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Polarization optics, which characterize the orientation of the electromagnetic field through Stokes vectors formalism, have been effectively used in lidar remote sensing to detect particles that differ in shape, such as mineral dust or pollen. In this study, for the first time, we explore the capability of polarization optics to distinguish the light-backscattering patterns of pollen and fungal spores, two complex-shaped particles that vary significantly in surface structure. A unique laboratory polarimeter operating at lidar backscattering at 180.0° was conducted to assess their light depolarization property in laboratory ambient air. If, at the precise lidar backscattering angle of 180.0°, the depolarization ratios of pollen and fungal spores were difficult to differentiate, slight deviations from 180.0° allowed us to reveal separate scattering matrices for pollen and fungal spores. This demonstrates that polarization optics can unambiguously differentiate these particles based on their light-(back)scattering properties. These findings are consistent at both 532 and 1064 nm. This non-invasive, real-time technique is valuable for environmental monitoring, where rapid identification of airborne allergens is essential, as well as in agricultural and health sectors. Polarization-based light scattering thus offers a valuable method for characterizing such atmospheric particles, aiding in managing airborne contaminants.

In this paper, the dependence of the particles' depolarization ratio (PDR) of mineral dust on the complex refractive index and size is for the first time investigated through a laboratory π-polarimeter operating at 180.0∘ backscattering angle and at (355, 532) nm wavelengths for lidar purposes. The dust PDR is indeed an important input parameter in polarization lidar experiments involving mineral dust. Our π-polarimeter provides 16 accurate ( %) values of the dust lidar PDR at 180.0∘ corresponding to four different complex refractive indices, studied at two size distributions (fine, coarse) ranging from 10 nm to more than 10 µm and at (355, 532) nm wavelengths while accounting for the highly irregular shape of mineral dust, which is difficult to model numerically. At 355 nm, the lidar PDR of coarser silica, the main oxide in mineral dust, is equal to (33±1) %, while that of coarser hematite, the main light absorbent in mineral dust, is (10±1) %. This huge difference is here explained by accounting for the high imaginary part of the hematite complex refractive index. In turn, Arizona dust exhibits higher depolarization than Asian dust, due to the higher proportion in hematite in the latter. As a result, when the strong light-absorbent hematite is involved, the dust lidar PDR primarily depends on the particles' complex refractive index, and its variations with size and shape are less pronounced. When hematite is less or not involved, the dust lidar PDR increases with increasing sizes, though the shape dependence may then also play a role. The (355, 532) nm wavelength dependence of the dust lidar PDR then allows discussing on the involved particle sizes, thus highlighting the importance of dual-wavelength (or more) polarization lidar instruments. We believe these laboratory findings will help improve our understanding of the challenging dependence of the dust lidar PDR with complex refractive index and size to help interpret the complexity and the wealth of polarization lidar signals.

Pollen is nowadays recognized as one of the main atmospheric particles affecting public human health as well as the Earth's climate. In this context, an important issue concerns our ability to detect and differentiate among the existing pollen taxa. In this paper, the potential differences that may exist in light scattering by four of the most common pollen taxa, namely ragweed, birch, pine and ash, are analysed in the framework of the scattering matrix formalism at two wavelengths simultaneously (532 and 1064 nm). Interestingly, our laboratory experimental error bars are precise enough to show that these four pollen taxa, when embedded in ambient air, exhibit different spectral and polarimetric light-scattering characteristics, in the form of 10 scattering matrix elements (5 per wavelength), which allow each to be identified separately. To end with, a simpler light-scattering criterion is proposed for classification among the four considered pollen taxa by performing a principal component (PC) analysis, which still accounts for more than 99 % of the observed variance. We thus believe this work may open new insights for future atmospheric pollen detection.

We show that our developed free-running, bidirectional ring Ti:Sa laser cavity meets the requirements for Dual Comb Spectroscopy in the UV range (UV-DCS). Two counter-propagative frequency combs with slightly different repetition rate are generated in such a cavity and we show quantitatively that this repetition rate difference can be explained by the self-steepening effect. Molecular absorption lines of the O2 A-band centered around 760~nm are measured with a 1,5 GHz spectral resolution, demonstrating that the mutual coherence of the two combs allows GHz-resolution DCS measurements. Moreover, we demonstrate that the generated output peak power allows for efficient second harmonic generation (SHG), in the scope of developing laboratory and open-path UV-DCS experiments.

While pollen is expected to impact public human health and the Earth’s climate more and more in the coming decades, lidar remote sensing of pollen has become an important developing research field. To differentiate among the pollen taxa, a polarization lidar is an interesting tool since pollen exhibit non-spherical complex shapes. A key attribute is thus the lidar particle depolarization ratio (PDR) of pollen, which is however difficult to quantify as pollen are large and complex-shaped particles, far beyond the reach of light scattering numerical simulations. In this paper, a laboratory π-polarimeter is used to accurately evaluate the PDR of pure pollen, for the first time at the lidar exact backscattering angle of 180.0°. We hence reveal the lidar PDR of pure ragweed, ash, birch, pine, cypress and spruce pollens at 355 and 532 nm lidar wavelengths, as presented at the ELC 2021 conference. A striking result is the spectral dependence of the lidar PDR, highlighting the importance of dual-wavelength (or more) polarization lidars to identify pollen taxa. These spectral and polarimetric fingerprints of pure pollen, as they are accurate, can be used by the lidar community to invert multi-wavelength lidar polarization measurements involving pollen.

The development of increasingly sensitive and robust instruments and new methodologies are essential to improve our understanding of the Earth’s climate and air pollution. In this context, Dual-Comb spectroscopy (DCS) has been successfully demonstrated as a remote laser-based instrument to probe infrared absorbing species such as greenhouse gases. We present here a study of the sensitivity of Dual-Comb spectroscopy to remotely monitor atmospheric gases focusing on molecules that absorb in the ultraviolet domain, where the most reactive molecules of the atmosphere (OH, HONO, BrO...) have their highest absorption cross-sections. We assess the achievable signal-to-noise ratio (SNR) and the corresponding minimum absorption sensitivity of DCS in the ultraviolet range. We propose a potential light source for remote sensing UV-DCS and discuss the degree of immunity of UV-DCS to atmospheric turbulences. We show that the characteristics of the currently available UV sources are compatible with the unambiguous identification of UV absorbing gases by UV-DCS.

While water and sulfuric acid droplets are the main component of stratospheric aerosols, measurements performed for about 30 years have shown that non-sulfate particles (NSPs) are also present. Such particles, released from the Earth mainly through volcanic eruptions, pollution or biomass burning, or coming from space, present a wide variety of compositions, sizes, and shapes. To better understand the origin of NSPs, we have performed measurements with the Light Optical Aerosol Counter (LOAC) during 151 flights under weather balloons in the 2013–2019 period reaching altitudes up to 35 km. Coupled with previous counting measurements conducted over the 2004–2011 period, the LOAC measurements indicate the presence of stratospheric layers of enhanced concentrations associated with NSPs, with a bimodal vertical repartition ranging between 17 and 30 km altitude. Such enhancements are not correlated with permanent meteor shower events. They may be linked to dynamical and photophoretic effects lifting and sustaining particles coming from the Earth. Besides, large particles, up to several tens of μm, were detected and present decreasing concentrations with increasing altitudes. All these particles can originate from Earth but also from meteoroid disintegrations and from the interplanetary dust cloud and comets.

Observations of new particle formation events in free troposphere are rather seldom and limited in time and space, mainly due to the complexity and the cost of the required on-board instrumentation for airplane field campaigns. In this paper, a calibrated (UV, VIS) polarization elastic lidar (2β + 2δ) is used to remotely sense new particle formation events in the free troposphere in the presence of mineral dust particles. Using very efficient (UV, VIS) light polarization discriminators (1:107) and after robust calibration, the contribution of mineral dust particles to the co-polarized (UV, VIS) lidar channels could be removed, to reveal the backscattering coefficient of the newly nucleated particles after these numerous particles have grown to a size detectable with our lidar. Since our polarization and wavelength cross-talks are fully negligible, the observed variation in the (UV, VIS) particle backscattering time−altitude maps could be related to variations in the particle microphysics. Hence, day and nighttime differences, at low and high dust loadings, were observed in agreement with the observed nucleation process promoted by mineral dust. While light backscattering is more sensitive to small-sized particles at the UV lidar wavelength of 355 nm, such new particle formation events are here for the first time also remotely sensed at the VIS lidar wavelength of 532 nm at which most polarization lidars operate. Moreover, by addressing the (UV, VIS) backscattering Angstrom exponent, we could discuss the particles’ sizes addressed with our (UV, VIS) polarization lidar. As nucleation concerns the lowest modes of the particles’ size distribution, such a methodology may then be applied to reveal the lowest particle sizes that a (UV, VIS) polarization lidar can address, thus improving our understanding of the vertical and temporal extent of nucleation in free troposphere, where measurements are rather seldom.

During transport by advection, atmospheric nonspherical particles, such as volcanic ash, desert dust or sea-salt particles experience several chemical and physical processes, leading to a complex vertical atmospheric layering at remote sites where intrusion episodes occur. In this paper, a new methodology is proposed to analyse this complex vertical layering in the case of a two/three-component particle external mixtures. This methodology relies on an analysis of the spectral and polarization properties of the light backscattered by atmospheric particles. It is based on combining a sensitive and accurate UV-VIS polarization lidar experiment with T-matrix numerical simulations and air mass back trajectories. The Lyon UV-VIS polarization lidar is used to efficiently partition the particle mixture into its nonspherical components, while the T-matrix method is used for simulating the backscattering and depolarization properties of nonspherical volcanic ash, desert dust and sea-salt particles. It is shown that the particle mixtures' depolarization ratio δ p differs from the nonspherical particles' depolarization ratio δns due to the presence of spherical particles in the mixture. Hence, after identifying a tracer for nonspherical particles, particle backscattering coefficients specific to each nonspherical component can be retrieved in a two-component external mixture. For three-component mixtures, the spectral properties of light must in addition be exploited by using a dual-wavelength polarization lidar. Hence, for the first time, in a three-component external mixture, the nonsphericity of each particle is taken into account in a so-called 2β + 2δ formalism. Applications of this new methodology are then demonstrated in two case studies carried out in Lyon, France, related to the mixing of Eyjafjallajökull volcanic ash with sulfate particles (case of a two-component mixture) and to the mixing of dust with sea-salt and water-soluble particles (case of a three-component mixture). This new methodology, which is able to provide separate vertical profiles of backscattering coefficient for mixed atmospheric dust, sea-salt and water-soluble particles, may be useful for accurate radiative forcing assessments.

Monitoring the emission of gases is difficult to achieve in industrial sites and in environments presenting poor infrastructures. Hence, robust methodologies should be developed and coupled to Lidar technology to allow remote sensing of gas emission. OSAS is a new methodology to evaluate gas concentration emission from spectrally integrated differential absorption measurements. Proof of concept of OSAS-Lidar for CH4 emission monitoring is here presented.

The MEthane Remote sensing Lidar missioN (MERLIN) aims at demonstrating the spaceborne active measurement of atmospheric methane, a potent greenhouse gas, based on an Integrated Path Differential Absorption (IPDA) nadir-viewing LIght Detecting and Ranging (Lidar) instrument. MERLIN is a joint French and German space mission, with a launch currently scheduled for the timeframe 2021/22. The German Space Agency (DLR) is responsible for the payload, while the platform (MYRIADE Evolutions product line) is developed by the French Space Agency (CNES). The main scientific objective of MERLIN is the delivery of weighted atmospheric columns of methane dry-air mole fractions for all latitudes throughout the year with systematic errors small enough (

In this contribution, we present recent work on the ability to achieve range-resolved greenhouse gases concentration measurements in the Earth’s atmosphere (CH4, H2O) by combining broadband optical correlation spectroscopy (OCS) with lidar. We show that OCS-Lidar is a robust methodology, allowing trace gases remote sensing with a low dependence on the temperature and pressure-variation absorption cross section. Moreover, we evaluate, as an experimental proof, the water vapor profile in the planetary boundary layer using the 4ν 720 nm absorption band.

In this contribution, we present the results of two recent papers [1,2] published in Optics Express, dedicated to the development of two new lidar methodologies. In [1], while the carbon aerosol (for example, soot particles) is recognized as a major uncertainty on climate and public health, we couple lidar remote sensing with Laser-Induced-Incandescence (LII) to allow retrieving the vertical profile of very low thermal radiation emitted by the carbon aerosol, in agreement with Planck’s law, in an urban atmosphere over several hundred meters altitude. In paper [2], awarded as June 2014 OSA Spotlight, we identify the optical requirements ensuring an elastic lidar to be sensitive to new particles formation events (NPF-events) in the atmosphere, while, in the literature, all the ingredients initiating nucleation are still being unrevealed [3]. Both papers proceed with the same methodology by identifying the optical requirements from numerical simulation (Planck and Kirchhoff’s laws in [1], Mie and T-matrix numerical codes in [2]), then presenting lidar field application case studies. We believe these new lidar methodologies may be useful for climate, geophysical, as well as fundamental purposes.

In this paper, an optical remote sensing method is proposed to retrieve the number concentration of non spherical volcanic ash particles. An UV-polarization sensitive remote sensing experiment is interpreted in the frame of the scattering matrix formalism. It follows that UV-optical scattering and depolarization, when they are used together and in correlation with laboratory measurements on scattering matrix elements, are meaningful to retrieve information on volcanic ash particles such as shape or number concentration.