Properties of dust aerosol particles transported to Portugal from the Sahara desert

Aerosol properties of mineral particles in the far field of an African desert dust outbreak were investigated that brought Saharan dust over the Mediterranean in different layers to Portugal. The measurements were performed inside the project Desert Aerosols over Portugal (DARPO) which was linked to the Saharan Mineral Dust Experiment (SAMUM). The maximum particle mass concentration was about 150 μg m⁻³ and the corresponding scattering coefficient was 130 M m⁻¹ which results in a mass scattering efficiency of 0.87 m² g⁻¹. The aerosol optical depth reached values up to 0.53 and the lidar ratio was between 45 and 50 in the whole dust loaded column. A comparison between particle size distributions and refractive indices derived from different instruments and models showed a general good agreement but some minor differences could also be observed. Measurements as well as calculations with a particle transport model suggest that there is a relatively higher concentration of very large particles in the upper region of the dust layer than on the surface which is likely connected with meteorological conditions at the observational site (Évora, Portugal).     

Evolution of boundary‐layer aerosol particles due to in‐cloud chemical reactions during the 2nd Lagrangian experiment of ACE‐2

The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO₂ concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO₂ to sulphate aerosol. The modelled SO₂ concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH₃ and HCl gas were also found to play an important rôle in cloud processing in the model.     

State of mixing, shape factor, number size distribution, and hygroscopic growth of the Saharan anthropogenic and mineral dust aerosol at Tinfou, Morocco

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May and June 2006 in Tinfou, Morocco. A H-TDMA system and a H-DMA-APS system were used to obtain hygroscopic properties of mineral dust particles at 85% RH. Dynamic shape factors of 1.11, 1.19 and 1.25 were determined for the volume equivalent diameters 720, 840 and 960 nm, respectively.
During a dust event, the hydrophobic number fraction of 250 and 350 nm particles increased significantly from 30 and 65% to 53 and 75%, respectively, indicating that mineral dust particles can be as small as 200 nm in diameter. Log-normal functions for mineral dust number size distributions were obtained from total particle number size distributions and fractions of hydrophobic particles. The geometric mean diameter for Saharan dust particles was 715 nm during the dust event and 570 nm for the Saharan background aerosol.
Measurements of hygroscopic growth showed that the Saharan aerosol consists of an anthropogenic fraction (predominantly non natural sulphate and carbonaceous particles) and of mineral dust particles. Hygroscopic growth and hysteresis curve measurements of the 'more' hygroscopic particle fraction indicated ammonium sulphate as a main component of the anthropogenic aerosol. Particles larger than 720 nm in diameter were completely hydrophobic meaning that mineral dust particles are not hygroscopic.     

Aircraft study of aerosol vertical distributions over Beijing and their optical properties

A set of 152 vertical profiles of aerosol number concentration and size distribution with diameter ranging from 0.12 to 3.0 μm observed by the airborne optical spectrometer probe in Beijing, China, between February 2005 and September 2006 is analysed and discussed. The statistic of aerosol number concentration ( N _a) reveals a high aerosol number density in this region with average surface level number concentration ( N ₀) of about 6600 cm⁻³ (0.12–3.0 μm). The average vertical profile of N _a approximately satisfies an exponential decline function with a scale height of 1419 m. The N _a profiles are influenced by the structures of planetary boundary layer (PBL) significantly and two typical types of N _a profile under different conditions of PBL are presented and parametrized in this study. The observations of aerosol size distribution show that, in most cases the aerosol size distributions are not very sensitive to altitude, with effective radii ranging from 0.16 to 0.28 μm. Comparison between aircraft-derived aerosol optical depth (AOD) and Moderate Resolution Imaging Spectroradiometer-derived AOD shows good agreement. The Mie model calculations suggest that the surface level number concentration, the PBL height and the structure of PBL can influence the AOD significantly.     

Spectral absorption coefficients and imaginary parts of refractive indices of Saharan dust during SAMUM-1

During the SAMUM-1 experiment, absorption coefficients and imaginary parts of refractive indices of mineral dust particles were investigated in southern Morocco. Main absorbing constituents of airborne samples were identified to be iron oxide and soot. Spectral absorption coefficients were measured using a spectral optical absorption photometer (SOAP) in the wavelength range from 300 to 800 nm with a resolution of 50 nm. A new method that accounts for a loading-dependent correction of fibre filter based absorption photometers, was developed. The imaginary part of the refractive index was determined using Mie calculations from 350 to 800 nm. The spectral absorption coefficient allowed a separation between dust and soot absorption. A correlation analysis showed that the dust absorption coefficient is correlated ( R ² up to 0.55) with the particle number concentration for particle diameters larger than 0.5 μm, whereas the coefficient of determination R ² for smaller particles is below 0.1. Refractive indices were derived for both the total aerosol and a dust aerosol that was corrected for soot absorption. Average imaginary parts of refractive indices of the entire aerosol are 7.4 × 10⁻³, 3.4 × 10⁻³ and 2.0 × 10⁻³ at wavelengths of 450, 550 and 650 nm. After a correction for the soot absorption, imaginary parts of refractive indices are 5.1 × 10⁻³, 1.6 × 10⁻³ and 4.5 × 10⁻⁴.     

Spectral surface albedo over Morocco and its impact on radiative forcing of Saharan dust

In May–June 2006, airborne and ground-based solar (0.3–2.2 μm) and thermal infrared (4–42 μm) radiation measurements have been performed in Morocco within the Saharan Mineral Dust Experiment (SAMUM). Upwelling and downwelling solar irradiances have been measured using the Spectral Modular Airborne Radiation Measurement System (SMART)-Albedometer. With these data, the areal spectral surface albedo for typical surface types in southeastern Morocco was derived from airborne measurements for the first time. The results are compared to the surface albedo retrieved from collocated satellite measurements, and partly considerable deviations are observed. Using measured surface and atmospheric properties, the spectral and broad-band dust radiative forcing at top-of-atmosphere (TOA) and at the surface has been estimated. The impact of the surface albedo on the solar radiative forcing of Saharan dust is quantified. In the SAMUM case of 19 May 2006, TOA solar radiative forcing varies by 12 W m⁻² per 0.1 surface-albedo change. For the thermal infrared component, values of up to +22 W m⁻² were derived. The net (solar plus thermal infrared) TOA radiative forcing varies between −19 and +24 W m⁻² for a broad-band solar surface albedo of 0.0 and 0.32, respectively. Over the bright surface of southeastern Morocco, the Saharan dust always has a net warming effect.     

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

As part of the 2nd A erosol C haracterisation E xperiment (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 (Ångstrom 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.     

Desert dust aerosol air mass mapping in the western Sahara, using particle properties derived from space-based multi-angle imaging

Coincident observations made over the Moroccan desert during the Sahara mineral dust experiment (SAMUM) 2006 field campaign are used both to validate aerosol amount and type retrieved from multi-angle imaging spectroradiometer (MISR) observations, and to place the suborbital aerosol measurements into the satellite's larger regional context. On three moderately dusty days during which coincident observations were made, MISR mid-visible aerosol optical thickness (AOT) agrees with field measurements point-by-point to within 0.05–0.1. This is about as well as can be expected given spatial sampling differences; the space-based observations capture AOT trends and variability over an extended region. The field data also validate MISR's ability to distinguish and to map aerosol air masses, from the combination of retrieved constraints on particle size, shape and single-scattering albedo. For the three study days, the satellite observations (1) highlight regional gradients in the mix of dust and background spherical particles, (2) identify a dust plume most likely part of a density flow and (3) show an aerosol air mass containing a higher proportion of small, spherical particles than the surroundings, that appears to be aerosol pollution transported from several thousand kilometres away.     

Numerical simulations of optical properties of Saharan dust aerosols with emphasis on lidar applications

In the framework of the Saharan Mineral Dust Experiment (SAMUM) for the first time the spectral dependence of particle linear depolarization ratios was measured by combining four lidar systems. In this paper these measurements are compared with results from scattering theory based on the T-matrix method. For this purpose, in situ measurements—size distribution, shape distribution and refractive index—were used as input parameters; particle shape was approximated by spheroids. A sensitivity study showed that lidar-related parameters—lidar ratio   S _p   and linear depolarization ratio  δ _p   —are very sensitive to changes of all parameters. The simulated values of the  δ _p   are in the range of 20% and 31% and thus in the range of the measurements. The spectral dependence is weak, so that it could not be resolved by the measurements. Calculated lidar ratios based on the measured microphysics and considering equivalent radii up to 7.5 μm show a range of possible values between 29 and 50 sr at  λ= 532 nm  . Larger   S _p   might be possible if the real part of the refractive index is small and the imaginary part is large. A strict validation was however not possible as too many microphysical parameters influence   S _p   and  δ _p   that could not be measured with the required accuracy.     

Broadband extinction method to determine atmospheric aerosol optical properties

The equivalent wavelength ( λ _E), at which the aerosol optical depth (AOD) is equal to broadband AOD (BAOD), can change in a wide range from 0.619 μm to 1.575 μm in the usual aerosol conditions. By using the least squares technique and some empirical corrections, a parameterized relationship of λ _E with BAOD, Ångström wavelength exponent ( α ), solar zenith angle ( θ ₀) and H₂O amount is developed. Using this relationship, and based on the strong sensitivity of BAOD on θ ₀ when θ ₀>70°, the broadband extinction method to derive the spectral AOD and α is further proposed. As shown in comparative simulations to retrieve AOD by the present, Molineaux et al. and Gueymard methods, the present method has the best accuracy in most simulations using Junge, MODTRAN, log‐normal and Deirmendjian aerosol models. A key question of the pyrheliometer method to determine wavelength-dependent AODs is the effect of uncertainty in the aerosol size istribution. It is found that the AOD solution around λ _E is less sensitive to the uncertainty. The wavelength exponent α is derived using an assumption of the stable atmospheric turbidity. If the pyrheliometer data from θ ₀=85° to 70° are used and the change of the turbidity is ±10%, the error of solution α is usually within ±0.32. If the variation of the turbidity is random, the mean value of a lot of the measurements of α would be very reasonable.     

Saharan dust absorption and refractive index from aircraft-based observations during SAMUM 2006

During the Saharan Mineral Dust Experiment (SAMUM) conducted in summer 2006 in southeast Morocco, the complex refractive index of desert dust was determined from airborne measurements of particle size distributions and aerosol absorption coefficients at three different wavelengths in the blue (467 nm), green (530 nm) and red (660 nm) spectral regions. The vertical structure of the dust layers was analysed by an airborne high spectral resolution lidar (HSRL). The origin of the investigated dust layers was estimated from trajectory analyses, combined with Meteosat 2nd Generation (MSG) scenes and wind field data analyses. The real part n of the dust refractive index was found almost constant with values between 1.55 and 1.56, independent of the wavelength. The values of the imaginary part k varied between the blue and red spectral regions by a factor of three to ten depending on the dust source region. Absolute values of k ranged from 3.1 × 10⁻³ to 5.2 × 10⁻³ at 450 nm and from 0.3 × 10⁻³ to 2.5 × 10⁻³ at 700 nm. Groupings of k values could be attributed to different source regions.     

Aerosol monitoring at multiple locations in China: contributions of EC and dust to aerosol light absorption

This paper reports on the analysis of 24-h aerosol data measured during 2006, at 14 monitoring sites in China. Measurements included seven-wavelength Aethalometers, thermal/optical reflectance analyses of filter samples and determination of dust aerosols. Black (elemental) carbon (BC, EC) is found to be the principal light-absorbing aerosol over many parts of China; however, the fraction of apparent light absorption attributed to dust varied from 14% in winter, to 11% in spring, to 5% in summer to 9% in autumn. Aerosol light absorption in urban areas was larger than in rural areas by factors of 2.4 in winter, 3.1 in spring and 2.5 in both summer and autumn. These differences may lead to contrasts in radiative, thermal and cloud modification effects between urban and rural areas. Absorption 'hotspots' were located in the Sichuan Basin, the provinces south of Beijing, the Pearl Delta River regions and the Guanzhong Plain. The mass absorption coefficient for aerosol BC (σ_BC) based on Aethalometer data is estimated to be 11.7 m² g⁻¹ at 880 nm wavelength (λ) with inverse (λ⁻¹) wavelength scaling, whereas the mass absorption coefficient for dust (σ_dust) is 1.3 m² g⁻¹ on average without significant wavelength dependence.     

Vertical profiling of convective dust plumes in southern Morocco during SAMUM

Lifting of dust particles by dust devils and convective plumes may significantly contribute to the global mineral dust budget. During the Saharan Mineral Dust Experiment (SAMUM) in May–June 2006 vertical profiling of dusty plumes was performed for the first time. Polarization lidar observations taken at Ouarzazate (30.9°N, 6.9°W, 1133 m height above sea level) are analyzed. Two cases with typical and vigorous formation of convective plumes and statistical results of 5 d are discussed. The majority of observed convective plumes have diameters on order of 100–400 m. Most of the plumes (typically 50–95%) show top heights <1 km or 0.3DLH with the Saharan dust layer height DLH of typically 3–4 km. Height-to-diameter ratio is mostly 2–10. Maximum plume top height ranges from 1.1 to 2.9 km on the 5 d. 5–26 isolated plumes and clusters of plumes per hour were detected. A low dust optical depth (<0.3) favours plume evolution. Observed surface, 1 and 2–m air temperatures indicate that a difference of 17–20 K between surface and 2-m air temperature and of 0.9–1 K between the 1 and 2-m temperatures are required before convective plumes develop. Favourable horizontal wind speeds are 2–7 m s⁻¹.     

基于Grimm180粒子仪对塔克拉玛干沙漠沙尘暴的定量观测

为了得到沙尘粒子和沙尘质量浓度的实时定量特征,利用Grimm180粒子仪在塔克拉玛干沙漠对沙尘暴进行了实时观测。通过分析Grimm180粒子仪在2018年5月20日和24日两次沙尘暴过程观测的数据得到:在浮尘、扬沙和沙尘暴期间,PM_2.5的质量浓度值随时间变化不大,一般PM_2.5浓度值<1500μg·m^-3,而PM₁₀在不同阶段的变化比较明显,数值在2000~6000μg·m^-3。沙尘粒子谱和沙尘质量浓度谱的分布形状在浮尘、扬沙和沙尘暴基本相同,当粒子直径>0.35μm时,粒子数浓度随直径的增大近似符合M-P分布。从浮尘到扬沙再到沙尘暴,小粒子区(D≤1μm)的占比越来越小,而中粒子区(1μm10μm)的粒子数越来越多并且占比越来越大。当粒子直径为0.35μm左右时,粒子数浓度达到最大值;当粒子直径在25~32μm时,沙尘质量浓度的值最大。在浮尘和扬沙阶段,PM_2.5/PM₁₀>25%;每分钟1 L体积内的沙尘粒子总数大约是4×10⁵,最大沙尘质量浓度<20μg·L^-1。在沙尘暴阶段,PM_2.5/PM₁₀<15%;每分钟1 L体积内的沙尘粒子总数>5×10⁵,最大沙尘质量浓度>25μg·L^-1。这些结论为准确地分析沙尘暴的定量特征提供了科学依据。     

Vertical profiling of Saharan dust with Raman lidars and airborne HSRL in southern Morocco during SAMUM

Three ground-based Raman lidars and an airborne high-spectral-resolution lidar (HSRL) were operated during SAMUM 2006 in southern Morocco to measure height profiles of the volume extinction coefficient, the extinction-to-backscatter ratio and the depolarization ratio of dust particles in the Saharan dust layer at several wavelengths. Aerosol Robotic Network (AERONET) Sun photometer observations and radiosoundings of meteorological parameters complemented the ground-based activities at the SAMUM station of Ouarzazate. Four case studies are presented. Two case studies deal with the comparison of observations of the three ground-based lidars during a heavy dust outbreak and of the ground-based lidars with the airborne lidar. Two further cases show profile observations during satellite overpasses on 19 May and 4 June 2006. The height resolved statistical analysis reveals that the dust layer top typically reaches 4–6 km height above sea level (a.s.l.), sometimes even 7 km a.s.l.. Usually, a vertically inhomogeneous dust plume with internal dust layers was observed in the morning before the evolution of the boundary layer started. The Saharan dust layer was well mixed in the early evening. The 500 nm dust optical depth ranged from 0.2–0.8 at the field site south of the High Atlas mountains, Ångström exponents derived from photometer and lidar data were between 0–0.4. The volume extinction coefficients (355, 532 nm) varied from 30–300 Mm⁻¹ with a mean value of 100 Mm⁻¹ in the lowest 4 km a.s.l.. On average, extinction-to-backscatter ratios of 53–55 sr (±7–13 sr) were obtained at 355, 532 and 1064 nm.     

Modelling dust distributions in the atmospheric boundary layer on Mars

A time and height dependent eddy diffusion model is used to investigate possible scenarios for the size distribution of dust in the lower atmosphere of Mars. The dust is assumed to either have been advected from a distant source or to have originated locally. In the former case, the atmosphere is assumed to initially contain dust particles with sizes following a modified gamma distribution. Larger particles are deposited relatively rapidly while small particles are well mixed up to the maximum height of the afternoon boundary layer and are deposited more slowly. In other cases, a parameterization of the dust source at the surface is proposed. Model results show that smaller particles are rapidly mixed within the Martian boundary layer, while larger particles (r > 10 μm) are concentrated near the ground with a stronger diurnal cycle. In all simulations we assume that the initial concentration or surface source depend on a modified gamma function distribution. For small particles (cross- sectional area weighted mean radius, r_eff = 1.6 μm) distributions retain essentially the same form, though with variations in the mean and variance of the area-weighted radius, and the gamma function can be used to represent the particle size distribution reasonably well at most heights within the boundary layer. In the case of a surface source of larger particles (mean radius 50 μm) the modified gamma function does not fit the resulting particle size distribution. All results are normalised by a scaling factor that can be adjusted to correspond to an optical depth for assumed particle optical scattering properties.     

Spectral aerosol optical depth characterization of desert dust during SAMUM 2006

The aerosol optical depth (AOD) in the range 340–1550 nm was monitored at Ouarzazate (Morocco) during the Saharan Mineral Dust Experiment (SAMUM) experiment in May–June 2006. Two different sun photometers were used for this purpose. The mean AOD at 500 nm was 0.28, with a maximum of 0.83, and the mean Ångström exponent (AE) was 0.35. The aerosol content over the site changed alternatively from very low turbidity, associated to Atlantic air masses, to moderate dust load, associated to air masses arriving in the site from Algeria, Tunisia and Libya. The dusty conditions were predominant in the measurement period (78% of data), with AOD (500 nm) above 0.15 and AE below 0.4. The spectral features of the AOD under dusty conditions are discussed. Air mass back trajectory analysis is carried out to investigate the origin and height patterns of the dust loaded air masses. The advection of dust occurred mainly at atmospheric heights below 3000 m, where east flow is the predominant. At the 5000 m level, the air masses originate mainly over the Atlantic Ocean. Finally the Optical Properties of Aerosols and Clouds (OPAC) model is used to perform a set of simulations with different aerosol mixtures to illustrate the measured AOD and AE values under varying dust concentrations, and a brief comparison with other measurement sites is presented.     

Effect of sea salt on dust settling to the ocean

Dust particles frequently become mixtures of mineral dust and sea salt during their transport in the marine boundary layer, consequently growing in size, which causes changes in their settling velocities. In this study, the effect of sea salt on the gravitational settling of dust particles is investigated. Results show that the adhering of sea salt to dust particles can dramatically increase the gravitational settling of the particles, in particular if the particles become larger than 3–4 μm. Estimates with the observational data from six dust events in southwestern Japan revealed that, due to sea salt adhering, the gravitational settling flux of mineral dust increased approximately 14–17% in well-mixed events and 4–6% in less-mixed events, indicating a potential significant effect of sea salt on dust settling and the importance of considering this effect in the schemata of particle gravitational settling when mapping dust flux to the ocean.     

Tests for individual Sulfate－Containing Particles in Urban Atmosphere in Beijing

Thin film methods and X ray energy dispersive technique were applied to analyze sulfate-containing particles in Beijing in order to examine their features and sources. Atmospheric aerosol particles were collected on electron mi-croscope meshes according to two size ranges: coarse particles (r>0.5μm) and fine particles (0.5μm≥r≥0.1μm) by using a two-stage impactor. It was found fiat more than seventy percent of the fine particles and about twenty percent of the coarse particles were sulfate-containing particles. These particles were formed mainly through heterogeneous nucleation. The element composition analyses revealed that the atmospheric aerosol particles in Beijing were domi-nated by crustal particles and construction dust.     

Depolarization ratio profiling at several wavelengths in pure Saharan dust during SAMUM 2006

Vertical profiles of the linear particle depolarization ratio of pure dust clouds were measured during the Saharan Mineral Dust Experiment (SAMUM) at Ouarzazate, Morocco (30.9°N, –6.9°E), close to source regions in May–June 2006, with four lidar systems at four wavelengths (355, 532, 710 and 1064 nm). The intercomparison of the lidar systems is accompanied by a discussion of the different calibration methods, including a new, advanced method, and a detailed error analysis. Over the whole SAMUM periode pure dust layers show a mean linear particle depolarization ratio at 532 nm of 0.31, in the range between 0.27 and 0.35, with a mean Ångström exponent (AE, 440–870 nm) of 0.18 (range 0.04–0.34) and still high mean linear particle depolarization ratio between 0.21 and 0.25 during periods with aerosol optical thickness less than 0.1, with a mean AE of 0.76 (range 0.65–1.00), which represents a negative correlation of the linear particle depolarization ratio with the AE. A slight decrease of the linear particle depolarization ratio with wavelength was found between 532 and 1064 nm from 0.31 ± 0.03 to 0.27 ± 0.04.