To study the feasibility of a fluorescence lidar for aerosol characterization, the fluorescence channel is added to the LILAS multiwavelength Mie–Raman lidar of Lille University, France. A part of the fluorescence spectrum induced by 355 nm laser radiation is selected by the interference filter of 44 nm bandwidth centered at 466 nm. Such an approach has proved to have high sensitivity, allowing fluorescence signals from weak aerosol layers to be detected and the fluorescence backscattering coefficient from the ratio of fluorescence and nitrogen Raman backscatters to be calculated. Observations were performed during the November 2019–February 2020 period. The fluorescence capacity (ratio of fluorescence to elastic backscattering coefficients), measured under conditions of low relative humidity, varied in a wide range, being the highest for the smoke and the lowest for the dust particles. The results presented also demonstrate that the fluorescence measurements can be used for monitoring the aerosol inside the cloud layers.

The paper presents an approach to revealing the variability in aerosol type, at high spatiotemporal resolution, by combining fluorescence and Mie–Raman lidar observations. The multiwavelength Mie–Raman lidar system in operation at the ATOLL (ATmospheric Observation at liLLe) platform, Laboratoire d'Optique Atmosphérique, University of Lille, has included, since 2019, a wideband fluorescence channel allowing the derivation of the fluorescence backscattering coefficient β_F. The fluorescence capacity G_F, which is the ratio of β_F to the aerosol backscattering coefficient, is an intensive particle property, strongly changing with aerosol type, thus providing a relevant basis for aerosol classification. In this first stage of research, only two intensive properties are used for classification, namely the particle depolarization ratio at 532 nm, δ₅₃₂, and the fluorescence capacity, G_F. These properties are considered because they can be derived at high spatiotemporal resolution and are quite specific to each aerosol type. In particular, in this study, we use a δ₅₃₂–G_F diagram to identify smoke, dust, pollen, and urban aerosol particles. We applied our new classification approach to lidar data obtained during the 2020–2021 period, which includes strong smoke, dust, and pollen episodes. The particle classification was performed with a height resolution of about 60 m and temporal resolution better than 8 min.

The multiwavelength Mie–Raman–fluorescence lidar of the University of Lille has the capability to measure three aerosol backscattering coefficients, two extinction coefficients and three linear depolarization ratios, together with fluorescence backscattering at 466 nm. It was used to characterize aerosols during the pollen season in the north of France for the period March–June 2020. The results of observations demonstrate that the presence of pollen grains in aerosol mixture leads to an increase in the depolarization ratio. Moreover, the depolarization ratio exhibits a strong spectral dependence increasing with wavelength, which is expected for the mixture containing fine background aerosols with low depolarization and strongly depolarizing pollen grains. A high depolarization ratio correlates with the enhancement of the fluorescence backscattering, corroborating the presence of pollen grains. Obtained results demonstrate that simultaneous measurements of particle depolarization and fluorescence allows for the separation of dust, smoke particles and aerosol mixtures containing the pollen grains.

A shipborne Sun–sky–lunar photometer of type CE318-T was tested during two trans-Atlantic cruises aboard the German research vessel Polarstern from 54^∘ N to 54^∘ S in May/June and December 2018. The continuous observations of the motion-stabilized shipborne CE318-T enabled the first-time observation of a full diurnal cycle of aerosol optical depth (AOD) and column-mean Ångström coefficient of a mixed dust–smoke episode. The latitudinal distribution of the AOD from the shipborne CE318-T, Raman lidar and MICROTOPS II shows the same trend with highest values in the dust belt from 0 to 20^∘ N and overall low values in the Southern Hemisphere. The linear-regression coefficients of determination between MICROTOPS II and the CE318-T were 0.988, 0.987, 0.994 and 0.994 for AODs at 380, 440, 500 and 870 nm and 0.896 for the Ångström exponent at 440–870 nm. The root-mean-squared differences of AOD at 380, 440, 500 and 870 nm were 0.015, 0.013, 0.010 and 0.009, respectively.

A five-channel fluorescence lidar was developed for the study of atmospheric aerosol. The fluorescence spectrum induced by 355 nm laser emission is analyzed in five spectral intervals using interference filters. Central wavelengths and the widths of these five interference filters are, respectively, as follows: 438 and 29, 472 and 32, 513 and 29, 560 and 40, and 614 and 54 nm. The relative calibration of these channels has been performed using a tungsten–halogen lamp with a color temperature of 2800 K. This new lidar system was operated during summer–autumn 2022, when strong forest fires occurred in the Moscow region and generated a series of smoke plumes analyzed in this study. Our results demonstrate that, for urban aerosol, the maximal fluorescence backscattering is observed in a 472 nm channel. For the smoke, the maximum is shifted toward longer wavelengths, and the fluorescence backscattering coefficients in 472, 513 and 560 nm channels have comparable values. Thus, from the analysis of the ratios of fluorescence backscattering in available channels, we show that it is possible to identify smoke layers. The particle classification based on single-channel fluorescence capacity (ratio of the fluorescence backscattering to the elastic one) has limitations at high relative humidity (RH). The fluorescence capacity indeed decreases when water uptake of particles enhances the elastic scattering. However, the spectral variation of fluorescence backscattering does not exhibit any dependence on RH and can be therefore applied to aerosol identification.

Aerosols are essential climate variables that need to be observed at a global scale to monitor the evolution of the atmospheric composition and potential climate impacts. We used the measurements performed over the May 2007–December 2019 period by a ground-based sun photometer installed at the island of La Réunion (21°S, 55°E), together with a linear regression fitting model, to assess the climatology and types of aerosols reaching this observation site located in a sparsely documented pristine area, and the forcings responsible for the variability of the observed aerosol optical depth (AOD) and related trend. The climatology of the aerosol optical depth (AOD) at 440 nm (AOD₄₄₀) and Ångström exponent between 500 and 870 nm (α) revealed that sea salts could be considered as the La Réunion AOD₄₄₀ and α baselines (0.06 ± 0.03 and 0.61 ± 0.40, respectively, from December to August), which were mainly modulated by biomass burning (BB) plumes passing over La Réunion (causing a doubling of AOD₄₄₀ and α up to 0.13 ± 0.07 and 1.06 ± 0.34, respectively, in October). This was confirmed by the retrieved aerosol volume size distributions showing that the coarse-mode (fine-mode) dominated the total volume concentration for AOD₄₄₀ lower (higher) than 0.2 with a mean radius equal to 3 μm (0.15 μm). The main contribution to the AOD₄₄₀ variability over La Réunion was evaluated to be the BB activity (67.4 ± 28.1%), followed by marine aerosols (16.3 ± 4.2%) and large-scale atmospheric structures (5.5 ± 1.7%). The calculated trend for AOD₄₄₀ equaled 0.02 ± 0.01 per decade (2.6 ± 1.3% per year). These results provide a scientific reference base for upcoming studies dedicated to the quantification of the impact of wildfire emissions on the southwestern Indian Ocean’s atmospheric composition and radiative balance.