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We present direct measurements of biogenic volatile organic compound (BVOC)-induced nitrate radical (NO3) reactivity (kVOC) through the diel cycle in the suburban, temperate forest of Rambouillet near Paris (France). The data were obtained in a 6-week summer period in 2022 as part of the Atmospheric ChemistRy Of the Suburban foreSt (ACROSS) campaign. kVOC was measured in a small (700 m2) clearing mainly at a height of 5.5 m above ground level but also at 40 m (for 5 d and nights). At nighttime, mean values (and 25th–75th percentile ranges) of knightVOC(5.5m) = (0.24-0.06+0.32) s-1 and knightVOC(40m) = (0.016-0.007+0.018) s-1 indicate a significant vertical gradient and low NO3 reactivity above the canopy, whereas knightVOC (5.5 m) showed peak values of up to 2 s-1 close to the ground. The strong vertical gradient in NO3 reactivity could be confirmed by measurements between 0 and 24 m on one particular night characterized by a strong temperature inversion and is a result of the decoupling of air masses aloft from the ground- and canopy-level sources of BVOCs (and nitric oxide, NO). No strong vertical gradient was observed in the mean daytime NO3 reactivity, with kdayVOC(5.5m) = (0.12±0.04) s-1 for the entire campaign and kdayVOC(40m) = (0.07±0.02) s-1 during the 5 d period. Within the clearing, the fractional contribution of VOCs to the total NO3 loss rate coefficient (ktot , determined by photolysis, reaction with NO and VOCs) was 80 %–90 % during the night and ∼ 50 % during the day. In terms of chemical losses of α -pinene below canopy height in the clearing, we find that at nighttime hydroxyl radicals (OH) and ozone (O3) dominate, with NO3 contributing "only" 17 %, which decreases further to 8.5 % during the day. Based on measured OH, measured O3 , and calculated NO3 concentrations, the chemical lifetime of BVOCs at noon is about 1 h and is likely to be longer than timescales of transport out of the canopy (typically of the order of minutes), thus significantly reducing the importance of daytime in-canopy processing. Clearly, in forested regions where sufficient nitric oxide and nitrogen dioxide (NOx) is available, the role of NO3 and OH as initiators of BVOC oxidation is not strictly limited to nighttime and daytime, respectively, as often implied in e.g. atmospheric chemistry textbooks. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate forcers with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a 2-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi (PDM) located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded Aethalometer AE33, a thermal-optical analyser Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations in the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy were explained by the mass absorption cross section (MAC) that was too low and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentrations were below 25 µgCcm-2 , which is probably linked to the incorrect determination of the organic carbon (OC)–EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow for the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution is needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

We present direct measurements of BVOC-induced nitrate radical (NO3) reactivity (kVOC) through the diel cycle in the suburban, temperate forest of Rambouillet near Paris (France). The data were obtained in a six-week summer period in 2022 as part of the ACROSS campaign (Atmospheric ChemistRy Of the Suburban foreSt). kVOC was measured in a small (700 m²) clearing mainly at a height of 5.5 m above ground level, but also at 40 m (for 5 days/nights). At nighttime, mean values of kVOCnight (5.5 m) = (0.24 ± 0.27) s-1 and kVOCnight (40 m) = (0.016 ± 0.007) s-1 indicate a significant vertical gradient and low NO3 reactivity above the canopy, whereas kVOCnight (5.5 m) showed peak values of up to 2 s-1 close to the ground. The strong vertical gradient in NO3 reactivity could be confirmed by measurements between 0 and 24 m on one particular night characterised by a strong temperature inversion, and is a result of the decoupling of air masses aloft from the ground- and canopy-level sources of BVOCs (and NO). No strong vertical gradient was observed in the mean daytime NO3 reactivity with kVOCnight(5.5 m) = (0.12 ± 0.04) s-1 for the entire campaign and kVOCnight(40 m) = (0.07 ± 0.02) s-1 during the 5-day period. Within the clearing, the fractional contribution of VOCs to the total NO3 loss rate (LNO3, determined by photolysis, reaction with NO and VOCs) was 80-90 % during the night and ~50 % during the day. In terms of chemical losses of α-pinene below canopy height in the clearing, we find that at nighttime OH and O3 dominate with NO3 contributing "only" 17 %, which decreases further to 8.5 % during the day. Based on OH, O3 and NO3 concentrations, the chemical lifetime of BVOCs at noon is about one hour and is likely to be longer than timescales of transport out of the canopy (typically in the order of minutes), thus significantly reducing the importance of daytime, in-canopy processing. Clearly, in forested regions where sufficient NOX is available, the role of NO3 and OH as initiators of BVOC oxidation are not strictly limited to the night and to the day, respectively, as often implied in e.g. atmospheric chemistry text-books. [ABSTRACT FROM AUTHOR]

Black-carbon-containing particles strongly absorb light, causing substantial radiative heating of the atmosphere. The climate-relevant properties of black carbon (BC) are poorly constrained in high-altitude mountain regions, where many complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents 2-year measurements of BC microphysical and optical properties at the Pic du Midi (PDM) research station, a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the long-term monitoring sites in the world, PDM is subject to limited influence from the planetary boundary layer (PBL), making it a suitable site for characterizing the BC in the free troposphere (FT). The classification of the dominant aerosol type using aerosol spectral optical properties indicates that BC is the predominant aerosol absorption component at PDM and controls the variation in single-scattering albedo (SSA) throughout the 2 years. Single-particle soot photometer (SP2) measurements of refractory BC (rBC) show a mean mass concentration (MrBC) of 35 ngm-3 and a relatively constant rBC core mass-equivalent diameter of about 180 nm, which are typical values for remote mountain sites. Combining the MrBC with in situ absorption measurements, a rBC mass absorption cross-section (MAC rBC) of 9.2 ± 3.7 m2g-1 at λ=880 nm has been obtained, which corresponds to an absorption enhancement (Eabs) of ∼2.2 compared to that of bare rBC particles with equal rBC core size distribution. A significant reduction in the ΔMrBC/ΔCO ratio when precipitation occurred along the air mass transport suggests wet removal of rBC. However we found that the wet removal process did not affect the rBC size, resulting in unchanged Eabs. We observed a large seasonal contrast in rBC properties with higher MrBC and Eabs in summer than in winter. In winter a high diurnal variability in MrBC (Eabs) with higher (lower) values in the middle of the day was linked to the injection of rBC originating from the PBL. On the contrary, in summer, MrBC showed no diurnal variation despite more frequent PBL conditions, implying that MrBC fluctuations are rather dominated by regional and long-range transport in the FT. Combining the ΔMrBC/ΔCO ratio with air mass transport analysis, we observed additional sources from biomass burning in summer leading to an increase in MrBC and Eabs. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of ∼2.9 observed at midday. We suggest that this daily variation may result from a photochemical process driving the rBC mixing state rather than a change in BC emission sources. Such direct 2-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model-predicted and observed effects of BC on the regional radiation budget and climate. The results demonstrate the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate forcer with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a two-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded aethalometer AE33, a thermal-optical analyzer Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations of the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type, despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy was explained by the too low MAC and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentration were below 25 µ gC cm−2 , which is probably linked to the incorrect determination of the OC-EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution are needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

Through observations of NO, NO2, NOY and O3 in the Rambouillet forest near Paris, France, (as part of the ACROSS campaign, 2022) we have gained insight into nighttime processes controlling NOX in an anthropogenically impacted forest environment. O3 mixing ratios displayed a strong diel profile at the site, which was driven by a variable but generally rapid deposition to soil and foliar surfaces. The O3 diel profile was strongly influenced by relative humidity, which impacted the surface resistance to uptake, and temperature inversion, which influenced the rate of entrainment of O3 from above the canopy. Only when the O3 mixing ratio was sufficiently low (and thus the NO lifetime sufficiently long), were sustained NO peaks observed above the instrumental detection limit, enabling derivation of average NO emission rates from the soil of ~1.4 ppbv h‑1. Observations of the lack of increase in NO2 at night, despite a significant production rate from the reaction of NO with O3, enabled an effective lifetime of NO2 of ⁓0.5–3 h to be derived. As the loss of NO2 was not compensated by the formation of gas- or particle-phase reactive nitrogen species it was presumably driven by deposition to soil and foliar surfaces, or any products formed were themselves short-lived with respect to deposition. By comparison, the daytime lifetime of NO2 with respect to loss by reaction with OH is about 1 day. We conclude that the nighttime deposition of NO2 is a major sink of boundary layer NOX in this temperate forest environment. [ABSTRACT FROM AUTHOR]

Through observations of NO, NO2, NOY and O3 in the Rambouillet forest near Paris, France, (as part of the ACROSS campaign, 2022) we have gained insight into nighttime processes controlling NOX in an anthropogenically impacted forest environment. O3 mixing ratios displayed a strong diel profile at the site, which was driven by a variable but generally rapid deposition to soil and foliar surfaces. The O3 diel profile was strongly influenced by relative humidity, which impacted the surface resistance to uptake, and temperature inversion, which influenced the rate of entrainment of O3 from above the canopy. Only when the O3 mixing ratio was sufficiently low (and thus the NO lifetime sufficiently long), were sustained NO peaks observed above the instrumental detection limit, enabling derivation of average NO emission rates from the soil of -1.4 ppbv h-1. Observations of the lack of increase in NO2 at night, despite a significant production rate from the reaction of NO with O3, enabled an effective lifetime of NO2 of -0.5-3 h to be derived. As the loss of NO2 was not compensated by the formation of gas- or particle-phase reactive nitrogen species it was presumably driven by deposition to soil and foliar surfaces, or any products formed were themselves short-lived with respect to deposition. By comparison, the daytime lifetime of NO2 with respect to loss by reaction with OH is about 1 day. We conclude that the nighttime deposition of NO2 is a major sink of boundary layer NOX in this temperate forest environment. [ABSTRACT FROM AUTHOR]

Black Carbon containing particles (BC) are strong light absorbers, causing substantial radiative heating of the atmosphere. The climate-relevant properties of BC are poorly constrained in high-elevation mountain regions, where numerous complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents two-year measurements of BC microphysical and optical properties at the research station of Pic du Midi (PDM), a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the worldwide existing long-term monitoring sites, PDM has experiences limited influence of the planetary boundary layer (PBL), making it an appropriate site for characterizing free tropospheric (FT) BC. The classification of the dominant aerosol type using the spectral optical properties of the aerosols indicates that BC was the predominant absorption component of aerosols at PDM and controlled the variation of Single Scattering Albedo (SSA) throughout the two years. Single-particle soot photometer (SP2) measurements showed a mean mass concentrations of BC (MBC) of 35 ng m−3 and a relatively constant BC core mass-equivalent diameter of around 180 nm, which are typical values for remote mountain sites. Combining the MBC with in situ absorption measurements yielded a BC mass absorption coefficient (MACBC) of 9.8 ± 2.7 m2 g−1 at 880 nm, which corresponds to an absorption enhancement (Eabs) of 2.4 compared to that of bare BC particles with equal BC core size distribution. A significant reduction of the ratio ∆BC / ∆CO when precipitation occurred along the air mass transport suggests wet removal of BC. However we found that the wet removal process did not affect the size of BC, resulting in unchanged Eabs. We observed a large seasonal contrast in BC properties with higher MBC and Eabs in summer than winter. In winter a strong diurnal variability of MBC (Eabs) with higher (lower) values in the middle of the day was linked to the injection of BC originating from the PBL. During summer in contrast, MBC showed no diurnal variation was rather constant despite more frequent PBL-conditions, implying that MBC fluctuations were rather dominated by regional and long-range transport in the FT. A body of evidence suggests that biomass burning emissions effectively altered the concentration and optical properties of BC at PDM, leading to higher Eabs in summer compared to winter. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of 2.9 observed at noon. We suggest that this daily variation results from photochemical processing driving BC mixing state rather than a change in BC emission source. Such direct two-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model predicted and observed effects of BC on regional radiation budget and climate. The results demonstrates the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC. [ABSTRACT FROM AUTHOR]

Low level stratiform clouds (LLSCs), covering a large area, appear frequently during the wet monsoon season in southernWest Africa. This region is also the place where different types of aerosols coexist, including biomass burning aerosols coming from Central and South Africa and anthropogenic aerosols emitted by local activities. We investigate the semi-direct and indirect effects of these aerosols on the diurnal cycle of LLSCs by constructing a case study based on aircraft-based and ground-based observations from the Dynamic-Aerosol-Chemistry-Cloud-Interaction in West Africa (DACCIWA) field campaign. This case is modelled using a Large Eddy Simulation (LES) model with fine scale resolution and in-situ aerosol measurements including size distribution and chemical composition. The model has successfully reproduced the observed life cycle of the LLSC, from stratus formation to stabilization during the night, to upward development after sunrise until break-up of cloud deck in afternoon. Various sensitivity simulations using different measured aerosol profiles based on measurements also suggest that aerosols can affect the cloud life cycle through both the indirect and semi-direct effect. Despite precipitation produced by the modeled cloud is nearly negligible, clouds lifetime is still sensitive to the aerosol concentration. As expected, modeled cloud microphysical features including cloud droplet number concentration, mean radius, and thus cloud reflectivity are all controlled by aerosol concentration. However, it is found that the difference in cloud reflectivity is not always the only factor in determining the variation of the incoming solar radiation at ground and cloud life cycle specifically beyond sunrise. Instead, the difference in cloud-void space brought by dry air entrainment from above and thus the speed of consequent evaporation - also influenced by aerosol concentration, is an another important factor to consider. Results have shown that clouds in the case with lower aerosol concentration and larger droplet size appear to be less affected by entrainment and convection. In addition, we found that an excessive atmospheric heating up to 12 K day-1 produced by absorbing black carbon aerosols (BC) in our modeled cases can also affect the life cycle of modeled clouds. Such a heating is found to lower the height of cloud top and stabilize the cloud layer, resulting a less extent in vertical development and accelerating clouds break-up. The semi-direct effect impacts on indirect effect by reducing cloud reflectivity particularly in case of polluted environment. Finally, semi-direct effect is found to contribute positively to the indirect radiative forcing due to a decreased cloud-void space, and negatively by causing thinner clouds that would break-up faster in late afternoon, all depending on the phase in stratiform cloud diurnal cycle. [ABSTRACT FROM AUTHOR]

Aerosol aware microphysics parameterisation schemes are increasingly being introduced into numerical weather prediction models, allowing for regional and case specific parameterisation of cloud condensation nuclei (CCN) and cloud droplet interactions. In this paper, the Thompson aerosol aware microphysics scheme, within the Weather, Research and Forecasting (WRF) model, is parameterised for two fog cases during September 2017 over Namibia. Measurements of CCN and fog microphysics were undertaken during the Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign at Henties Bay on the coast of Namibia during September 2017. A key concept of the microphysics scheme is the conversion of water friendly aerosols to cloud droplets (hereafter referred to as CCN activation), which could be estimated from the observations. A fog monitor 100 (FM100) provided cloud droplet size distribution, number concentration (Nt), liquid water content (LWC) and mean volumetric diameter (MVD). These measurements are used to evaluate and parameterise WRF model simulations of Nt, LWC and MVD. A sensitivity analysis was conducted through variations to the initial CCN concentration, CCN radius and the minimum updraft speed, important factors that influence droplet activation in the microphysics scheme of the model. The first model scenario made use of the default settings with a constant initial CCN number concentration of 300 cm-3 and underestimated the cloud droplet number concentration while the LWC was in good agreement with the observations. This resulted in droplet size being larger than the observations. Another scenario used modelled data as CCN initial conditions which were an order of magnitude higher than other scenarios. However, these provided the most realistic values of Nt, LWC, MVD and droplet size distribution. From this it was concluded that CCN activation of around 10 % in the simulations is too low, while the observed appears to be higher reaching between with a mean (median) of 0.55 (0.56) during fog events. To achieve this level of activation in the model, the minimum updraft speed for CCN activation was increased from 0.01 to 0.1 ms-1. This scenario provided Nt, LWC, MVD and droplet size distribution in the range of the observations with the added benefit of a realistic initial CCN concentration. These results demonstrate the benefits of a dynamic aerosol aware scheme when parameterised with observations. [ABSTRACT FROM AUTHOR]

During the West African summer monsoon, pollutants emitted in urbanized coastal areas modify cloud cover and precipitation patterns. The Dynamics-Aerosol-Chemistry-Cloud-Interactions in West Africa (DACCIWA) field campaign provided numerous aircraft-based and ground-based observations, which are used here to evaluate two experiments made with the coupled WRF-CHIMERE model, integrating both the direct and indirect aerosol effect on meteorology. During one well-documented week (1-7 July 2016), the impacts of anthropogenic aerosols on the diurnal cycle of low-level clouds and precipitation are analyzed in detail using high and moderate intensity of anthropogenic emissions in the experiments. Over the continent and close to major anthropogenic emission sources, the breakup time of low-level clouds is delayed by one hour, and the daily precipitation rate decreased by 7.5 % with the enhanced anthropogenic emission experiment (with high aerosol load). Despite the small modifications on daily average of low-level cloud cover (+2.6 %) with high aerosol load compared to moderate, there is an increase by more than 20 % from 14:00 to 22:00 UTC on hourly average. Moreover, modifications of the modeled low-level cloud and precipitation rate occur far from the major anthropogenic emission sources, to the south over the ocean and to the north up to 11° N. The present study adds evidence to recent findings that enhanced pollution levels in West Africa may reduce precipitation. [ABSTRACT FROM AUTHOR]

Aerosol particles contribute to the climate forcing through their optical properties. Measuring these aerosol optical properties is still challenging, especially considering the hygroscopic growth of aerosol particles, which alters their optical properties. Lidar and in-situ techniques can derive a variety of aerosol optical properties, like aerosol particle light extinction, backscattering, and absorption. But these techniques are subject to some limitations and uncertainties. Within this study, we compared with Mie-theory modeled aerosol optical properties with direct measurements. At dried state they were with airborne and ground-based in-situ measurements; at ambient state with lidar estimates. Also, we examined the dependence of the aerosol particle light extinction-to-backscatter ratio, also lidar ratio (LR), to relative humidity. The used model was fed with measured physicochemical aerosol properties and ambient atmospheric conditions. The model considered aerosol particles in an internal core-shell mixing state with constant volume fractions of the aerosol components over the entire observed aerosol particle size-range. The underlying set of measurements was conducted near the measurement site Melpitz, Germany, during two campaigns in summer, 2015, and winter, 2017, and represent Central European background aerosol conditions. Two airborne payloads deployed on a helicopter and a balloon provided measurements of microphysical and aerosol optical properties and were complemented by the polarization Raman lidar system PollyXT as well as by a holistic set of microphysical, chemical and optical aerosol measurements derived at ground level. The calculated aerosol optical aerosol properties agreed within 13% (3%) with the ground-based in-situ measured aerosol optical properties at a dried state (relative humidity below 40%) in terms of scattering at 450 nm wavelength during the winter (summer) campaign. The model also represented the aerosol particle light absorption at 637 nm within 8% (18%) during the winter (summer) campaign and agreed within 13% with the airborne in-situ aerosol particle light extinction measurements during summer. During winter, in a comparatively clean case with equivalent black carbon mass-concentrations of around 0.2 µg m-3 the modeled airborne measurement-based aerosol particle light absorption, was up to 32-37% larger than the measured values during a relatively clean period. However, during a high polluted case, with an equivalent black carbon mass concentration of around 4 µg m-3, the modeled aerosol particle light absorption coefficient was, depending on the wavelength, 13-32% lower than the measured values. Spread and magnitude of the disagreement highlighted the importance of the aerosol mixing state used within the model, the requirement of the inclusion of brown carbon, and a wavelength-dependent complex refractive index of black and brown carbon when such kind of model is used to validate aerosol particle light absorption coefficient estimates of, e.g., lidar systems. Besides dried state comparisons, ambient modeled aerosol particle light extinction, as well as aerosol particle light backscattering, were compared with lidar estimates of these measures. During summer, on average, for four of the twelve conducted measurement flights, the model calculated lower aerosol particle light extinction (up to 29% lower) as well as backscattering (up to 32% lower) than derived with the lidar. In winter, the modeled aerosol particle light extinction coefficient was 17%-41% lower, the aerosol particle light backscattering coefficient 14%-42% lower than the lidar estimates. For both, the winter and summer cases, the Mie-model estimated reasonable extinction-to-backscatter ratios (LR). Measurement-based Mie-modeling showed evidence of the dependence of the LR on relative humidity (RH). With this result, we presented a fit for lidar wavelengths of 355, 532, and 1064 nm with an underlying equation of f[sub LR](TH, γ(λ)) = f[sub LR] (RH = 0, λ) x (1 - RH)-γ(λ) and estimates of γ(355 nm) = 0.29 (±0.01), γ(532 nm) = 0.48 (±0.01), and γ(1064 nm) = 0.31 (±0.01). However, further measurements are required to entangle the behavior of the LR with respect to different aerosol types, to set up a climatology, and to assess the influence of the aerosol mixing state. This comprehensive study combining airborne and ground-based in-situ and remote sensing measurements, which simulated multiple aerosol optical coefficients in the ambient and dry state, is with its complexity unique of its kind. [ABSTRACT FROM AUTHOR]