North Atlantic Free Troposphere Research Articles

Unravelling the transport of moisture into the Saharan Air Layer using passive tracers and isotopes

AbstractThe subtropical free troposphere plays a critical role in the radiative balance of the Earth. However, the complex interactions controlling moisture in this sensitive region and, in particular, the relative importance of long‐range transport compared to lower‐tropospheric mixing, remain unclear. This study uses the regional COSMO model equipped with stable water isotopes and passive water tracers to quantify the contributions of different evaporative sources to the moisture and its stable isotope signals in the eastern subtropical North Atlantic free troposphere. In summer, this region is characterized by two alternating large‐scale circulation regimes: (i) dry, isotopically depleted air from the upper‐level extratropics, and (ii) humid, enriched air advected from Northern Africa within the Saharan Air Layer (SAL) consisting of a mixture of moisture of diverse origin (tropical and extratropical North Atlantic, Africa, Europe, the Mediterranean). This diversity of moisture sources in regime (ii) arises from the convergent inflow at low levels of air from different neighbouring regions into the Saharan heat low (SHL), where it is mixed and injected by convective plumes into the large‐scale flow aloft, and thereafter expelled to the North Atlantic within the SAL. Remarkably, this regime is associated with a large contribution of moisture that evaporated from the North Atlantic, which makes a detour through the SHL and eventually reaches the 850–550 hPa layer above the Canaries. Moisture transport from Europe via the SHL to the same layer leads to the strongest enrichment in heavy isotopes (δ2H correlates most strongly with this tracer). The vertical profiles over the North Atlantic show increased humidity and δ2H and reduced static stability in the 850–550 hPa layer, and smaller cloud fraction in the boundary layer in regime (ii) compared to regime (i), highlighting the key role of moisture transport through the SHL in modulating the radiative balance in this region.

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

A 10-year characterization of the Saharan Air Layer lidar ratio in the subtropical North Atlantic

Abstract. Particle extinction-to-backscatter ratio (lidar ratio) is a key parameter for a correct interpretation of elastic lidar measurements. Of particular importance is the determination of the lidar ratio of the Saharan Air Layer mineral dust transported into the free troposphere over the North Atlantic region. The location of the two sun photometer stations managed by the Izaña Atmospheric Research Centre (IARC) on the island of Tenerife and a decade of available micropulse lidar (MPL) data allow us to determine the lidar ratio under almost pure-dust conditions. This result can be considered representative of the Saharan dust transported westward over the North Atlantic in the subtropical belt. Three different methods have been used to calculate the lidar ratio in this work: (1) using the inversion of sky radiance measurements from a sun–sky photometer installed at the Izaña Observatory (2373 m a.s.l.) under free-troposphere conditions; (2) the one-layer method, a joint determination using a micropulse lidar sited at the Santa Cruz de Tenerife sea-level station and photometric information considering one layer of aerosol characterized by a single lidar ratio; and (3) the two-layer method, a joint determination using the micropulse lidar and photometric information considering two layers of aerosol with two different lidar ratios. The one-layer method only uses data from a co-located photometer at Santa Cruz de Tenerife, while the two-layer conceptual approach incorporates photometric information at two heights from the observatories of Izaña and Santa Cruz de Tenerife. The almost pure-dust lidar ratio retrieval from the sun–sky photometer and from the two-layer method give similar results, with lidar ratios at 523 nm of 49 ± 6 and 50 ± 11 sr. These values obtained from a decade of data records are coincident with other studies in the literature reporting campaigns in the subtropical North Atlantic region. This result shows that the two-layer method is an improved conceptual approach compared to the single-layer approach, which matches the real lower-troposphere structure well. The two-layer method is able to retrieve reliable lidar ratios and therefore aerosol extinction profiles despite the inherent limitations of the elastic lidar technique. We found a lack of correlation between lidar ratio and Ångström exponent (α), which indicates that the dust lidar ratio can be considered independent of dust size distribution in this region. This finding suggests that dust is, under most atmospheric conditions, the predominant aerosol in the North Atlantic free troposphere, which is in agreement with previous studies conducted at the Izaña Observatory.

Description of the Baseline Surface Radiation Network (BSRN) station at the Izaña Observatory (2009–2017): measurements and quality control/assurance procedures

Abstract. The Baseline Surface Radiation Network (BSRN) was implemented by the World Climate Research Programme (WCRP) starting observations with nine stations in 1992, under the auspices of the World Meteorological Organization (WMO). Currently, 59 BSRN stations submit their data to the WCRP. One of these stations is the Izaña station (station IZA, no. 61) that enrolled in this network in 2009. This is a high-mountain station located in Tenerife (Canary Islands, Spain, at 28.3∘ N, 16.5∘ W; 2373 m a.s.l.) and is a representative site of the subtropical North Atlantic free troposphere. It contributes with basic-BSRN radiation measurements, such as global shortwave radiation (SWD), direct radiation (DIR), diffuse radiation (DIF) and longwave downward radiation (LWD), and extended-BSRN measurements, including ultraviolet ranges (UV-A and UV-B), shortwave upward radiation (SWU) and longwave upward radiation (LWU), and other ancillary measurements, such as vertical profiles of temperature, humidity and wind obtained from radiosonde profiles (WMO station no. 60018) and total column ozone from the Brewer spectrophotometer. The IZA measurements present high-quality standards since more than 98 % of the data are within the limits recommended by the BSRN. There is an excellent agreement in the comparison between SWD, DIR and DIF (instantaneous and daily) measurements with simulations obtained with the LibRadtran radiative transfer model. The root mean square error (RMSE) for SWD is 2.28 % for instantaneous values and 1.58 % for daily values, while the RMSE for DIR is 2.00 % for instantaneous values and 2.07 % for daily values. IZA is a unique station that provides very accurate solar radiation data in very contrasting scenarios: most of the time under pristine sky conditions and periodically under the effects of the Saharan air layer characterized by a high content of mineral dust. A detailed description of the BSRN program at IZA, including quality control and quality assurance activities, is given in this work.

Importance of the Saharan heat low in controlling the North Atlantic free tropospheric humidity budget deduced from IASI <i>δ</i>D observations

Abstract. The isotopic composition of water vapour in the North Atlantic free troposphere is investigated with Infrared Atmospheric Sounding Interferometer (IASI) measurements of the D ∕ H ratio (δD) above the ocean. We show that in the vicinity of West Africa, the seasonality of δD is particularly strong (130 ‰), which is related with the influence of the Saharan heat low (SHL) during summertime. The SHL indeed largely influences the dynamic in that region by producing deep turbulent mixing layers, yielding a specific water vapour isotopic footprint. The influence of the SHL on the isotopic budget is analysed on various time and space scales and is shown to be large, highlighting the importance of the SHL dynamics on the moistening and the HDO enrichment of the free troposphere over the North Atlantic. The potential influence of the SHL is also investigated on the inter-annual scale as we also report important variations in δD above the Canary archipelago region. We interpret the variability in the enrichment, using backward trajectory analyses, in terms of the ratio of air masses coming from the North Atlantic and air masses coming from the African continent. Finally, the interest of IASI high sampling capabilities is further illustrated by presenting spatial distributions of δD and humidity above the North Atlantic from which we show that the different sources and dehydration pathways controlling the humidity can be disentangled thanks to the added value of δD observations. More generally, our results demonstrate the utility of δD observations obtained from the IASI sounder to gain insight into the hydrological cycle processes in the West African region.

Speciation of organic aerosols in the Saharan Air Layer and in the free troposphere westerlies

Abstract. We focused this research on the composition of the organic aerosols transported in the two main airflows of the subtropical North Atlantic free troposphere: (i) the Saharan Air Layer – the warm, dry and dusty airstream that expands from North Africa to the Americas at subtropical and tropical latitudes – and (ii) the westerlies, which flow from North America over the North Atlantic at mid- and subtropical latitudes. We determined the inorganic compounds (secondary inorganic species and elemental composition), elemental carbon and the organic fraction (bulk organic carbon and organic speciation) present in the aerosol collected at Izaña Observatory, ∼ 2400 m a.s.l. on the island of Tenerife. The concentrations of all inorganic and almost all organic compounds were higher in the Saharan Air Layer than in the westerlies, with bulk organic matter concentrations within the range 0.02–4.0 µg m−3. In the Saharan Air Layer, the total aerosol population was by far dominated by dust (93 % of bulk mass), which was mixed with secondary inorganic pollutants ( < 5 %) and organic matter ( ∼ 1.5 %). The chemical speciation of the organic aerosols (levoglucosan, dicarboxylic acids, saccharides, n-alkanes, hopanes, polycyclic aromatic hydrocarbons and those formed after oxidation of α-pinene and isoprene, determined by gas chromatography coupled with mass spectrometry) accounted for 15 % of the bulk organic matter (determined by the thermo-optical transmission technique); the most abundant organic compounds were saccharides (associated with surface soils), secondary organic aerosols linked to oxidation of biogenic isoprene (SOA ISO) and dicarboxylic acids (linked to several primary sources and SOA). When the Saharan Air Layer shifted southward, Izaña was within the westerlies stream and organic matter accounted for ∼ 28 % of the bulk mass of aerosols. In the westerlies, the organic aerosol species determined accounted for 64 % of the bulk organic matter, with SOA ISO and dicarboxylic acids being the most abundant; the highest concentration of organic matter (3.6 µg m−3) and of some organic species (e.g. levoglucosan and some dicarboxylic acids) were associated with biomass burning linked to a fire in North America. In the Saharan Air Layer, the correlation found between SOA ISO and nitrate suggests a large-scale impact of enhancement of the formation rate of secondary organic aerosols due to interaction with anthropogenic NOx emissions.

Impact of North America on the aerosol composition in the North Atlantic free troposphere

Abstract. In the AEROATLAN project we study the composition of aerosols collected over ∼ 5 years at Izaña Observatory (located at ∼ 2400 m a.s.l. in Tenerife, the Canary Islands) under the prevailing westerly airflows typical of the North Atlantic free troposphere at subtropical latitudes and midlatitudes. Mass concentrations of sub-10 µm aerosols (PM10) carried by westerly winds to Izaña, after transatlantic transport, are typically within the range 1.2 and 4.2 µg m−3 (20th and 80th percentiles). The main contributors to background levels of aerosols (PM10 within the 1st–50th percentiles = 0.15–2.54 µg m−3) are North American dust (53 %), non-sea-salt sulfate (14 %) and organic matter (18 %). High PM10 events (75th–95th percentiles ≈ 4.0–9.0 µg m−3) are prompted by dust (56 %), organic matter (24 %) and non-sea-salt sulfate (9 %). These aerosol components experience a seasonal evolution explained by (i) their spatial distribution in North America and (ii) the seasonal shift of the North American outflow, which migrates from low latitudes in winter (∼ 32° N, January–March) to high latitudes in summer (∼ 52° N, August–September). The westerlies carry maximum loads of non-sea-salt sulfate, ammonium and organic matter in spring (March–May), of North American dust from midwinter to mid-spring (February–May) and of elemental carbon in summer (August–September). Our results suggest that a significant fraction of organic aerosols may be linked to sources other than combustion (e.g. biogenic); further studies are necessary for this topic. The present study suggests that long-term evolution of the aerosol composition in the North Atlantic free troposphere will be influenced by air quality policies and the use of soils (potential dust emitter) in North America.

Soluble iron dust export in the high altitude Saharan Air Layer

Every summer huge amounts of desert dust particles are exported from the hyperarid subtropical Sahara to the North Atlantic the so-called Saharan Air Layer (SAL), a dry, warm and dust-laden corridor that expands from the North African coast (1–5 km.a.s.l.) to the Americas above the marine boundary layer. Because of the potential impact of the dust deposited on the ocean on marine biogeochemistry and climate, we studied the Fe solubility (in seawater) of atmospheric aerosols samples directly collected in the SAL off the North African coast, i.e. the fresh aerosols recently exported from the Sahara in the SAL. The aerosol sampling was performed at ∼2400 m.a.s.l. in Izaña observatory in Tenerife island. In the total aerosols, we found low Fe concentrations and high fractional Fe solubility (FFS ∼2%) in the North Atlantic free troposphere airflows and high Fe concentrations and low FFS (∼0.7%) within the SAL; the resulting FFS versus total dust (or total Fe) plot shows a hyperbolic trend attributed to the conservative mixing of ‘fine combustion aerosols’ and ‘lithogenic mineral dust’. We then focused on the soluble Fe in the SAL. Our results indicate that ∼70% of soluble Fe is associated with the dissolution of submicron dust particles, probably involving Fe-bearing clays. We found a FFS of submicron dust (∼6%) higher than that typically observed in submicron particles of soil dust samples (<1%). The correlation between FFS and the ammonium-sulphate/dust ratio and the low variability in the Fe/Al ratio in the dust samples, suggests that the increase in the FFS of submicron dust aerosols (with respect to soil dust particles) may be related to the presence of acid pollutants mixed with dust. Previous studies had focused on dust processing and changes of Fe solubility during the trans-Atlantic transport of dust in the SAL. We found that submicron dust exported off the coast of North Africa may have already experienced acid processing over the Sahara, i.e. before dust export to the Atlantic. Export of soluble submicron Fe dust and deposition of coarse and depleted in soluble Fe dust particles during the trans-Atlantic transport may account for the observed variability in dust, soluble Fe and FFS.

Assessment of atmospheric processes driving ozone variations in the subtropical North Atlantic free troposphere

Abstract. An analysis of the 22-yr ozone (O3) series (1988–2009) at the subtropical high mountain Izaña~station (IZO; 2373 m a.s.l.), representative of free troposphere (FT) conditions, is presented. Diurnal and seasonal O3 variations as well as the O3 trend (0.19 ± 0.05 % yr−1 or 0.09 ppbv yr−1), are assessed. A climatology of O3 transport pathways using backward trajectories shows that higher O3 values are associated with air masses travelling above 4 km altitude from North America and North Atlantic Ocean, while low O3 is transported from the Saharan continental boundary layer (CBL). O3 data have been compared with PM10, 210Pb, 7Be, potential vorticity (PV) and carbon monoxide (CO). A clear negative logarithmic relationship was observed between PM10 and surface O3 for all seasons. A similar relationship was found between O3 and 210Pb. The highest daily O3 values (90th percentile) are observed in spring and in the first half of summer time. A positive correlation between O3 and PV, and between O3 and 7Be is found throughout the year, indicating that relatively high surface O3 values at IZO originate from the middle and upper troposphere. We find a good correlation between O3 and CO in winter, supporting the hypothesis of long-range transport of photochemically generated O3 from North America. Aged air masses, in combination with sporadic inputs from the upper troposphere, are observed in spring, summer and autumn. In summer time high O3 values seem to be the result of stratosphere-to-troposphere (STT) exchange processes in regions neighbouring the Canary Islands. Since 1995–1996, the North Atlantic Oscillation has changed from a predominantly high positive phase to alternating between negative, neutral or positive phases. This change results in an increased flow of the westerlies in the mid-latitude and subtropical North Atlantic, thus favouring the transport of O3 and its precursors from North America, and a higher frequency of storms over North Atlantic, with a likely higher incidence of STT processes in mid-latitudes. These processes lead to an increase of tropospheric O3 in the subtropical North Atlantic region after 1996 that has been reflected in surface O3 records at IZO.

Transport of desert dust mixed with North African industrial pollutants in the subtropical Saharan Air Layer

Abstract. An analysis of chemical composition data of particulate matter samples (TSP, PM10 and PM2.5) collected from 2002 to 2008 in the North Atlantic free troposphere at the Izaña Global Atmospheric Watch (GAW) observatory (Tenerife, Canary Islands) shows that desert dust is very frequently mixed with particulate pollutants in the Saharan Air Layer (SAL). The study of this data set with Median Concentrations At Receptor (MCAR) plots allowed the identification of the potential source regions of the dust and particulate pollutants. Areas located at the south of the southern slope of the Atlas mountains emerge as the most frequent source of the soil desert dust advected to the northern edge of the SAL in summer. Industrial emissions occurring in Northern Algeria, Eastern Algeria, Tunisia and the Atlantic coast of Morocco appear as the most important source of the nitrate, ammonium and a fraction of sulphate (at least 60 % of the sulphate &lt;10 μm transported from some regions) observed in the SAL. These emissions are mostly linked to crude oil refineries, phosphate-based fertilizer industry and power plants. Although desert dust emissions appear as the most frequent source of the phosphorous observed in the SAL, high P concentrations are observed when the SAL is affected by emissions from open mines of phosphate and phosphate based fertilizer industry. The results also show that a significant fraction of the sulphate (up to 90 % of sulphate &lt;10 μm transported from some regions) observed in the SAL may be influenced by soil emissions of evaporite minerals in well defined regions where dry saline lakes (chotts) are present. These interpretations of the MCAR plots are consistent with the results obtained with the Positive Matrix Factorization (PMF2) receptor modelling. The results of this study show that North African industrial pollutants may be mixed with desert dust and exported to the North Atlantic in the Saharan Air Layer.

Measurements of aerosol optical depth above 3570 m asl in the North Atlantic free troposphere: results from ACE-2

As part of the 2nd Aerosol Characterisation Experiment (ACE-2), conducted during summer 1997 in the North Atlantic region between the Canary Islands and Portugal, we measured aerosol optical depths (AOD) at a mid-tropospheric site, near the top of the volcanic mountain “El Teide”(28°16′N, 16°36′ W, 3570 m asl). Our instrument was located at the highest altitude in a network of sunphotometers that extended down to sea level. Clear conditions dominated the ACE-2 period, and, although suggested by back-trajectories at 300 hPa, no evidence of anthropogenic pollution was found in our data. Three distinct dust episodes were observed. Vertical soundings and back trajectories suggested mineral dust from the Sahel region as a source. During these episodes, AOD increased an order of magnitude with respect to background conditions (from 0.017 up to 0.19 at λ=500 nm). A shift towards neutrality of the extinction spectral dependence (Angstrom exponent α down to 0.13), indicated that the coarse mode (particle diameter >2 μm) dominated the aerosol size distribution. For 6 days during the episodes of mineral dust, a monomodal size distribution between 2 and 20 μm diameter was obtained from Mie based size distribution calculations. Estimates, at 500 nm, of the single scattering albedo ω0(0.87–0.96), and the aerosol asymmetry parameter g(0.72–0.73) suggest that the dust layer causes a net cooling forcing at the top of the atmosphere.

OH and HO2 chemistry in the North Atlantic free troposphere

Interactions between atmospheric hydrogen oxides and aircraft nitrogen oxides determine the impact of aircraft exhaust on atmospheric chemistry. To study these interactions, the Subsonic Assessment: Ozone and Nitrogen Oxide Experiment (SONEX) assembled the most complete measurement complement to date for studying HOx (OH and HO2) chemistry in the free troposphere. Observed and modeled HOx agree on average to within experimental uncertainties (±40%). However, significant discrepancies occur as a function of NO and at solar zenith angles &gt;70°. Some discrepancies appear to be removed by model adjustments to HOx‐NOx chemistry, particularly by reducing HO2NO2 (PNA) and by including heterogeneous reactions on aerosols and cirrus clouds.