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Mineral dust in Central Asia: Combining lidar and other measurements during the Central Asian dust experiment (CADEX)
Mineral dust needs to be characterized comprehensively since it contributes to the climate change in Tajikistan / Central Asia. Lidar results from the measurements of mineral dust during CADEX are compared with results of sun photometer measurements, satellite-based measurements, and chemical analysis of ground samples. Although the dust is often advected from far-range sources, it impacts on the local conditions considerably.
Long-term profiling of mineral dust and pollution aerosol with multiwavelength polarization Raman lidar at the Central Asian site of Dushanbe, Tajikistan: Case studies
For the first time, continuous vertically resolved aerosol measurements were performed by lidar in Tajikistan, Central Asia. Observations with the multiwavelength polarization Raman lidar PollyXT were conducted during CADEX (Central Asian Dust EXperiment) in Dushanbe, Tajikistan, from March 2015 to August 2016. Co-located with the lidar, a sun photometer was also operated. The goal of CADEX is to provide an unprecedented data set on vertically resolved aerosol optical properties in Central Asia, an area highly affected by climate change but largely missing vertically resolved aerosol measurements. During the 18-month measurement campaign, mineral dust was detected frequently from ground to the cirrus level height. In this study, an overview of the measurement period is given and four typical but different example measurement cases are discussed in detail. Three of them are dust cases and one is a contrasting pollution aerosol case. Vertical profiles of the measured optical properties and the calculated dust and non-dust mass concentrations are presented. Dust source regions were identified by means of backward trajectory analyses. A lofted layer of Middle Eastern dust with an aerosol optical thickness (AOT) of 0.4 and an extinction-related Ångström exponent of 0.41 was measured. In comparison, two near-ground dust cases have Central Asian sources. One is an extreme dust event with an AOT of 1.5 and Ångström exponent of 0.12 and the other one is a most extreme dust event with an AOT of above 4 (measured by sun photometer) and an Ångström exponent of −0.08. The observed lidar ratios (and particle linear depolarization ratios) in the presented dust cases range from 40.3 to 46.9sr (and 0.18–0.29) at 355nm and from 35.7 to 42.9sr (0.31–0.35) at 532nm wavelength. The particle linear depolarization ratios indicate almost unpolluted dust in the case of a lofted dust layer and pure dust in the near-ground dust cases. The lidar ratio values are lower than typical lidar ratio values for Saharan dust (50–60sr) and comparable to Middle Eastern or west-Asian dust lidar ratios (35–45sr). In contrast, the presented case of pollution aerosol of local origin has an Ångström exponent of 2.07 and a lidar ratio (particle linear depolarization ratio) of 55.8sr (0.03) at 355nm and 32.8sr (0.08) at 532nm wavelength.
Composition of ice particle residuals in mixed-phase clouds at Jungfraujoch (Switzerland): Enrichment and depletion of particle groups relative to total aerosol
Ice particle residuals (IRs) and the total aerosol particle population were sampled in parallel during mixed-phase cloud events at the high-altitude research station Jungfraujoch in January-February 2017. Particles were sampled behind an ice-selective counterflow impactor (Ice-CVI) for IRs and a heated total inlet for the total aerosol particles. A dilution set-up was used to collect total particles with the same sampling duration as for IRs to prevent overloading of the substrates. About 4000 particles from 10 Ice-CVI samples (from 7 days of cloud events at temperatures at the site between g-10 and g-18°C) were analysed and classified with operator-controlled scanning electron microscopy. Contamination particles (identified by their chemical composition), most likely originating from abrasion in the Ice-CVI and collection of secondary ice, were excluded from further analysis. Approximately 3000 total aerosol particles (IRs and interstitial particles) from 5 days in clouds were also analysed. Enrichment and depletion of the different particle groups (within the IR fraction relative to the total aerosol reservoir) are presented as an odds ratio relative to alumosilicate (particles only consisting of Al, Si, and O), which was chosen as reference due to the large enrichment of this group relative to total aerosol and the relatively high number concentration of this group in both total aerosol and the IR samples. Complex secondary particles and soot are the major particle groups in the total aerosol samples but are not found in the IR fraction and are hence strongly depleted. C-rich particles (most likely organic particles) showed a smaller enrichment compared to aluminosilicates by a factor of ∼ 20. The particle groups with enrichment similar to aluminosilicate are silica, Fe aluminosilicates, Ca-rich particles, Ca sulfates, sea-salt-containing particles, and metal/metal oxide. Other aluminosilicates-consisting of variable amounts of Na, K, Ca, Si, Al, O, Ti, and Fe-are somewhat more enriched (factor ∼ 2) and Pb-rich particles are more (factor ∼ 8) enriched than aluminosilicates. None of the sampled IR groups showed a temperature or size dependence in respect to ice activity, which might be due to the limited sampling temperature interval and the similar size of the particles. Footprint plots and wind roses could explain the different total aerosol composition in one sample (carbonaceous particle emission from the urban/industrial area of Po Valley), but this did not affect the IR composition. Taking into account the relative abundance of the particle groups in total aerosol and the ice nucleation ability, we found that silica, aluminosilicates, and other aluminosilicates were the most important ice particle residuals at Jungfraujoch during the mixed-phase cloud events in winter 2017.
Thermal IR radiative properties of mixed mineral dust and biomass aerosol during SAMUM-2
Ground-based high spectral resolution measurements of downwelling radiances from 800 to 1200 cm−1 were conducted between 20 January and 6 February 2008 within the scope of the SAMUM-2 field experiment. We infer the spectral signature of mixed biomass burning/mineral dust aerosols at the surface from these measurements and at top of the atmosphere from IASI observations. In a case study for a day characterized by the presence of high loads of both dust and biomass we attempt a closure with radiative transfer simulations assuming spherical particles. A detailed sensitivity analysis is performed to investigate the effect of uncertainties in the measurements ingested into the simulation on the simulated radiances. Distinct deviations between modelled and observed radiances are limited to a spectral region characterized by resonance bands in the refractive index. A comparison with results obtained during recent laboratory studies and field experiments reveals, that the deviations could be caused by the aerosol particles’ non-sphericity, although an unequivocal discrimination from measurement uncertainties is not possible. Based on radiative transfer simulations we estimate the aerosol’s direct radiative effect in the atmospheric window region to be 8 W m−2 at the surface and 1 W m−2 at top of the atmosphere.
New particle formation and sub-10nm size distribution measurements during the A-LIFE field experiment in Paphos, Cyprus
Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMAtrain) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 μ m was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMAtrain, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (< 10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements. © 2020 Author(s).
Dry versus wet marine particle optical properties: RH dependence of depolarization ratio, backscatter, and extinction from multiwavelength lidar measurements during SALTRACE
Triple-wavelength lidar observations of the depolarization ratio and the backscatter coefficient of marine aerosol as a function of relative humidity (RH) are presented with a 5min time resolution. The measurements were performed at Barbados (13°N, 59°W) during the Saharan Aerosol Long-range Transport and Aerosol-Cloud interaction Experiment (SALTRACE) winter campaign in February 2014. The phase transition from spherical sea salt particles to cubic-like sea salt crystals was observed with a polarization lidar. The radiosonde and water-vapor Raman lidar observations show a drop in RH below 50% in the marine aerosol layer simultaneously with a strong increase in particle linear depolarization ratio, which reaches values up to 0.12±0.08 (at 355nm), 0.15±0.03 (at 532nm), and 0.10±0.01 (at 1064nm). The lidar ratio (extinction-to-backscatter ratio) increased from 19 and 23sr for spherical sea salt particles to 27 and 25sr (at 355 and 532nm, respectively) for cubic-like particle ensembles. Furthermore the scattering enhancement due to hygroscopic growth of the marine aerosol particles under atmospheric conditions was measured. Extinction enhancement factors from 40 to 80% RH of 1.94±0.94 at 355nm, 3.70±1.14 at 532nm, and 5.37±1.66 at 1064nm were found. The enhanced depolarization ratios and lidar ratios were compared to modeling studies of cubic sea salt particles.
In situ aerosol characterization at Cape Verde, Part 1: Particle number size distributions, hygroscopic growth and state of mixing of the marine and Saharan dust aerosol
Particle number size distributions and hygroscopic properties of marine and Saharan dust aerosol were investigated during the SAMUM-2 field study at Cape Verde in winter 2008. Aitken and accumulation mode particles were mainly assigned to the marine aerosol, whereas coarse mode particles were composed of sea-salt and a variable fraction of Saharan mineral dust. A new methodical approach was used to derive hygroscopic growth and state of mixing for a particle size range (volume equivalent) from dpve = 26 nm to 10 μm. For hygroscopic particles with dpve < 100 nm, the median hygroscopicity parameter κ is 0.35. From 100 nm < dpve < 350 nm, κ increases to 0.65. For larger particles, κ at dpve = 350 nm was used. For nearly hydrophobic particles, κ is between 0 and 0.1 for dpve < 250 nm and decreases to 0 for dpve > 250 nm. The mixing state of Saharan dust in terms of the number fraction of nearly hydrophobic particles showed the highest variation and ranges from 0.3 to almost 1. This study was used to perform a successful mass closure at ambient conditions and demonstrates the important role of hygroscopic growth of large sea-salt particles.
Differences and Similarities of Central Asian, African, and Arctic Dust Composition from a Single Particle Perspective
Mineral dust composition affects a multitude of processes in the atmosphere and adjacent compartments. Dust dry deposition was collected near source in northwest Africa, in Central Asia, and on Svalbard and at three locations of the African outflow regime. Samples were subjected to automated scanning electron microscopy with energy-dispersive X-ray analysis to obtain size and composition of 216,000 individual particles. Results show low temporal variation in estimated optical properties for each location, but considerable differences between the African, Central Asian, and Arctic regimes. No significant difference was found between the K-feldspar relative abundances, indicating comparable related ice-nucleation abilities. The mixing state between calcium and iron compounds was different for near source and transport regimes, potentially in part due to size sorting effects. As a result, in certain situations (high acid availability, limited time) atmospheric processing of the dust is expected to lead to less increased iron solubility for near-source dusts (in particular for Central Asian ones) than for transported ones (in particular of Sahelian origin). © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
Properties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic
Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.
Modelling lidar-relevant optical properties of complex mineral dust aerosols
We model lidar-relevant optical properties of mineral dust aerosols and compare the modelling results with optical properties derived from lidar measurements during the SAMUM field campaigns. The Discrete Dipole Approximation is used for optical modelling of single particles. For modelling of ensemble properties, the desert aerosol type of the OPAC aerosol dataset is extended by mixtures of absorbing and non-absorbing irregularly shaped mineral dust particles. Absorbing and non-absorbing particles are mixed to mimic the natural mineralogical inhomogeneity of dust particles. A sensitivity study reveals that the mineralogical inhomogeneity is critical for the lidar ratio at short wavelengths; it has to be considered for agreement with the observed wavelength dependence of the lidar ratio. The amount of particles with low aspect ratios (about 1.4 and lower) affects the lidar ratio at any lidar wavelength; their amount has to be low for agreement with SAMUM observations. Irregularly shaped dust particles with typical refractive indices, in general, have higher linear depolarization ratios than corresponding spheroids, and improve the agreement with the observations.