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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 1 ( 2022-01-13), p. 505-533
    Abstract: Abstract. We present here the results obtained during an intensive field campaign conducted in the framework of the French “BIO-MAÏDO” (Bio-physico-chemistry of tropical clouds at Maïdo (Réunion Island): processes and impacts on secondary organic aerosols' formation) project. This study integrates an exhaustive chemical and microphysical characterization of cloud water obtained in March–April 2019 in Réunion (Indian Ocean). Fourteen cloud samples have been collected along the slope of this mountainous island. Comprehensive chemical characterization of these samples is performed, including inorganic ions, metals, oxidants, and organic matter (organic acids, sugars, amino acids, carbonyls, and low-solubility volatile organic compounds, VOCs). Cloud water presents high molecular complexity with elevated water-soluble organic matter content partly modulated by microphysical cloud properties. As expected, our findings show the presence of compounds of marine origin in cloud water samples (e.g. chloride, sodium) demonstrating ocean–cloud exchanges. Indeed, Na+ and Cl− dominate the inorganic composition contributing to 30 % and 27 %, respectively, to the average total ion content. The strong correlations between these species (r2 = 0.87, p value: 〈 0.0001) suggest similar air mass origins. However, the average molar Cl-/Na+ ratio (0.85) is lower than the sea-salt one, reflecting a chloride depletion possibly associated with strong acids such as HNO3 and H2SO4. Additionally, the non-sea-salt fraction of sulfate varies between 38 % and 91 %, indicating the presence of other sources. Also, the presence of amino acids and for the first time in cloud waters of sugars clearly indicates that biological activities contribute to the cloud water chemical composition. A significant variability between events is observed in the dissolved organic content (25.5 ± 18.4 mg C L−1), with levels reaching up to 62 mg C L−1. This variability was not similar for all the measured compounds, suggesting the presence of dissimilar emission sources or production mechanisms. For that, a statistical analysis is performed based on back-trajectory calculations using the CAT (Computing Atmospheric Trajectory Tool) model associated with the land cover registry. These investigations reveal that air mass origins and microphysical variables do not fully explain the variability observed in cloud chemical composition, highlighting the complexity of emission sources, multiphasic transfer, and chemical processing in clouds. Even though a minor contribution of VOCs (oxygenated and low-solubility VOCs) to the total dissolved organic carbon (DOC) (0.62 % and 0.06 %, respectively) has been observed, significant levels of biogenic VOC (20 to 180 nmol L−1) were detected in the aqueous phase, indicating the cloud-terrestrial vegetation exchange. Cloud scavenging of VOCs is assessed by measurements obtained in both the gas and aqueous phases and deduced experimental gas-/aqueous-phase partitioning was compared with Henry's law equilibrium to evaluate potential supersaturation or unsaturation conditions. The evaluation reveals the supersaturation of low-solubility VOCs from both natural and anthropogenic sources. Our results depict even higher supersaturation of terpenoids, evidencing a deviation from thermodynamically expected partitioning in the aqueous-phase chemistry in this highly impacted tropical area.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 2
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 8 ( 2020-08-17), p. 4353-4392
    Abstract: Abstract. Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 22 ( 2021-11-25), p. 17185-17223
    Abstract: Abstract. Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 102 cm−3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 103–104 cm−3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 102–103 cm−3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either 〉50 nm or 〉100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm−3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 8 ( 2017-04-25), p. 5355-5378
    Abstract: Abstract. The STRAP (Synergie Transdisciplinaire pour Répondre aux Aléas liés aux Panaches volcaniques) campaign was conducted over the entire year of 2015 to investigate the volcanic plumes of Piton de La Fournaise (La Réunion, France). For the first time, measurements at the local (near the vent) and at the regional scales were conducted around the island. The STRAP 2015 campaign has become possible thanks to strong cross-disciplinary collaboration between volcanologists and meteorologists. The main observations during four eruptive periods (85 days) are summarised. They include the estimates of SO2, CO2 and H2O emissions, the altitude of the plume at the vent and over different areas of La Réunion Island, the evolution of the SO2 concentration, the aerosol size distribution and the aerosol extinction profile. A climatology of the volcanic plume dispersion is also reported. Simulations and measurements show that the plumes formed by weak eruptions have a stronger interaction with the surface of the island. Strong SO2 mixing ratio and particle concentrations above 1000 ppb and 50 000 cm−3 respectively are frequently measured over a distance of 20 km from Piton de la Fournaise. The measured aerosol size distribution shows the predominance of small particles in the volcanic plume. Several cases of strong nucleation of sulfuric acid have been observed within the plume and at the distal site of the Maïdo observatory. The STRAP 2015 campaign provides a unique set of multi-disciplinary data that can now be used by modellers to improve the numerical parameterisations of the physical and chemical evolution of the volcanic plumes.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 5
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 10, No. 9 ( 2017-09-15), p. 3359-3373
    Abstract: Abstract. In order to recognize the importance of ozone (O3) in the troposphere and lower stratosphere in the tropics, a DIAL (differential absorption lidar) tropospheric O3 lidar system (LIO3TUR) was developed and installed at the Université de la Réunion campus site (close to the sea) on Reunion Island (southern tropics) in 1998. From 1998 to 2010, it acquired 427 O3 profiles from the low to the upper troposphere and has been central to several studies. In 2012, the system was moved up to the new Maïdo Observatory facility (2160 m a.m.s.l. – metres above mean sea level) where it started operation in February 2013. The current system (LIO3T) configuration generates a 266 nm beam obtained with the fourth harmonic of a Nd:YAG laser sent into a Raman cell filled up with deuterium (using helium as buffer gas), generating the 289 and 316 nm beams to enable the use of the DIAL method for O3 profile measurements. The optimal range for the actual system is 6–19 km a.m.s.l., depending on the instrumental and atmospheric conditions. For a 1 h integration time, vertical resolution varies from 0.7 km at 6 km a.m.s.l. to 1.3 km at 19 km a.m.s.l., and mean uncertainty within the 6–19 km range is between 6 and 13 %. Comparisons with eight electrochemical concentration cell (ECC) sondes simultaneously launched from the Maïdo Observatory show good agreement between data sets with a 6.8 % mean absolute relative difference (D) between 6 and 17 km a.m.s.l. (LIO3T lower than ECC). Comparisons with 37 ECC sondes launched from the nearby Gillot site during the daytime in a ±24 h window around lidar shooting result in a 9.4 % D between 6 and 19 km a.m.s.l. (LIO3T lower than ECC). Comparisons with 11 ground-based Network for Detection of Atmospheric Composition Change (NDACC) Fourier transform infrared (FTIR) spectrometer measurements acquired during the daytime in a ±24 h window around lidar shooting show good agreement between data sets with a D of 11.8 % for the 8.5–16 km partial column (LIO3T higher than FTIR), and comparisons with 39 simultaneous Infrared Atmospheric Sounding Interferometer (IASI) observations over Reunion Island show good agreement between data sets with a D of 11.3 % for the 6–16 km partial column (LIO3T higher than IASI). ECC, LIO3TUR and LIO3T O3 monthly climatologies all exhibit the same range of values and patterns. In particular, the Southern Hemisphere biomass burning seasonal enhancement and the ozonopause altitude decrease in late austral winter–spring, as well as the sign of deep convection bringing boundary layer O3-poor air masses up to the middle–upper troposphere in late austral summer, are clearly visible in all data sets.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 24 ( 2017-12-19), p. 15019-15036
    Abstract: Abstract. 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 19 ( 2018-10-01), p. 13881-13901
    Abstract: Abstract. Atmospheric carbon monoxide (CO) and methane (CH4) mole fractions are measured by ground-based in situ cavity ring-down spectroscopy (CRDS) analyzers and Fourier transform infrared (FTIR) spectrometers at two sites (St Denis and Maïdo) on Reunion Island (21∘ S, 55∘ E) in the Indian Ocean. Currently, the FTIR Bruker IFS 125HR at St Denis records the direct solar spectra in the near-infrared range, contributing to the Total Carbon Column Observing Network (TCCON). The FTIR Bruker IFS 125HR at Maïdo records the direct solar spectra in the mid-infrared (MIR) range, contributing to the Network for the Detection of Atmospheric Composition Change (NDACC). In order to understand the atmospheric CO and CH4 variability on Reunion Island, the time series and seasonal cycles of CO and CH4 from in situ and FTIR (NDACC and TCCON) measurements are analyzed. Meanwhile, the difference between the in situ and FTIR measurements are discussed. The CO seasonal cycles observed from the in situ measurements at Maïdo and FTIR retrievals at both St Denis and Maïdo are in good agreement with a peak in September–November, primarily driven by the emissions from biomass burning in Africa and South America. The dry-air column averaged mole fraction of CO (XCO) derived from the FTIR MIR spectra (NDACC) is about 15.7 ppb larger than the CO mole fraction near the surface at Maïdo, because the air in the lower troposphere mainly comes from the Indian Ocean while the air in the middle and upper troposphere mainly comes from Africa and South America. The trend for CO on Reunion Island is unclear during the 2011–2017 period, and more data need to be collected to get a robust result. A very good agreement is observed in the tropospheric and stratospheric CH4 seasonal cycles between FTIR (NDACC and TCCON) measurements, and in situ and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite measurements, respectively. In the troposphere, the CH4 mole fraction is high in August–September and low in December–January, which is due to the OH seasonal variation. In the stratosphere, the CH4 mole fraction has its maximum in March–April and its minimum in August–October, which is dominated by vertical transport. In addition, the different CH4 mole fractions between the in situ, NDACC and TCCON CH4 measurements in the troposphere are discussed, and all measurements are in good agreement with the GEOS-Chem model simulation. The trend of XCH4 is 7.6±0.4 ppb yr−1 from the TCCON measurements over the 2011 to 2017 time period, which is consistent with the CH4 trend of 7.4±0.5 ppb yr−1 from the in situ measurements for the same time period at St Denis.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 8
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 14, No. 1 ( 2021-01-05), p. 89-116
    Abstract: Abstract. The Integrated Carbon Observation System (ICOS) is a pan-European research infrastructure which provides harmonized and high-precision scientific data on the carbon cycle and the greenhouse gas budget. All stations have to undergo a rigorous assessment before being labeled, i.e., receiving approval to join the network. In this paper, we present the labeling process for the ICOS atmosphere network through the 23 stations that were labeled between November 2017 and November 2019. We describe the labeling steps, as well as the quality controls, used to verify that the ICOS data (CO2, CH4, CO and meteorological measurements) attain the expected quality level defined within ICOS. To ensure the quality of the greenhouse gas data, three to four calibration gases and two target gases are measured: one target two to three times a day, the other gases twice a month. The data are verified on a weekly basis, and tests on the station sampling lines are performed twice a year. From these high-quality data, we conclude that regular calibrations of the CO2, CH4 and CO analyzers used here (twice a month) are important in particular for carbon monoxide (CO) due to the analyzer's variability and that reducing the number of calibration injections (from four to three) in a calibration sequence is possible, saving gas and extending the calibration gas lifespan. We also show that currently, the on-site water vapor correction test does not deliver quantitative results possibly due to environmental factors. Thus the use of a drying system is strongly recommended. Finally, the mandatory regular intake line tests are shown to be useful in detecting artifacts and leaks, as shown here via three different examples at the stations.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 9
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 12 ( 2020-12-21), p. 6999-7024
    Abstract: Abstract. The TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (S5P) satellite was launched on 13 October 2017 to provide the atmospheric composition for atmosphere and climate research. The S5P is a Sun-synchronous polar-orbiting satellite providing global daily coverage. The TROPOMI swath is 2600 km wide, and the ground resolution for most data products is 7.2×3.5 km2 (5.6×3.5 km2 since 6 August 2019) at nadir. The Finnish Meteorological Institute (FMI) is responsible for the development of the TROPOMI UV algorithm and the processing of the TROPOMI surface ultraviolet (UV) radiation product which includes 36 UV parameters in total. Ground-based data from 25 sites located in arctic, subarctic, temperate, equatorial and Antarctic areas were used for validation of the TROPOMI overpass irradiance at 305, 310, 324 and 380 nm, overpass erythemally weighted dose rate/UV index, and erythemally weighted daily dose for the period from 1 January 2018 to 31 August 2019. The validation results showed that for most sites 60 %–80 % of TROPOMI data was within ±20 % of ground-based data for snow-free surface conditions. The median relative differences to ground-based measurements of TROPOMI snow-free surface daily doses were within ±10 % and ±5 % at two-thirds and at half of the sites, respectively. At several sites more than 90 % of cloud-free TROPOMI data was within ±20 % of ground-based measurements. Generally median relative differences between TROPOMI data and ground-based measurements were a little biased towards negative values (i.e. satellite data 〈 ground-based measurement), but at high latitudes where non-homogeneous topography and albedo or snow conditions occurred, the negative bias was exceptionally high: from −30 % to −65 %. Positive biases of 10 %–15 % were also found for mountainous sites due to challenging topography. The TROPOMI surface UV radiation product includes quality flags to detect increased uncertainties in the data due to heterogeneous surface albedo and rough terrain, which can be used to filter the data retrieved under challenging conditions.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 17 ( 2020-09-10), p. 10565-10586
    Abstract: Abstract. Balloon-borne measurements of cryogenic frost-point hygrometer (CFH) water vapor, ozone and temperature and water vapor lidar measurements from the Maïdo Observatory on Réunion Island in the southwest Indian Ocean (SWIO) were used to study tropical cyclones' influence on tropical tropopause layer (TTL) composition. The balloon launches were specifically planned using a Lagrangian model and Meteosat-7 infrared images to sample the convective outflow from tropical storm (TS) Corentin on 25 January 2016 and tropical cyclone (TC) Enawo on 3 March 2017. Comparing the CFH profile to Aura's Microwave Limb Sounder's (MLS) monthly climatologies, water vapor anomalies were identified. Positive anomalies of water vapor and temperature, and negative anomalies of ozone between 12 and 15 km in altitude (247 to 121 hPa), originated from convectively active regions of TS Corentin and TC Enawo 1 d before the planned balloon launches according to the Lagrangian trajectories. Near the tropopause region, air masses on 25 January 2016 were anomalously dry around 100 hPa and were traced back to TS Corentin's active convective region where cirrus clouds and deep convective clouds may have dried the layer. An anomalously wet layer around 68 hPa was traced back to the southeast Indian Ocean where a monthly water vapor anomaly of 0.5 ppmv was observed. In contrast, no water vapor anomaly was found near or above the tropopause region on 3 March 2017 over Maïdo as the tropopause region was not downwind of TC Enawo. This study compares and contrasts the impact of two tropical cyclones on the humidification of the TTL over the SWIO. It also demonstrates the need for accurate balloon-borne measurements of water vapor, ozone and aerosols in regions where TTL in situ observations are sparse.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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