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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). In the presented study, the retrieved CINDI-2 MAX-DOAS trace gas (NO2, HCHO) and aerosol vertical profiles of 15 participating groups using different inversion algorithms are compared and validated against the colocated supporting observations, with the focus on aerosol optical thicknesses (AOTs), trace gas vertical column densities (VCDs) and trace gas surface concentrations. The algorithms are based on three different techniques: six use the optimal estimation method, two use a parameterized approach and one algorithm relies on simplified radiative transport assumptions and analytical calculations. To assess the agreement among the inversion algorithms independent of inconsistencies in the trace gas slant column density acquisition, participants applied their inversion to a common set of slant columns. Further, important settings like the retrieval grid, profiles of O3, temperature and pressure as well as aerosol optical properties and a priori assumptions (for optimal estimation algorithms) have been prescribed to reduce possible sources of discrepancies. The profiling results were found to be in good qualitative agreement: most participants obtained the same features in the retrieved vertical trace gas and aerosol distributions; however, these are sometimes at different altitudes and of different magnitudes. Under clear-sky conditions, the root-mean-square differences (RMSDs) among the results of individual participants are in the range of 0.01–0.1 for AOTs, (1.5–15) ×1014molec.cm-2 for trace gas (NO2, HCHO) VCDs and (0.3–8)×1010molec.cm-3 for trace gas surface concentrations. These values compare to approximate average optical thicknesses of 0.3, trace gas vertical columns of 90×1014molec.cm-2 and trace gas surface concentrations of 11×1010molec.cm-3 observed over the campaign period. The discrepancies originate from differences in the applied techniques, the exact implementation of the algorithms and the user-defined settings that were not prescribed. For the comparison against supporting observations, the RMSDs increase to a range of 0.02–0.2 against AOTs from the Sun photometer, (11–55)×1014molec.cm-2 against trace gas VCDs from direct-sun DOAS observations and (0.8–9)×1010molec.cm-3 against surface concentrations from the long-path DOAS instrument. This increase in RMSDs is most likely caused by uncertainties in the supporting data, spatiotemporal mismatch among the observations and simplified assumptions particularly on aerosol optical properties made for the MAX-DOAS retrieval. As a side investigation, the comparison was repeated with the participants retrieving profiles from their own differential slant column densities (dSCDs) acquired during the campaign. In this case, the consistency among the participants degrades by about 30 % for AOTs, by 180 % (40 %) for HCHO (NO2) VCDs and by 90 % (20 %) for HCHO (NO2) surface concentrations. In former publications and also during this comparison study, it was found that MAX-DOAS vertically integrated aerosol extinction coefficient profiles systematically underestimate the AOT observed by the Sun photometer. For the first time, it is quantitatively shown that for optimal estimation algorithms this can be largely explained and compensated by considering biases arising from the reduced sensitivity of MAX-DOAS observations to higher altitudes and associated a priori assumptions.

We present two-dimensional scanning Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations of nitrogen dioxide (NO2) and formaldehyde (HCHO) in Munich. Vertical columns and vertical distribution profiles of aerosol extinction coefficient, NO2 and HCHO are retrieved from the 2D MAX-DOAS observations. The measured surface aerosol extinction coefficients and NO2 mixing ratios derived from the retrieved profiles are compared to in situ monitoring data, and the surface NO2 mixing ratios show a good agreement with in situ monitoring data with a Pearson correlation coefficient (R) of 0.91. The aerosol optical depths (AODs) show good agreement as well (R = 0.80) when compared to sun photometer measurements. Tropospheric vertical column densities (VCDs) of NO2 and HCHO derived from the MAX-DOAS measurements are also used to validate Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI) satellite observations. Monthly averaged data show a good correlation; however, satellite observations are on average 30 % lower than the MAX-DOAS measurements. Furthermore, the MAX-DOAS observations are used to investigate the spatiotemporal characteristic of NO2 and HCHO in Munich. Analysis of the relations between aerosol, NO2 and HCHO shows higher aerosol-to-HCHO ratios in winter, which reflects a longer atmospheric lifetime of secondary aerosol and HCHO during winter. The analysis also suggests that secondary aerosol formation is the major source of these aerosols in Munich.

We present a new aerosol extinction profile retrieval algorithm for multi-axis differential optical absorption spectrometer (MAX-DOAS) measurements at high-altitude sites. The algorithm is based on the lookup table method. It is applied to retrieve aerosol extinction profiles from the long-term MAX-DOAS measurements (February 2012 to February 2016) at the Environmental Research Station Schneefernerhaus (UFS), Germany (47.417∘ N, 10.980∘ E), which is located near the summit of Zugspitze at an altitude of 2650 m. The lookup table consists of simulated O4 differential slant column densities (DSCDs) corresponding to numerous possible aerosol extinction profiles. The sensitivities of O4 absorption to several parameters were investigated for the design and parameterization of the lookup table. In the retrieval, simulated O4 DSCDs for each possible profile are derived by interpolating the lookup table to the observation geometries. The cost functions are calculated for each aerosol profile in the lookup table based on the simulated O4 DSCDs, the O4 DSCD observations, and the measurement uncertainties. Valid profiles are selected from all the possible profiles according to the cost function, and the optimal solution is defined as the weighted mean of all the valid profiles. A comprehensive error analysis is performed to better estimate the total uncertainty. Based on the assumption that the lookup table covers all possible profiles under clear-sky conditions, we determined a set of O4 DSCD scaling factors for different elevation angles and wavelengths. The profiles retrieved from synthetic measurement data can reproduce the synthetic profile. The results also show that the retrieval is insensitive to measurement noise, indicating the retrieval is robust and stable. The aerosol optical depths (AODs) retrieved from the long-term measurements were compared to coinciding and co-located sun photometer observations. High correlation coefficients (R) of 0.733 and 0.798 are found for measurements at 360 and 477 nm, respectively. However, especially in summer, the sun photometer AODs are systematically higher than the MAX-DOAS retrievals by a factor of ∼2. The discrepancy might be related to the limited measurement range of the MAX-DOAS and is probably also related to the decreased sensitivity of the MAX-DOAS measurements at higher altitudes. The MAX-DOAS measurements indicate the aerosol extinction decreases with increasing altitude during all seasons, which agrees with the co-located ceilometer measurements. Our results also show maximum AOD and maximum Ångström exponent in summer, which is consistent with observations at an AERONET station located ∼43 km from the UFS.

Recently, polarimetry has been used to enhance classical photometry to infer aerosol optical properties, as polarized radiation contains additional information about the particles. Therefore, we have equipped the Sun–sky automatic radiometer (SSARA) with polarizer filters to measure linearly polarized light at 501.5 nm. We describe an improved radiometric and polarimetric calibration method, which allows us to simultaneously determine the linear polarizers' diattenuation and relative orientation with high accuracy (0.002 and 0.1∘, respectively). Furthermore, we employed a new calibration method for the alt-azimuthal mount capable of correcting the instrument's pointing to within 32 arcmin. So far, this is limited by the accuracy of the Sun tracker. Both these methods are applicable to other Sun and sky radiometers, such as the Cimel CE318-DP instruments used in the AErosol RObotic NETwork (AERONET). During the A-LIFE (Absorbing aerosol layers in a changing climate: aging, LIFEtime and dynamics) field campaign in April 2017, SSARA collected 22 d of data. Here, we present two case studies. The first demonstrates the performance of an aerosol retrieval from SSARA observations under partially cloudy conditions. In the other case, a high aerosol load due to a Saharan dust layer was present during otherwise clear-sky conditions.

The Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE) was devoted to the investigation of Saharan dust properties over the Caribbean. The campaign took place in June–July 2013. A wide set of ground-based and airborne aerosol instrumentation was deployed at the island of Barbados for a comprehensive experiment. Several sun photometers performed measurements during this campaign: two AERONET (Aerosol Robotic Network) Cimel sun photometers and the Sun and Sky Automatic Radiometer (SSARA). The sun photometers were co-located with the ground-based multi-wavelength lidars BERTHA (Backscatter Extinction lidar Ratio Temperature Humidity profiling Apparatus) and POLIS (Portable Lidar System). Aerosol properties derived from direct sun and sky radiance observations are analyzed, and a comparison with the co-located lidar and in situ data is provided. The time series of aerosol optical depth (AOD) allows identifying successive dust events with short periods in between in which the marine background conditions were observed. The moderate aerosol optical depth in the range of 0.3 to 0.6 was found during the dust periods. The sun photometer infrared channel at the 1640 nm wavelength was used in the retrieval to investigate possible improvements to aerosol size retrievals, and it was expected to have a larger sensitivity to coarse particles. The comparison between column (aerosol optical depth) and surface (dust concentration) data demonstrates the connection between the Saharan Air Layer and the boundary layer in the Caribbean region, as is shown by the synchronized detection of the successive dust events in both datasets. However the differences of size distributions derived from sun photometer data and in situ observations reveal the difficulties in carrying out a column closure study.

With the rapidly growing number of automated single-wavelength backscatter lidars (ceilometers), their potential benefit for aerosol remote sensing received considerable scientific attention. When studying the accuracy of retrieved particle backscatter coefficients, it must be considered that most of the ceilometers are influenced by water vapor absorption in the spectral range around 910 nm. In the literature methodologies have been proposed to correct for this effect; however, a validation was not yet performed. In the framework of the ceilometer intercomparison campaign CeiLinEx2015 in Lindenberg, Germany, hosted by the German Weather Service, it was possible to tackle this open issue. Ceilometers from Lufft (CHM15k and CHM15kx, operating at 1064 nm), from Vaisala (CL51 and CL31) and from Campbell Scientific (CS135), all operating at a wavelength of approximately 910 nm, were deployed together with a multi-wavelength research lidar (RALPH) that served as a reference. In this paper the validation of the water vapor correction is performed by comparing ceilometer backscatter signals with measurements of the reference system extrapolated to the water vapor regime. One inherent problem of the validation is the spectral extrapolation of particle optical properties. For this purpose AERONET measurements and inversions of RALPH signals were used. Another issue is that the vertical range where validation is possible is limited to the upper part of the mixing layer due to incomplete overlap and the generally low signal-to-noise ratio and signal artifacts above that layer. Our intercomparisons show that the water vapor correction leads to quite a good agreement between the extrapolated reference signal and the measurements in the case of CL51 ceilometers at one or more wavelengths in the specified range of the laser diode's emission. This ambiguity is due to the similar effective water vapor transmission at several wavelengths. In the case of CL31 and CS135 ceilometers the validation was not always successful. That suggests that error sources beyond the water vapor absorption might be dominant. For future applications we recommend monitoring the emitted wavelength and providing “dark” measurements on a regular basis.

We present an automatic aerosol classification method based solely on the European Aerosol Research Lidar Network (EARLINET) intensive optical parameters with the aim of building a network-wide classification tool that could provide near-real-time aerosol typing information. The presented method depends on a supervised learning technique and makes use of the Mahalanobis distance function that relates each unclassified measurement to a predefined aerosol type. As a first step (training phase), a reference dataset is set up consisting of already classified EARLINET data. Using this dataset, we defined 8 aerosol classes: clean continental, polluted continental, dust, mixed dust, polluted dust, mixed marine, smoke, and volcanic ash. The effect of the number of aerosol classes has been explored, as well as the optimal set of intensive parameters to separate different aerosol types. Furthermore, the algorithm is trained with literature particle linear depolarization ratio values. As a second step (testing phase), we apply the method to an already classified EARLINET dataset and analyze the results of the comparison to this classified dataset. The predictive accuracy of the automatic classification varies between 59 % (minimum) and 90 % (maximum) from 8 to 4 aerosol classes, respectively, when evaluated against pre-classified EARLINET lidar. This indicates the potential use of the automatic classification to all network lidar data. Furthermore, the training of the algorithm with particle linear depolarization values found in the literature further improves the accuracy with values for all the aerosol classes around 80 %. Additionally, the algorithm has proven to be highly versatile as it adapts to changes in the size of the training dataset and the number of aerosol classes and classifying parameters. Finally, the low computational time and demand for resources make the algorithm extremely suitable for the implementation within the single calculus chain (SCC), the EARLINET centralized processing suite.

In this paper, we present a comparison of model simulations of aerosol profiles with measurements of the ceilometer network operated by the German Weather Service (DWD) over 1 year from September 2015 to August 2016. The aerosol forecasts are produced by the Copernicus Atmosphere Monitoring Service (CAMS) using the aerosol module developed within the Global and regional Earth-system Monitoring using Satellite and in-situ data (GEMS) and Monitoring Atmospheric Composition and Climate (MACC) projects and coupled into the European Centre for Medium-Range Weather Forecasts Integrated Forecasting System (ECMWF-IFS). As the model output provides mass mixing ratios of different types of aerosol, whereas the ceilometers do not, it is necessary to determine a common physical quantity for the comparison. We have chosen the attenuated backscatter β∗ for this purpose. The β∗ profiles are calculated from the mass mixing ratios of the model output assuming the inherent aerosol microphysical properties. Comparison of the attenuated backscatter averaged between an altitude of 0.2 km (typical overlap range of ceilometers) and 1 km in general shows similar annual average values. However, the standard deviation of the difference between model and observation is larger than the average in 8 out of 12 sites.To investigate possible reasons for the differences, we have examined the role of the hygroscopic growth of particles and the particle shape. Our results show that using a more recent particle growth model would result in a ∼ 22 % reduction of particle backscatter for sea salt aerosols, corresponding to a 10 % reduction of the total backscatter signal on average. Accounting for nonspherical dust particles in the model would reduce attenuated backscatter of dust particles by ∼ 30 %. As the concentration of dust aerosol is in general very low in Germany, a significant effect on the total backscatter signal is restricted to dust episodes. In summary, consideration of both effects tends to improve the agreement between model and observations but without leading to a perfect consistency.In addition, a strong Saharan dust event was investigated to study the agreement of the spatiotemporal distribution of particles. It was found that the arrival time of the dust layer and its vertical extent very well agree between model and ceilometer measurements for several stations. This underlines the potential of a network of ceilometers to validate the dispersion of aerosol layers.

The spatiotemporal distribution and characterization of aerosol particles are usually determined by remote-sensing and optical in situ measurements. These measurements are indirect with respect to microphysical properties, and thus inversion techniques are required to determine the aerosol microphysics. Scattering theory provides the link between microphysical and optical properties; it is not only needed for such inversions but also for radiative budget calculations and climate modeling. However, optical modeling can be very time-consuming, in particular if nonspherical particles or complex ensembles are involved.In this paper we present the MOPSMAP package (Modeled optical properties of ensembles of aerosol particles), which is computationally fast for optical modeling even in the case of complex aerosols. The package consists of a data set of pre-calculated optical properties of single aerosol particles, a Fortran program to calculate the properties of user-defined aerosol ensembles, and a user-friendly web interface for online calculations. Spheres, spheroids, and a small set of irregular particle shapes are considered over a wide range of sizes and refractive indices. MOPSMAP provides the fundamental optical properties assuming random particle orientation, including the scattering matrix for the selected wavelengths. Moreover, the output includes tables of frequently used properties such as the single-scattering albedo, the asymmetry parameter, or the lidar ratio. To demonstrate the wide range of possible MOPSMAP applications, a selection of examples is presented, e.g., dealing with hygroscopic growth, mixtures of absorbing and non-absorbing particles, the relevance of the size equivalence in the case of nonspherical particles, and the variability in volcanic ash microphysics.The web interface is designed to be intuitive for expert and nonexpert users. To support users a large set of default settings is available, e.g., several wavelength-dependent refractive indices, climatologically representative size distributions, and a parameterization of hygroscopic growth. Calculations are possible for single wavelengths or user-defined sets (e.g., of specific remote-sensing application). For expert users more options for the microphysics are available. Plots for immediate visualization of the results are shown. The complete output can be downloaded for further applications. All input parameters and results are stored in the user's personal folder so that calculations can easily be reproduced. The web interface is provided at https://mopsmap.net (last access: 9 July 2018) and the Fortran program including the data set is freely available for offline calculations, e.g., when large numbers of different runs for sensitivity studies are to be made.

The Berlin Air quality and Ecosystem Research: Local and long-range Impact of anthropogenic and Natural hydrocarbons (BAERLIN2014) campaign was conducted during the 3 summer months (June–August) of 2014. During this measurement campaign, both stationary and mobile measurements were undertaken to address complementary aims. This paper provides an overview of the stationary measurements and results that were focused on characterization of gaseous and particulate pollution, including source attribution, in the Berlin–Potsdam area, and quantification of the role of natural sources in determining levels of ozone and related gaseous pollutants. Results show that biogenic contributions to ozone and particulate matter are substantial. One indicator for ozone formation, the OH reactivity, showed a 31 % (0.82 ± 0.44 s−1) and 75 % (3.7 ± 0.90 s−1) contribution from biogenic non-methane volatile organic compounds (NMVOCs) for urban background (2.6 ± 0.68 s−1) and urban park (4.9 ± 1.0 s−1) location, respectively, emphasizing the importance of such locations as sources of biogenic NMVOCs in urban areas. A comparison to NMVOC measurements made in Berlin approximately 20 years earlier generally show lower levels today for anthropogenic NMVOCs. A substantial contribution of secondary organic and inorganic aerosol to PM10 concentrations was quantified. In addition to secondary aerosols, source apportionment analysis of the organic carbon fraction identified the contribution of biogenic (plant-based) particulate matter, as well as primary contributions from vehicles, with a larger contribution from diesel compared to gasoline vehicles, as well as a relatively small contribution from wood burning, linked to measured levoglucosan.

The mixing layer height (MLH) is a measure for the vertical turbulent exchange within the boundary layer, which is one of the controlling factors for the dilution of pollutants emitted near the ground. Based on continuous MLH measurements with a Vaisala CL51 ceilometer and measurements from an air quality network, the relationship between MLH and near-surface pollutant concentrations has been investigated. In this context the uncertainty of the MLH retrievals and the representativeness of ground-based in situ measurements are crucial. We have investigated this topic by using data from the BAERLIN2014 campaign in Berlin, Germany, conducted from June to August 2014. To derive the MLH, three versions of the proprietary software BL-VIEW and a novel approach COBOLT were compared. It was found that the overall agreement is reasonable if mean diurnal cycles are considered. The main advantage of COBOLT is the continuous detection of the MLH with a temporal resolution of 10 min and a lower number of cases when the residual layer is misinterpreted as mixing layer. We have calculated correlations between MLH as derived from the different retrievals and concentrations of pollutants (PM10, O3 and NOx) for different locations in the metropolitan area of Berlin. It was found that the correlations with PM10 are quite different for different sites without showing a clear pattern, whereas the correlation with NOx seems to depend on the vicinity of emission sources in main roads. In the case of ozone as a secondary pollutant, a clear correlation was found. We conclude that the effects of the heterogeneity of the emission sources, chemical processing and mixing during transport exceed the differences due to different MLH retrievals. Moreover, it seems to be unrealistic to find correlations between MLH and near-surface pollutant concentrations representative for a city like Berlin (flat terrain), in particular when traffic emissions are dominant. Nevertheless it is worthwhile to use advanced MLH retrievals for ceilometer data, for example as input to dispersion models and for the validation of chemical transport models.

Halo displays in the sky contain valuable information about ice crystal shape and orientation: e.g., the 22° halo is produced by randomly oriented hexagonal prisms while parhelia (sundogs) indicate oriented plates. HaloCam, a novel sun-tracking camera system for the automated observation of halo displays is presented. An initial visual evaluation of the frequency of halo displays for the ACCEPT (Analysis of the Composition of Clouds with Extended Polarization Techniques) field campaign from October to mid-November 2014 showed that sundogs were observed more often than 22° halos. Thus, the majority of halo displays was produced by oriented ice crystals. During the campaign about 27 % of the cirrus clouds produced 22° halos, sundogs or upper tangent arcs. To evaluate the HaloCam observations collected from regular measurements in Munich between January 2014 and June 2016, an automated detection algorithm for 22° halos was developed, which can be extended to other halo types as well. This algorithm detected 22° halos about 2 % of the time for this dataset. The frequency of cirrus clouds during this time period was estimated by co-located ceilometer measurements using temperature thresholds of the cloud base. About 25 % of the detected cirrus clouds occurred together with a 22° halo, which implies that these clouds contained a certain fraction of smooth, hexagonal ice crystals. HaloCam observations complemented by radiative transfer simulations and measurements of aerosol and cirrus cloud optical thickness (AOT and COT) provide a possibility to retrieve more detailed information about ice crystal roughness. This paper demonstrates the feasibility of a completely automated method to collect and evaluate a long-term database of halo observations and shows the potential to characterize ice crystal properties.

In recent years attention was increasingly paid to backscatter profiles of ceilometers as a new source of aerosol information. Several case studies have shown that – although originally intended for cloud detection only – ceilometers can provide the planetary boundary layer height and even quantitative information such as the aerosol backscatter coefficient βp, provided that the signals have been calibrated. It is expected that the retrieval of aerosol parameters will become widespread as the number of ceilometers is steadily increasing, and continuous and unattended operation is provided. In this context however one should be aware of the fact that the majority of ceilometers provides signals that are influenced by atmospheric water vapor. As a consequence, profiles of aerosol parameters can only be retrieved if water vapor absorption is taken into account. In this paper we describe the influence of water vapor absorption on ceilometer signals at wavelengths around λ = 910 nm. Spectrally high-resolved absorption coefficients are calculated from HITRAN on the basis of realistic emission spectra of ceilometers. These results are used as a reference to develop a methodology ("WAPL") for routine and near-real time corrections of the water vapor influence. Comparison of WAPL with the reference demonstrates its very high accuracy. Extensive studies with simulations based on measurements reveal that the error when water vapor absorption is ignored in the βp-retrieval can be in the order of 20 % for mid-latitudes and more than 50 % for the tropics. It is concluded that the emission spectrum of the laser source should be provided by the manufacturer to increase the accuracy of WAPL, and that 910 nm is better suited than 905 nm. With WAPL systematic errors can be avoided, that would exceed the inherent errors of the Klett solutions by far.

The European Aerosol Research Lidar Network, EARLINET, was founded in 2000 as a research project for establishing a quantitative, comprehensive, and statistically significant database for the horizontal, vertical, and temporal distribution of aerosols on a continental scale. Since then EARLINET has continued to provide the most extensive collection of ground-based data for the aerosol vertical distribution over Europe. This paper gives an overview of the network's main developments since 2000 and introduces the dedicated EARLINET special issue, which reports on the present innovative and comprehensive technical solutions and scientific results related to the use of advanced lidar remote sensing techniques for the study of aerosol properties as developed within the network in the last 13 years. Since 2000, EARLINET has developed greatly in terms of number of stations and spatial distribution: from 17 stations in 10 countries in 2000 to 27 stations in 16 countries in 2013. EARLINET has developed greatly also in terms of technological advances with the spread of advanced multiwavelength Raman lidar stations in Europe. The developments for the quality assurance strategy, the optimization of instruments and data processing, and the dissemination of data have contributed to a significant improvement of the network towards a more sustainable observing system, with an increase in the observing capability and a reduction of operational costs. Consequently, EARLINET data have already been extensively used for many climatological studies, long-range transport events, Saharan dust outbreaks, plumes from volcanic eruptions, and for model evaluation and satellite data validation and integration. Future plans are aimed at continuous measurements and near-real-time data delivery in close cooperation with other ground-based networks, such as in the ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) www.actris.net, and with the modeling and satellite community, linking the research community with the operational world, with the aim of establishing of the atmospheric part of the European component of the integrated global observing system.

With the establishment of ceilometer networks by national weather services, a discussion commenced to which extent these simple backscatter lidars can be used for aerosol research. Though primarily designed for the detection of clouds it was shown that at least observations of the vertical structure of the boundary layer might be possible. However, an assessment of the potential of ceilometers for the quantitative retrieval of aerosol properties is still missing. In this paper we discuss different retrieval methods to derive the aerosol backscatter coefficient βp, with special focus on the calibration of the ceilometers. Different options based on forward and backward integration methods are compared with respect to their accuracy and applicability. It is shown that advanced lidar systems such as those being operated in the framework of the European Aerosol Research Lidar Network (EARLINET) are excellent tools for the calibration, and thus βp retrievals based on forward integration can readily be implemented and used for real-time applications. Furthermore, we discuss uncertainties introduced by incomplete overlap, the unknown lidar ratio, and water vapor absorption. The latter is relevant for the very large number of ceilometers operating in the spectral range around λ = 905–910 nm. The accuracy of the retrieved βp mainly depends on the accuracy of the calibration and the long-term stability of the ceilometer. Under favorable conditions, a relative error of βp on the order of 10% seems feasible. In the case of water vapor absorption, corrections assuming a realistic water vapor distribution and laser spectrum are indispensable; otherwise errors on the order of 20% could occur. From case studies it is shown that ceilometers can be used for the reliable detection of elevated aerosol layers below 5 km, and can contribute to the validation of chemistry transport models, e.g., the height of the boundary layer. However, the exploitation of ceilometer measurements is still in its infancy, so more studies are urgently needed to consolidate the present state of knowledge, which is based on a limited number of case studies.

The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.

Since a few years, the number of active remote sensing systems has been rapidly increasing as national weather services started to build up networks of ceilometers. As ceilometers can be considered as "simple" backscatter lidars, it is obvious to investigate to which extent they can provide quantitative aerosol information. In this context, the calibration of the ceilometer is the most crucial point: whereas previous studies primarily have relied on the comparisons with co-incident sun photometer measurements and the Rayleigh calibration, we provide an absolute calibration of the ceilometer. The advantage of this approach is that backscatter profiles can be derived during daytime and nighttime, and even in cases when the signal-to-noise ratio of signals from the free troposphere is very low. Moreover, the retrieval can easily be automated. In this paper, we consider the Jenoptik CHM15kx-ceilometer. We discuss the methodology and the achievable accuracy and present a set of examples to highlight the wide range of applications, and the limitations. The achievable temporal resolution is of the order of a few minutes; the relative error of the particle backscatter coefficient is less than 10%. It is emphasized that the accuracy of extinction coefficients and – as a consequence – of the aerosol optical depth is limited due to the unknown lidar ratio. This is, however, an inherent problem of any backscatter lidar and not a special feature of the ceilometer.

The spatial structure and the progression speed of the first ash layer from the Icelandic Eyjafjallajökull volcano which reached Germany on 16/17 April is investigated from remote sensing data and numerical simulations. The ceilometer network of the German Meteorological Service was able to follow the progression of the ash layer over the whole of Germany. This first ash layer turned out to be a rather shallow layer of only several hundreds of metres thickness which was oriented slantwise in the middle troposphere and which was brought downward by large-scale sinking motion over Southern Germany and the Alps. Special Raman lidar measurements, trajectory analyses and in-situ observations from mountain observatories helped to confirm the volcanic origin of the detected aerosol layer. Ultralight aircraft measurements permitted the detection of the arrival of a second major flush of volcanic material in Southern Germany. Numerical simulations with the Eulerian meso-scale model MCCM were able to reproduce the temporal and spatial structure of the ash layer. Comparisons of the model results with the ceilometer network data on 17 April and with the ultralight aircraft data on 19 April were satisfying. This is the first example of a model validation study from this ceilometer network data.

Airborne lidar and in-situ measurements of aerosols and trace gases were performed in volcanic ash plumes over Europe between Southern Germany and Iceland with the Falcon aircraft during the eruption period of the Eyjafjalla volcano between 19 April and 18 May 2010. Flight planning and measurement analyses were supported by a refined Meteosat ash product and trajectory model analysis. The volcanic ash plume was observed with lidar directly over the volcano and up to a distance of 2700 km downwind, and up to 120 h plume ages. Aged ash layers were between a few 100 m to 3 km deep, occurred between 1 and 7 km altitude, and were typically 100 to 300 km wide. Particles collected by impactors had diameters up to 20 μm diameter, with size and age dependent composition. Ash mass concentrations were derived from optical particle spectrometers for a particle density of 2.6 g cm−3 and various values of the refractive index (RI, real part: 1.59; 3 values for the imaginary part: 0, 0.004 and 0.008). The mass concentrations, effective diameters and related optical properties were compared with ground-based lidar observations. Theoretical considerations of particle sedimentation constrain the particle diameters to those obtained for the lower RI values. The ash mass concentration results have an uncertainty of a factor of two. The maximum ash mass concentration encountered during the 17 flights with 34 ash plume penetrations was below 1 mg m−3. The Falcon flew in ash clouds up to about 0.8 mg m−3 for a few minutes and in an ash cloud with approximately 0.2 mg m−3 mean-concentration for about one hour without engine damage. The ash plumes were rather dry and correlated with considerable CO and SO2 increases and O3 decreases. To first order, ash concentration and SO2 mixing ratio in the plumes decreased by a factor of two within less than a day. In fresh plumes, the SO2 and CO concentration increases were correlated with the ash mass concentration. The ash plumes were often visible slantwise as faint dark layers, even for concentrations below 0.1 mg m−3. The large abundance of volatile Aitken mode particles suggests previous nucleation of sulfuric acid droplets. The effective diameters range between 0.2 and 3 μm with considerable surface and volume contributions from the Aitken and coarse mode aerosol, respectively. The distal ash mass flux on 2 May was of the order of 500 (240–1600) kg s−1. The volcano induced about 10 (2.5–50) Tg of distal ash mass and about 3 (0.6–23) Tg of SO2 during the whole eruption period. The results of the Falcon flights were used to support the responsible agencies in their decisions concerning air traffic in the presence of volcanic ash.

Volcanic ash plumes, emitted by the Eyjafjallajökull volcano (Iceland) in spring 2010, were observed by the lidar systems MULIS and POLIS in Maisach (near Munich, Germany), and by a CIMEL Sun photometer and a JenOptik ceilometer in Munich. We retrieve mass concentrations of volcanic ash from the lidar measurements; spectral optical properties, i.e. extinction coefficients, backscatter coefficients, and linear depolarization ratios, are used as input for an inversion. The inversion algorithm searches for model aerosol ensembles with optical properties that agree with the measured values within their uncertainty ranges. The non-sphericity of ash particles is considered by assuming spheroids. Optical particle properties are calculated using the T-matrix method supplemented by the geometric optics approach. The lidar inversion is applied to observations of the pure volcanic ash plume in the morning of 17 April 2010. We find 1.45 g m−2 for the ratio between the mass concentration and the extinction coefficient at λ = 532 nm, assuming an ash density of 2.6 g cm−3. The uncertainty range for this ratio is from 0.87 g m−2 to 2.32 g m−2. At the peak of the ash concentration over Maisach the extinction coefficient at λ = 532 nm was 0.75 km−1 (1-h-average), which corresponds to a maximum mass concentration of 1.1 mg m−3 (0.65 to 1.8 mg m−3). Model calculations show that particle backscatter at our lidar wavelengths (λ ≤ 1064 nm), and thus the lidar retrieval, is hardly sensitive to large particles (r ≳ 3 μm); large particles, however, may contain significant amounts of mass. Therefore, as an independent cross check of the lidar retrieval and to investigate the presence of large particles in more detail, we model ratios of sky radiances in the aureole of the Sun and compare them to measurements of the CIMEL. These ratios are sensitive to particles up to r ≈ 10 μm. This approach confirms the mass concentrations from the lidar retrieval. We conclude that synergistic utilization of high quality lidar and Sun photometer data, in combination with realistic aerosol models, is recommended for improving ash mass concentration retrievals.

In this paper, we present long term observations of atmospheric aerosols and nitrogen dioxide (NO 2 ) in Hong Kong using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument. Ground based MAX-DOAS measurements were performed over 5years from December 2010 to November 2015. Vertical distribution profiles of aerosols and NO 2 were derived from MAX-DOAS O 4 and NO 2 observations by applying the optimal estimation method. Retrieved MAX-DOAS measurements of aerosols and NO 2 show good agreement with sun photometer observation of aerosol optical depths (AODs) and long path DOAS measurement of ground level NO 2 mixing ratios. Tropospheric vertical column densities (VCDs) of NO 2 derived from MAX-DOAS measurements are used to validate OMI satellite NO 2 observations. Daily data show reasonably good agreement with each other with Pearson correlation coefficient R=0.7. However, MAX-DOAS NO 2 VCDs are on average higher than OMI observations by a factor of 2. Introducing aerosols in the air mass factor calculation would enhance the OMI VCDs by 7-13%, the remaining discrepancy is mainly due to the differences in spatial coverage between the two instruments. Diurnal variation patterns of aerosols and NO 2 indicated significant contributions from local anthropogenic emissions. Analysis of air mass transport shows that the enhancement of surface aerosols and NO 2 concentrations mainly results from accumulation of local emissions under low wind speed conditions., (Copyright © 2017 Elsevier B.V. All rights reserved.)

An intercomparison of aerosol backscatter lidar algorithms was performed in 2001 within the framework of the European Aerosol Research Lidar Network to Establish an Aerosol Climatology (EARLINET). The objective of this research was to test the correctness of the algorithms and the influence of the lidar ratio used by the various lidar teams involved in the EARLINET for calculation of backscatter-coefficient profiles from the lidar signals. The exercise consisted of processing synthetic lidar signals of various degrees of difficulty. One of these profiles contained height-dependent lidar ratios to test the vertical influence of those profiles on the various retrieval algorithms. Furthermore, a realistic incomplete overlap of laser beam and receiver field of view was introduced to remind the teams to take great care in the nearest range to the lidar. The intercomparison was performed in three stages with increasing knowledge on the input parameters. First, only the lidar signals were distributed; this is the most realistic stage. Afterward the lidar ratio profiles and the reference values at calibration height were provided. The unknown height-dependent lidar ratio had the largest influence on the retrieval, whereas the unknown reference value was of minor importance. These results show the necessity of making additional independent measurements, which can provide us with a suitable approximation of the lidar ratio. The final stage proves in general, that the data evaluation schemes of the different groups of lidar systems work well.

The influence of multiple scattering on the retrieval of extinction coefficients of tropospheric aerosols from ground-based backscatter lidar measurements is numerically modeled. In a first step, lidar returns are computed by means of a Monte Carlo code for model atmospheres with different aerosol types and different extinction coefficient profiles. In so doing, synthetic lidar signals with and without multiple scattering can be simulated. In a second step, both types of signal are inverted by the most frequently used analytical solution, which, however, is based on the single-scatter assumption. From a comparison of the results, the error of the retrieved aerosol-extinction profiles can be quantitatively determined. It was found that the contribution of multiply scattered photons to the lidar signals is typically below 10% and never exceeds 20%. The relative errors of the retrieved aerosol-extinction profile in the planetary boundary layer are still smaller; they were determined to be less than 3% for all aerosol types, even for extinction coefficients as large as 3.9 km(-1). Thus, for ground-based lidar measurements and typical meteorological conditions, errors caused by neglecting multiple scattering are by far less significant than other errors in lidar data evaluation.

The data library of optical properties of hexagonal ice crystals for radiative modeling, Cirrus Optical Properties (COP), is introduced. It includes phase functions, asymmetry parameters, extinction cross sections, and single scattering albedos. Furthermore, lidar ratios and depolarization are given. The dependence of these parameters on wavelength, particle size, and shape is calculated, and different particle orientations are considered. In addition, a simple FORTRAN code is provided to calculate the corresponding properties of size distributions. Thus the data library is a very flexible tool for determining the optical parameters of ice clouds for climatological purposes and remote sensing. The data library and the FORTRAN code are distributed through electronic mail.

It is generally accepted that multiple scattering is important for evaluating backscatter lidar signals in the case of moderate or high optical depths and large receiver fields of view. On one hand, multiple scattering must be considered in inverting signals to obtain backscatter coefficients; on the other hand, it offers the opportunity to derive microphysical parameters of the scattering medium. Bissonnette developed a numerical code for the propagation of a continuous-wave laser beam through an atmosphere including multiple scattering. His model is also applicable to a backscatter lidar approximatively.

In this paper we investigate if the assumptions on which his backscatter lidar application is based are valid for typical atmospheric situations. It is found that for small and moderate optical depths, a prerequisite for the backscatter lidar application is fulfilled: second-order iterations of the solution to the radiative transfer equation can indeed be neglected as proposed by Bissonnette.

Furthermore, we propose an improvement of the simulation for limited fields of view that significantly alters the radial dependences of the backscattered signals. Essentially, on-axis backscattered signals are increased and the profiles tend to be somewhat narrower near the optical axis. The dependence of the radiative distribution on the phase function of the scattering medium, the optical depth, and on the field of view of the receiver is also changed. The modifications only slightly increase the computer time. Examples for typical atmospheric situations are shown, and proposals for intercomparisons with other models and measurements are made.