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Measurement of water vapor or humidity in the atmosphere is fundamental for many applications. Relative humidity measurements with a capacitive sensor in radiosondes are affected by several factors that need to be assessed and corrected. This work aims to address corrections for the main effects for the Meteomodem M10 radiosonde as a step to meet the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) requirements. The considered corrections are 1) the calibration correction; 2) a slow regime due to the slow diffusion of molecules through the sensor, especially at very high and very low relative humidity conditions; 3) the relative humidity sensor dependence on the gradient of temperature; and 4) the time lag at cold temperatures, which affects measurements in regions of strong relative humidity gradients. These corrections were tested for 26 nighttime and 25 daytime radiosondes in two midlatitude locations for which both Meteomodem M10 and Vaisala RS92 measurements were available. The results show that, after correcting for the four effects, M10 relative humidity measurements are, on average, consistent with the Vaisala RS92 relative humidity values within 2% RH at all altitudes for the nighttime launches (against 6% RH before the correction) and within 5% RH at all altitudes for the daytime launches (against 9% RH before the correction). [ABSTRACT FROM AUTHOR]

While droplets with pure mixtures of water and sulfuric acid are the main component of stratospheric aerosols, field measurements performed for more than 30 years have shown that non-sulfate materials, thereafter referred to by us as NSP (for Non-pure Sulfate Particles, not considering frozen material) are also present. Such materials, which are released from both the Earth through volcanic eruptions, pollution or biomass burning, and from space through interplanetary dust and micrometeoroids, present a wide variety of composition and shape, with sizes ranging from several nm to several hundreds of μm. No single instrumental technique, from ground, from airplanes, under balloons and onboard satellites using remote-sensing and in-situ instruments. can provide alone a global view of the stratospheric NSPs, which exhibit a strong variability in terms of spatial distribution and composition. To better understand the origin of the NSPs, we have performed new field measurements from mid- 2013 with the Light Optical Aerosol Counter (LOAC) instrument during 135 flights carried out under weather balloons at various latitudes and up to altitudes of 35 km. Coupled with previous measurements obtained with the Tropospheric and Stratospheric Aerosols Counter (STAC) under stratospheric balloons in the 2004–2011 period, the LOAC measurements show the presence of stratospheric layers presenting enhanced-concentrations associated with NSPs, with a bimodal vertical repartition centered by 17 and 30 km altitude. Also, large particles are detected, with sizes up to several tens of μm, with decreasing concentrations with increasing altitudes. Such observations, which are not correlated with meteor shower events, could be due to dynamical and photophoretic effects lifting and sustaining particles mainly coming from the Earth. When combining all the detections in the stratosphere from different methods of measurements, we may conclude that the concentrations and the vertical distributions of NSPs are highly variable and do not match the estimated concentrations of material in space at Earth orbit. The paper ends by highlighting some open questions on these stratospheric materials and presents some possible new strategies for frequent measurements, to confirm that NSPs are indeed mainly of terrestrial origin, and to better circumvent the NSPs impact on stratospheric chemistry and on the Earth’s climate. [ABSTRACT FROM AUTHOR]

This paper describes the aerosol measurement setup and results obtained during the BEXUS18 (Balloon-borne Experiments for University Students) stratospheric balloon within the A5-Unibo (Advanced Atmospheric Aerosol Acquisition and Analysis) experiment performed on 10 October 2014 in northern Sweden (Kiruna). The experimental setup was designed and developed by the University of Bologna with the aim of collecting and analyzing vertical profiles of atmospheric ions and particles together with atmospheric parameters (temperature, relative humidity, and pressure) all along the stratospheric ascent of the BEXUS18 stratospheric balloon. Particle size distributions were measured with the MeteoModem Light Optical Aerosol Counter (LOAC) and air ion density was measured with a set of two commercial and portable ion counters. Though the experimental setup was based upon relatively low-cost and light-weight sensors, vertical profiles of all the parameters up to an altitude of about 27 km were successfully collected. The results obtained are useful for elucidating the relationships between aerosols and charged particles between ground level and the stratosphere, with great potential in collecting and adding useful information in this field, also in the stratosphere where such measurements are rare. In particular, the equipment detected coherent vertical profiles for particles and ions, with a particularly strong correlation between negative ions and fine particles, possibly resulting from proposed associations between cosmic rays and ions as previously suggested. In addition, the detection of charged aerosols in the stratosphere is in agreement with the results obtained by a previous flight and with simulations conducted with a stratospheric ion–aerosol model. However, further measurements under stratospheric balloon flights equipped with a similar setup are needed to reach general conclusions about such important issues. [ABSTRACT FROM AUTHOR]

Mineral dust from arid areas is a major component of global aerosol and has strong interactions with climate and biogeochemistry. As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) to investigate atmospheric chemistry and its impacts in the Mediterranean region, an intensive field campaign was performed from mid- June to early August 2013 in the western basin including in situ balloon-borne aerosol measurements with the light optical aerosol counter (LOAC). LOAC is a counter/sizer that provides the aerosol concentrations in 19 size classes between 0.2 and 100 µm, and an indication of the nature of the particles based on dual-angle scattering measurements. A total of 27 LOAC flights were conducted mainly from Minorca Island (Balearic Islands, Spain) but also from Ile du Levant off Hyères city (SE France) under 17 light dilatable balloons (meteorological sounding balloons) and 10 boundary layer pressurised balloons (quasi-Lagrangian balloons). The purpose was to document the vertical extent of the plume and the time evolution of the concentrations at constant altitude (air density) by in situ observations. LOAC measurements are in agreement with ground-based measurements (lidar, photometer), aircraft measurements (counters), and satellite measurements (CALIOP) in the case of fair spatial and temporal coincidences. LOAC has often detected three modes in the dust particle volume size distributions fitted by lognormal laws at roughly 0.2, 4 and 30 µm in modal diameter. Thanks to the high sensitivity of LOAC, particles larger than 40 µm were observed, with concentrations up to about 10-4 cm-3. Such large particles were lifted several days before and their persistence after transport over long distances is in conflict with calculations of dust sedimentation. We did not observe any significant evolution of the size distribution during the transport from quasi-Lagrangian flights, even for the longest ones (~1 day). Finally, the presence of charged particles is inferred from the LOAC measurements and we speculate that electrical forces might counteract gravitational settling of the coarse particles. [ABSTRACT FROM AUTHOR]

After 43 years of inactivity, the Calbuco volcano, which is located in the southern part of Chile, erupted on 22 April 2015. The space-time evolutions (distribution and transport) of its aerosol plume are investigated by combining satellite (CALIOP, IASI, OMPS), in situ aerosol counting (LOAC OPC) and lidar observations, and the MIMOSA advection model. The Calbuco aerosol plume reached the Indian Ocean 1 week after the eruption. Over the Reunion Island site (21° S, 55.5° E), the aerosol signal was unambiguously enhanced in comparison with "background" conditions, with a volcanic aerosol layer extending from 18 to 21 km during the May-July period. All the data reveal an increase by a factor of ~2 in the SAOD (stratospheric aerosol optical depth) with respect to values observed before the eruption. The aerosol mass e-folding time is approximately 90 days, which is rather close to the value (~80 days) reported for the Sarychev eruption. Microphysical measurements obtained before, during, and after the eruption reflecting the impact of the Calbuco eruption on the lower stratospheric aerosol content have been analyzed over the Reunion Island site. During the passage of the plume, the volcanic aerosol was characterized by an effective radius of 0.16±0.02 μm with a unimodal size distribution for particles above 0.2 μm in diameter. Particle concentrations for sizes larger than 1 μm are too low to be properly detected by the LOAC OPC. The aerosol number concentration was ~20 times higher that observed before and 1 year after the eruption. According to OMPS and lidar observations, a tendency toward conditions before the eruption was observed by April 2016. The volcanic aerosol plume is advected eastward in the Southern Hemisphere and its latitudinal extent is clearly bounded by the subtropical barrier and the polar vortex. The transient behavior of the aerosol layers observed above Reunion Island between May and July 2015 reflects an inhomogeneous spatio-temporal distribution of the plume, which is controlled by the localization of these dynamical barriers. [ABSTRACT FROM AUTHOR]

Mineral dust from arid areas is a major component of the global aerosol and has strong interactions with climate and biogeochemistry. As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) to investigate atmospheric chemistry and its impacts in the Mediterranean region, an intensive field campaign was performed from mid-June to early August 2013 in the western basin including in situ balloon-borne aerosol measurements with the Light Optical Aerosol Counter (LOAC). LOAC is a counter/sizer that provides the aerosol concentrations in 19 size classes between 0.2 and 100 μm, and an indication of the nature of the particles based on dual angle scattering measurements. A total of 27 LOAC flights were conducted mainly from Minorca Island (Balearic Islands, Spain) but also from Ile du Levant off Hyères city (SE France) under 17 Light Dilatable Balloons (meteorological sounding balloons) and 10 Boundary Layer Pressurized Balloons (quasi-Lagrangian balloons). The purpose was to document the vertical extent of the plume and the time-evolution of the concentrations at constant altitude (air density) by in situ observations. LOAC measurements are in agreement with ground-based measurements (lidar, photometer), aircraft measurements (counters), and satellite measurements (CALIOP) in case of fair spatial and temporal coincidences. LOAC has often detected 3 modes in the dust particle volume size distributions fitted by lognormal laws at roughly 0.2, 4 and 30 μm in modal diameter. Particles larger than 40 μm were observed, with concentrations up to about 10-4 cm-3. Such large particles were lifted several days before and their persistence after transport over long distances is in conflict with calculations of dust sedimentation. We did not observe any significant evolution of the size distribution during the transport from quasi-Lagrangian flights, even for the longest ones (~ 1 day). Finally, the presence of charged particles is inferred from the LOAC measurements and we speculate that electrical forces might counteract gravitational settling of the coarse particles. [ABSTRACT FROM AUTHOR]

After 43 years of inactivity, the Calbuco volcano which is located in the southern part of Chile erupted on 22 April 2015. The space-time evolutions (distribution and transport) of its aerosol plume are investigated by combining satellite (CALIOP, IASI, OMPS), in situ aerosol counting (LOAC OPC) and lidar observations, and the MIMOSA advection model. The Calbuco aerosol plume reached the Indian Ocean 1 week after the eruption. Over the Reunion Island site (21°â€‰S; 55.5°â€‰E), the aerosol signal was unambiguously enhanced in comparison with "background" conditions with a volcanic aerosol layer extending from 18 km to 21 km during the May-July period. All the data reveal an increase by a factor of ~ 2 in the SAOD (Stratospheric Aerosol Optical Depth) with respect to values observed before the eruption. The aerosol e-folding time is approximately 90 days. Microphysical measurements obtained before, during and after the eruption reflecting the impact of the Calbuco eruption on the lower stratospheric aerosol content have been analyzed over Reunion site. During the passage of the plume, the volcanic aerosol was characterized by an effective radius of 0.16 ±â€‰0.02 μm with an unimodal lognormal size distribution and the aerosol number concentration appears 20 times higher than before and one year after the eruption. A tendency toward "background" conditions has been observed about one year after the eruption, by April 2016. The volcanic aerosol plume is advected eastward in the Southern Hemisphere and its latitudinal extent is clearly bounded by the subtropical barrier and the polar vortex. The transient behavior of the aerosol layers observed above Reunion Island between May and July 2015 reflects an inhomogeneous geographical distribution of the plume which is controlled by the latitudinal motion of these dynamical barriers. [ABSTRACT FROM AUTHOR]

The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at midlatitudes. Since then, only "moderate" but recurrent volcanic eruptions have modulated the stratospheric aerosol loading and are assumed to be one cause for the reported increase in the global aerosol content over the past 15 years. This particularly enhanced aerosol context raises questions about the effects on stratospheric chemistry which depend on the latitude, altitude and season of injection. In this study, we focus on the midlatitude Sarychev volcano eruption in June 2009, which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) into a lower stratosphere mainly governed by high-stratospheric temperatures. Together with in situ measurements of aerosol amounts, we analyse high-resolution in situ and/or remote-sensing observations of NO2, HNO3 and BrO from balloon-borne infrared and UV-visible spectrometers launched in Sweden in August-September 2009. It is shown that differences between observations and three-dimensional (3-D) chemistry-transport model (CTM) outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km altitude. Good measurement-model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of ~ 45 % and increases of ~ 11 % in NO2 and HNO3 amounts respectively over the August-September 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (~ 22 %) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2hydrolysis. We show that the chlorine partitioning is significantly controlled by enhanced BrONO2 hydrolysis. However, simulated effects of the Sarychev eruption on chlorine activation are very limited in the high-temperature conditions in the stratosphere in the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated chemical ozone loss due to the Sarychev aerosols is low with a reduction of -22 ppbv (-1.5 %) of the ozone budget around 16 km. This is at least 10 times lower than the maximum ozone depletion from chemical processes (up to -20 %) reported in the Northern Hemisphere lower stratosphere over the first year following the Pinatubo eruption. This study suggests that moderate volcanic eruptions have limited chemical effects when occurring at midlatitudes (restricted residence times) and outside winter periods (high-temperature conditions). However, it would be of interest to investigate longer-lasting tropical volcanic plumes or sulfur injections in the wintertime low-temperature conditions. [ABSTRACT FROM AUTHOR]

The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at mid-latitudes. Since then, only "moderate" but recurrent volcanic eruptions have modulated the stratospheric aerosol loading such as the eruption of the mid-latitude Sarychev volcano which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) in June 2009. In this study, we investigate the chemical impacts of the enhanced liquid sulfate aerosol loading resulting from this moderate eruption using data from a balloon campaign conducted in northern Sweden (Kiruna-Esrange, 67.5° N, 21.0° E) in August-September 2009. Balloon-borne observations of NO2, HNO3 and BrO from infrared and UV-visible spectrometers are compared with the outputs of a three-dimensional (3-D) Chemistry-Transport Model (CTM). It is shown that differences between observations and model outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km in altitude. Good measurement-model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of ~ 45% and increases of ~ 11% in NO2 and HNO3 amounts respectively over the summer 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (~ 22%) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2 hydrolysis. Simulated effects of the Sarychev eruption on chlorine activation and partitioning are very limited in the high temperature conditions in the stratosphere at the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated ozone loss due to the Sarychev aerosols is low with a reduction of 1.1% of the ozone budget at 16.5 km. Some comparisons with the reported Pinatubo chemical impacts are also provided and overall the Sarychev aerosols have led to less chemical effects than the Pinatubo event. [ABSTRACT FROM AUTHOR]

In the companion (Part I) paper, we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosol Counter), based on scattering measurements at angles of 12 and 60°. That allows for some typology identification of particles (droplets, carbonaceous, salts, and mineral dust) in addition to sizesegregated counting in a large diameter range from 0.2 µm up to possibly more than 100 µm depending on sampling conditions (Renard et al., 2016). Its capabilities overpass those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronicsized absorbing carbonaceous particles in polluted air to very coarse particles (>10-20 µm in diameter) in desert dust plumes or fog and clouds. LOAC's light and compact design allows measurements under all kinds of balloons, on-board unmanned aerial vehicles (UAVs) and at ground level. We illustrate here the first LOAC airborne results obtained from a UAV and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Vienna (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediterranean (during the Chemistry-Aerosol Mediterranean Experiment - ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in south-western France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes. [ABSTRACT FROM AUTHOR]

Coupled balloon-borne observations of Light Optical Aerosol Counter (LOAC), M10 meteorological global positioning system (GPS) sondes, ozonesondes, and GPS radio occultation data, are examined to identify gravity-wave (GW)-induced fluctuations on tracer gases and on the vertical distribution of stratospheric aerosol concentrations during the 2013 ChArMEx (Chemistry-Aerosol Mediterranean Experiment) campaign. Observations reveal signatures of GWs with short vertical wavelengths less than 4 km in dynamical parameters and tracer constituents, which are also correlated with the presence of thin layers of strong local enhancements of aerosol concentrations in the upper troposphere and the lower stratosphere. In particular, this is evident from a case study above Ile du Levant (43.02 N, 6.46 E) on 26-29 July 2013. Observations show a strong activity of dominant mesoscale inertia GWs with horizontal and vertical wavelengths of 370-510 km and 2-3 km respectively, and periods of 10-13 h propagating southward at altitudes of 13-20 km during 27-28 July. The European Centre for Medium-Range Weather Forecasts (ECMWF) analyses also show evidence of mesoscale inertia GWs with similar horizontal characteristics above the eastern part of France. Raytracing experiments indicate the jet-front system as the main source of observed GWs. Using a simplified linear GW theory, synthetic vertical profiles of dynamical parameters with large stratospheric vertical wind maximum oscillations of -40 mms-1 are produced for the dominant mesoscale GW observed at heights of 13-20 km. Parcel advection method reveals signatures of GWs in the ozone mixing ratio and the tropospheric-specific humidity. Simulated vertical wind perturbations of the dominant GWs and small-scale perturbations of aerosol concentration (aerosol size of 0.2-0.7 µm) are revealed to be in phase in the lower stratosphere. Present results support the importance of vertical wind perturbations in the GW-aerosol relationship. Observed mesoscale GWs induce a strong modulation of the amplitude of tracer gases and the stratospheric aerosol background. [ABSTRACT FROM AUTHOR]

The study of aerosols in the troposphere and in the stratosphere is of major importance both for climate and air quality studies. Among the numerous instruments available, optical aerosol particles counters (OPCs) provide the size distribution in diameter range from about 100 nm to a few tens of µm. Most of them are very sensitive to the nature of aerosols, and this can result in significant biases in the retrieved size distribution. We describe here a new versatile optical particle/sizer counter named LOAC (Light Optical Aerosol Counter), which is light and compact enough to perform measurements not only at the surface but under all kinds of balloons in the troposphere and in the stratosphere. LOAC is an original OPC performing observations at two scattering angles. The first one is around 12°, and is almost insensitive to the refractive index of the particles; the second one is around 60° and is strongly sensitive to the refractive index of the particles. By combining measurement at the two angles, it is possible to retrieve the size distribution between 0.2 and 100 µm and to estimate the nature of the dominant particles (droplets, carbonaceous, salts and mineral particles) when the aerosol is relatively homogeneous. This typology is based on calibration charts obtained in the laboratory. The uncertainty for total concentrations measurements is ±20% when concentrations are higher than 1 particle cm-3 (for a 10 min integration time). For lower concentrations, the uncertainty is up to about ±60% for concentrations smaller than 10-2 particle cm-3. Also, the uncertainties in size calibration are ±0.025 μm for particles smaller than 0.6 μm, 5% for particles in the 0.7-2 μm range, and 10% for particles greater than 2 μm. The measurement accuracy of submicronic particles could be reduced in a strongly turbid case when concentration of particles > 3 µm exceeds a few particles cm-3. Several campaigns of cross-comparison of LOAC with other particle counting instruments and remote sensing photometers have been conducted to validate both the size distribution derived by LOAC and the retrieved particle number density. The typology of the aerosols has been validated in well-defined conditions including urban pollution, desert dust episodes, sea spray, fog, and cloud. Comparison with reference aerosol mass monitoring instruments also shows that the LOAC measurements can be successfully converted to mass concentrations. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]