosol properties, respectively, and by approximately 10 % for trace gas vertical profiles. For an idealised scenario with a horizontally homogeneous atmosphere, our findings predict an improvement in the inversion results’ accuracy (root-mean-square deviations to the true values) of about 60 % for aerosol vertical column densities (VCDs) as well as for aerosol surface concentrations and by 40 % for aerosol properties. For trace gas VCDs, very little improvement is apparent, although the accuracy of trace gas surface concentrations improves by about 50 %.
Diese Richtlinie beschreibt das passive DOAS-Messverfahren mit natürlichen Strahlungsquellen, das vor allem für die Absorptionsspektroskopie im ultraviolettem sowie im sichtbaren und nahinfraroten Spektralbereich zum Einsatz kommt. Aufbau, Betrieb, Mindestanforderungen, Kalibrierung und Datenauswertung von Passiv-DOAS-Messsystemen sowie deren Anwendung für Messungen von gasförmigen Komponenten (z.B. SO2, NO2, O3, HCHO, H2O, HONO) sowie von Aerosoleigenschaften in der Atmosphäre werden erläutert. Das Verfahren wird durch eine Vielzahl an Anwendungen illustriert.
Tirpitz, J.-L., Frieß, U., Hendrick, F., Alberti, C., Allaart, M., Apituley, A., Bais, A., Beirle, S., Berkhout, S., Bognar, K., Bösch, T., Bruchkouski, I., Cede, A., Chan, K. L., den Hoed, M., Donner, S., Drosoglou, T., Fayt, C., Friedrich, M. M., Frumau, A., Gast, L., Gielen, C., Gomez-Martín, L., Hao, N., Hensen, A., Henzing, B., Hermans, C., Jin, J., Kreher, K., Kuhn, J., Lampel, J., Li, A., Liu, C., Liu, H., Ma, J., Merlaud, A., Peters, E., Pinardi, G., Piters, A., Platt, U., Puentedura, O., Richter, A., Schmitt, S., Spinei, E., Stein Zweers, D., Strong, K., Swart, D., Tack, F., Tiefengraber, M., van der Hoff, R., van Roozendael, M., Vlemmix, T., Vonk, J., Wagner, T., Wang, Y., Wang, Z., Wenig, M., Wiegner, M., Wittrock, F., Xie, P., Xing, C., Xu, J., Yela, M., Zhang, C., and Zhao, X.: Intercomparison of MAX-DOAS vertical profile retrieval algorithms: studies on field data from the CINDI-2 campaign, Atmos. Meas. Tech., 14, 1–35, https://doi.org/10.5194/amt-14-1-2021, 2021.
The second Cabauw Intercomparison of Nitrogen Dioxide measuring Instruments (CINDI-2) took place in Cabauw (the Netherlands) in September 2016 with the aim of assessing the consistency of multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of tropospheric species (NO2, HCHO, O3, HONO, CHOCHO and O4). This was achieved through the coordinated operation of 36 spectrometers operated by 24 groups from all over the world, together with a wide range of supporting reference observations (in situ analysers, balloon sondes, lidars, long-path DOAS, direct-sun DOAS, Sun photometer and meteorological instruments). (…)
Donner, S., Kuhn, J., Van Roozendael, M., Bais, A., Beirle, S., Bösch, T., Bognar, K., Bruchkouski, I., Chan, K. L., Dörner, S., Drosoglou, T., Fayt, C., Frieß, U., Hendrick, F., Hermans, C., Jin, J., Li, A., Ma, J., Peters, E., Pinardi, G., Richter, A., Schreier, S. F., Seyler, A., Strong, K., Tirpitz, J.-L., Wang, Y., Xie, P., Xu, J., Zhao, X., and Wagner, T.: Evaluating different methods for elevation calibration of MAX-DOAS (Multi AXis Differential Optical Absorption Spectroscopy) instruments during the CINDI-2 campaign, Atmos. Meas. Tech., 13, 685–712, https://doi.org/10.5194/amt-13-685-2020, 2020.
We present different methods for in-field elevation calibration of MAX-DOAS (Multi AXis Differential Optical Absorption Spectroscopy) instruments that were applied and inter-compared during the second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2). One necessary prerequisite of consistent MAX-DOAS retrievals is a precise and accurate calibration of the elevation angles of the different measuring systems. Therefore, different methods for this calibration were applied to several instruments during the campaign, and the results were inter-compared.
This work first introduces and explains the different methods, namely far- and near-lamp measurements, white-stripe scans, horizon scans and sun scans, using data and results for only one (mainly the Max Planck Institute for Chemistry) instrument. In the second part, the far-lamp measurements and the horizon scans are examined for all participating groups. Here, the results for both methods are first inter-compared for the different instruments; secondly, the two methods are compared amongst each other. (…)
We present the inter-comparison of delta slant column densities (SCDs) and vertical profiles of nitrous acid (HONO) derived from measurements of different multi-axis differential optical absorption spectroscopy (MAX-DOAS) instruments and using different inversion algorithms during the Second Cabauw Inter-comparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) in September 2016 at Cabauw, the Netherlands (51.97° N, 4.93° E). The HONO vertical profiles, vertical column densities (VCDs), and near-surface volume mixing ratios are compared between different MAX-DOAS instruments and profile inversion algorithms for the first time. (…)
Tropospheric NO2 and stratospheric NO2 vertical column densities are important TROPOspheric Monitoring Instrument (TROPOMI) data products. In order to validate the TROPOMI NO2 products, KNMI Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instruments have measured NO2 on ship cruises over the Atlantic and the Pacific oceans. The MAX-DOAS instruments have participated in five cruises on board RV Sonne (in 2017 and 2019) and RV Maria S. Merian (in 2018). The MAX-DOAS measurements were acquired over 7 months and spanned about 90° in latitude and 300° in longitude. During the cruises aerosol measurements from Microtops sun photometers were also taken. (…)
South-eastern Australia has been identified by modelling studies as a hotspot of biogenic volatile organic compound (VOC) emissions; however, long-term observational VOC studies are lacking in this region. Here, 2.5 years of multi-axis differential optical absorption spectroscopy (MAX-DOAS) formaldehyde (HCHO) measurements in Australasia are presented, from Broadmeadows, in northern Melbourne, Australia, and from Lauder, a rural site in the South Island of New Zealand. Across the measurement period from December 2016 to November 2019, the mean formaldehyde columns measured by the MAX-DOAS were 2.50±0.61×1015 molec. cm−2 at Lauder and 5.40±1.59×1015 molec. cm−2 at Broadmeadows. In both locations, the seasonal cycle showed a pronounced peak in Austral summer (December–January–February) consistent with temperature-dependent formaldehyde production from biogenic precursor gases. The amplitude of the seasonal cycle was 0.7×1015 molec. cm−2 at Lauder, and it was 2.0×1015 molec. cm−2 at Broadmeadows. The Lauder MAX-DOAS HCHO measurements are compared with 27 months of co-located Fourier transform infrared (FTIR) observations. The seasonal variation of Lauder MAX-DOAS HCHO, smoothed by the FTIR averaging kernels, showed good agreement with the FTIR measurements, with a linear regression slope of 1.03 and an R2 of 0.66 for monthly averaged formaldehyde partial columns (0–4 km). In addition to ground-based observations, a clear way to address the VOC measurement gap in areas such as Australasia is with satellite measurements. (…)
In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97° N, 4.93° E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. (…)
Retrieving the column of an absorbing trace gas from spectral data requires that all absorbers in the corresponding wavelength range are sufficiently well known. This is especially important for the retrieval of weak absorbers, whose absorptions are often in the 10−4 range.
Previous publications on the absorptions of the oxygen dimer O2–O2 (or short: O4) list absorption peaks at 328 and 419 nm, for which no spectrally resolved literature cross sections are available. As these absorptions potentially influence the spectral retrieval of various trace gases, such as HCHO, BrO, OClO and IO, their shape and magnitude need to be quantified.
We assume that the shape of the absorption peaks at 328 and 419 nm can be approximated by their respective neighbouring absorption peaks. Using this approach we obtain estimates for the wavelength of the absorption and its magnitude. Using long-path differential optical absorption spectroscopy (LP-DOAS) observations and multi-axis DOAS (MAX-DOAS) observations, we estimate the peak absorption cross sections of O4 to be (1.96 ± 0.20) × 10−47 cm5 molec−2 and determine the wavelength of its maximum at 328.59 ± 0.15 nm.
For the absorption at 419.13 ± 0.42 nm a peak O4 cross-section value is determined to be (5.0 ± 3.5) × 10−48 cm5 molec−2.
Experience of differential atmospheric absorption spectroscopy (DOAS) shows that a spectral shift between measurement spectra and reference spectra is frequently required in order to achieve optimal fit results, while the straightforward calculation of the optical density proves inferior. The shift is often attributed to temporal instabilities of the instrument but implicitly solved the problem of the tilt effect discussed/explained in this paper.
Spectral positions of Fraunhofer and molecular absorption lines are systematically shifted for different measurement geometries due to an overall slope – or tilt – of the intensity spectrum. The phenomenon has become known as the tilt effect for limb satellite observations, where it is corrected for in a first-order approximation, whereas the remaining community is less aware of its cause and consequences.
It is caused by the measurement process, because atmospheric absorption and convolution in the spectrometer do not commute. Highly resolved spectral structures in the spectrum will first be modified by absorption and scattering processes in the atmosphere before they are recorded with a spectrometer, which convolves them with a specific instrument function. In the DOAS spectral evaluation process, however, the polynomial (or other function used for this purpose) accounting for broadband absorption is applied after the convolution is performed.
In this paper, we derive that changing the order of the two modifications of the spectra leads to different results. Assuming typical geometries for the observations of scattered sunlight and a spectral resolution of 0.6 nm, this effect can be interpreted as a spectral shift of up to 1.5 pm, which is confirmed in the actual analysis of the ground-based measurements of scattered sunlight as well as in numerical radiative transfer simulations. If no spectral shift is allowed by the fitting routine, residual structures of up to 2.5 × 10−3 peak-to-peak are observed. Thus, this effect needs to be considered for DOAS applications aiming at an rms of the residual of 10−3 and below.
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. (…)
In remote sensing applications, such as differential optical absorption spectroscopy (DOAS), atmospheric scattering processes need to be considered. After inelastic scattering on N2 and O2 molecules, the scattered photons occur as additional intensity at a different wavelength, effectively leading to “filling-in” of both solar Fraunhofer lines and absorptions of atmospheric constituents, if the inelastic scattering happens after the absorption.
Measured spectra in passive DOAS applications are typically corrected for rotational Raman scattering (RRS), also called Ring effect, which represents the main contribution to inelastic scattering. Inelastic scattering can also occur in liquid water, and its influence on DOAS measurements has been observed over clear ocean water. In contrast to that, vibrational Raman scattering (VRS) of N2 and O2 has often been thought to be negligible, but it also contributes.
Consequences of VRS are red-shifted Fraunhofer structures in scattered light spectra and filling-in of Fraunhofer lines, additional to RRS. At 393 nm, the spectral shift is 25 and 40 nm for VRS of O2 and N2, respectively. We describe how to calculate VRS correction spectra according to the Ring spectrum. (…)
Active remote sensing measurement studies involving OPEN PATH instruments
Krause, K., Wittrock, F., Richter, A., Schmitt, S., Pöhler, D., Weigelt, A., and Burrows, J. P.: Estimation of ship emission rates at a major shipping lane by long-path DOAS measurements, Atmos. Meas. Tech., 14, 5791–5807, https://doi.org/10.5194/amt-14-5791-2021, 2021.
hips are an important source of SO2 and NOx, which are key parameters of air quality. Monitoring of ship emissions is usually carried out using in situ instruments on land, which depend on favourable wind conditions to transport the emitted substances to the measurement site. Remote sensing techniques such as long-path differential optical absorption spectroscopy (LP-DOAS) measurements can supplement those measurements, especially in unfavourable meteorological conditions. In this study 1 year of LP-DOAS measurements made across the river Elbe close to Hamburg (Germany) have been evaluated.
Peaks (i.e. elevated concentrations) in the NO2 and SO2 time series were assigned to passing ships, and a method to derive emission rates of SO2, NO2 and NOx from those measurements using a Gaussian plume model is presented. A total of 7402 individual ship passages have been monitored, and their respective NOx, SO2 and NO2 emission rates have been derived. The emission rates, coupled with the knowledge of the ship type, ship size and ship speed, have been analysed. Emission rates are compared to emission factors from previous studies and show good agreement. In contrast to emission factors (in grams per kilogram fuel), the derived emission rates (in grams per second) do not need further knowledge about the fuel consumption of the ship. To our knowledge this is the first time emission rates of air pollutants from individual ships have been derived from LP-DOAS measurements. (…)
More press releases and studies on demand.