Parametrization of relative humidity- and wavelength-dependent optical properties of mixed Saharan dust and marine aerosol

Aerosol particles interact with sunlight through scattering and absorption and have therefore a direct radiative effect. Hygroscopic aerosol particles take up water and are able to grow in size below 100% relative humidity, which involves the change of optical properties and the direct radiative effect. The change of aerosol optical properties for aerosol mixtures under humidification is presently not well understood, especially for the largest particle sources worldwide. The present PhD-thesis quantifies wavelength- and humidity-dependent aerosol optical properties for a mixture of Saharan mineral dust and marine aerosol. For quantification, an aerosol model was developed, which based on in-situ measurements of microphysical and optical properties at Cape Verde. With this model, aerosol optical properties were calculated from the dry state up to 90% relative humidity. To validate the model, a measure of the total extenuated light from particles under ambient conditions was used. Finally, the humidity dependence of aerosol optical properties for marine aerosol, Saharan dust aerosol, and a mixture of both species was described by two empirical equations. With the wavelength of the incident visible solar radiation, relative humidity, and dry dust volume fraction, the humidity dependence of optical properties can be calculated from tabulated values. To calculate radiative effects, aerosol optical properties were used as input parameters for global circulation models including radiative transfer. Due to the complexity of aerosol related processes, they have been treated implicitly, meaning in parameterized form. For modelling purposes, the present PhD-thesis provides a solution to include humidity effects of aerosol optical properties.Aerosolpartikel wechselwirken durch Streu- und Absorptionsprozesse mit der einfallenden Sonnenstrahlung und haben somit einen direkten Strahlungseffekt. Bei relativen Feuchten bis 100% können Aerosolpartikel aufquellen und somit ihre Größe ändern. Im Zuge des Aufquellens, ändern sich die optischen Eigenschaften und somit auch der direkte Strahlungseffekt der Aerosolpartikel. Speziell für Mischungen von verschiedenen Aerosolspezies ist die Änderung der optischen Eigenschaften des Aerosols durch Feuchte Einfuss noch nicht ausreichend verstanden. Gegenstand der vorliegenden Arbeit ist daher die Quantifizierung der wellenlängen- und feuchteabhängigen optischen Eigenschaften einer Mischung von Saharastaub- und marinen Aerosol. Die zur Quantifizierung notwendigen Daten wurden im Rahmen einer Feldmessung von mikrophysikalischen- und optischen Aerosol-Eigenschaften auf den Kapverdischen Inseln gesammelt. Auf Grundlage dieser Messungen wurde ein Aerosol-Modell entwickelt. Dieses Modell wurde daraufhin verwendet, um Berechnungen von optischen Aerosol-Eigenschaften bei relativen Feuchten bis 90% durchzuführen. Eine Messung der Lichtschwächung durch Aerosolpartikel unter Umgebungsbedingungen wurde verwandt, um das Modell bei Umgebungsfeuchten zu validieren. Die Wellenlängen- und Feuchteabhängigkeit der optischen Eigenschaften des Aerosols wurde parametrisiert und konnte anhand von zwei Parametergleichungen bestimmt werden. Unter Benutzung von tabellierten Werten und der Wellenlänge des einfallenden sichtbaren Sonnenlichtes, der relativen Feuchte, sowie der Staubvolumenfraktion, kann die Feuchteabhängigkeit von wichtigen Aerosol-optischen Eigenschaften für Saharastaub, marinen Aerosol und einer Mischung aus beiden Komponenten bestimmt werden. Globale Zirkulationsmodelle, die auch eine Berechnung von Strahlungseffekten durch Aerosolpartikel beinhalten, nutzen Aerosol-optische Eigenschaften als Eingabeparameter. Durch zunehmende Komplexitiät zur Beschreibung von Wechselwirkungen in der Atmosphäre, sind einfache Parametrisierungen unabdingbar. Die vorliegende Arbeit liefert daher einen wichtigen Beitrag für die Modellierung von Strahlungseffekten durch Aerosolpartikel und somit zum Verständnis des Strahlungshaushaltes der Erde

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 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

Characterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements

Measurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians- Universit¨at, M¨unchen, Germany, performed during SAMUM-2, were used to characterize the planetary boundary layer (PBL) over Praia, Cape Verde. A novel approach was used to determine the volume fraction of dust υd in the PBL. This approach primarily relies on accurate measurements of the linear depolarization ratio. Comparisons with independent in situ measurements showed the reliability of this approach. Based on our retrievals, two different phases could be distinguished within the measurement period of almost one month. The first (22–31 January 2008) was characterized by high aerosol optical depth (AOD) in the PBL and large υd > 95%. During the second phase, the AOD in the PBL was considerably lower and υd less than ∼40%. These findings were in very good agreement with ground based in situ measurements, when ambient volume fractions are considered that were calculated from the actual measurements of the dry volume fraction. Only in cases when dust was not the dominating aerosol component (second phase), effects due to hygroscopic growth became important

In situ aerosol characterization at Cape Verde, Part 2: Parametrization of relative humidity- and wavelength-dependent aerosol optical properties

An observation-based numerical study of humidity-dependent aerosol optical properties of mixed marine and Saharan mineral dust aerosol is presented. An aerosol model was developed based on measured optical and microphysical properties to describe the marine and Saharan dust aerosol at Cape Verde. A wavelength-dependent optical equivalent imaginary part of the refractive index and a scattering non-sphericity factor for Saharan dustwere derived. Simulations of humidity effects on optical properties by the aerosol model were validated with relative measurements of the extinction coefficient at ambient conditions. Parametrizations were derived to describe the humidity dependence of the extinction, scattering, and absorption coefficients as well as the asymmetry parameter and single scattering albedo. For wavelengths (300–950 nm) and dry dust volume fractions (0–1), aerosol optical properties as a function of relative humidity (RH = 0–90%) can be calculated from tabulated parameters. For instance, at a wavelength of 550 nm, a volume fraction of 0.5 of dust on the total particle volume (dry conditions) and a RH of 90%, the enhancements for the scattering, extinction and absorption coefficients are 2.55, 2.46 and 1.04, respectively, while the enhancements for the asymmetry parameter and single scattering albedo are 1.11 and 1.04

Solar radiative effects of a Saharan dust plume observed during SAMUM assuming spheroidal model particles

The solar optical properties of Saharan mineral dust observed during the Saharan Mineral Dust Experiment (SAMUM) were explored based on measured size-number distributions and chemical composition. The size-resolved complex refractive index of the dust was derived with real parts of 1.51–1.55 and imaginary parts of 0.0008–0.006 at 550 nm wavelength. At this spectral range a single scattering albedo ωo and an asymmetry parameter g of about 0.8 were derived. These values were largely determined by the presence of coarse particles. Backscatter coefficients and lidar ratios calculated with Mie theory (spherical particles) were not found to be in agreement with independently measured lidar data. Obviously the measured Saharan mineral dust particles were of non-spherical shape. With the help of these lidar and sun photometer measurements the particle shape as well as the spherical equivalence were estimated. It turned out that volume equivalent oblate spheroids with an effective axis ratio of 1:1.6 matched these data best. This aspect ratio was also confirmed by independent single particle analyses using a scanning electron microscope. In order to perform the non-spherical computations, a database of single particle optical properties was assembled for oblate and prolate spheroidal particles. These data were also the basis for simulating the non-sphericity effects on the dust optical properties: ωo is influenced by up to a magnitude of only 1% and g is diminished by up to 4% assuming volume equivalent oblate spheroids with an axis ratio of 1:1.6 instead of spheres. Changes in the extinction optical depth are within 3.5%. Non-spherical particles affect the downwelling radiative transfer close to the bottom of the atmosphere, however, they significantly enhance the backscattering towards the top of the atmosphere: Compared to Mie theory the particle non-sphericity leads to forced cooling of the Earth-atmosphere system in the solar spectral range for both dust over ocean and desert

Desert Dust 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 sub-orbital aerosol measurements into the satellite's larger regional context. On three moderately dusty days for which coincident observations were made, MISR mid-visible aerosol optical thickness (AOT) agrees with field measurements point-by-point to within 0.05 to 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 (a) highlight regional gradients in the mix of dust and background spherical particles, (b) identify a dust plume most likely part of a density flow, and (c) show an air mass containing a higher proportion of small, spherical particles than the surroundings, that appears to be aerosol pollution transported from several thousand kilometers away

Air quality in the German–Czech border region: A focus on harmful fractions of PM and ultrafine particles

A comprehensive air quality study has been carried out at two urban background sites in Annaberg-Buchholz (Germany) and Ústí nad Labem (Czech Republic) in the German–Czech border region between January 2012 and June 2014. Special attention was paid to quantify harmful fractions of particulate matter (PM) and ultrafine particle number concentration (UFP) from solid fuel combustion and vehicular traffic. Source type contributions of UFP were quantified by using the daily concentration courses of UFP and nitrogen oxide. Two different source apportionment techniques were used to quantify relative and absolute mass contributions: positive matrix factorization for total PM2.5 and elemental carbon in PM2.5 and chemical mass balance for total PM1 and organic carbon in PM1. Contributions from solid fuel combustion strongly differed between the non-heating period (April–September) and the heating period (October–March). Major sources of solid fuel combustion in this study were wood and domestic coal combustion, while the proportion of industrial coal combustion was low (<3%). In Ústí nad Labem combustion of domestic brown coal was the most important source of organic carbon ranging from 34% to 43%. Wood combustion was an important source of organic carbon in Annaberg-Buchholz throughout the year. Heavy metals and less volatile polycyclic aromatic hydrocarbons (PAH) in the accumulation mode were related to solid fuel combustion with enhanced concentrations during the heating period. In contrast, vehicular PAH emissions were allocated to the Aitken mode. Only in Ústí nad Labem a significant contribution of photochemical new particle formation (e.g. from sulfur dioxide) to UFP of almost 50% was observed during noontime. UFPs from traffic emissions (nucleation particles) and primary emitted soot particles dominated at both sites during the rest of the day. The methodology of a combined source apportionment of UFP and PM can be adapted to other regions of the world with similar problems of atmospheric pollution to calculate the relative risk in epidemiological health studies for different sub-fractions of PM and UFP. This will enhance the meaningfulness of published relative risks in health studies based on total PM and UFP number concentrations.

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

Regional modelling of Saharan dust and biomass-burning smoke, Part I: Model description and evaluation

The spatio-temporal evolution of the Saharan dust and biomass-burning plume during the SAMUM-2 field campaign in January and February 2008 is simulated at 28 km horizontal resolution with the regional model-system COSMOMUSCAT. The model performance is thoroughly tested using routine ground-based and space-borne remote sensing and local field measurements. Good agreement with the observations is found in many cases regarding transport patterns, aerosol optical thicknesses and the ratio of dust to smoke aerosol. The model also captures major features of the complex aerosol layering. Nevertheless, discrepancies in the modelled aerosol distribution occur, which are analysed in detail. The dry synoptic dynamics controlling dust uplift and transport during the dry season are well described by the model, but surface wind peaks associated with the breakdown of nocturnal low-level jets are not always reproduced. Thus, a strong dust outbreak is underestimated. While dust emission modelling is a priori more challenging, since strength and placement of dust sources depend on on-line computed winds, considerable inaccuracies also arise in observation-based estimates of biomass-burning emissions. They are caused by cloud and spatial errors of satellite fire products and uncertainties in fire emission parameters, and can lead to unrealistic model results of smoke transport

Decreasing trends of particle number and black carbon mass concentrations at 16 observational sites in Germany from 2009 to 2018

Anthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009-2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between-13.1% and-1.7% per year. The slopes of the PNCs vary from-17.2% to-1.7 %,-7.8% to-1.1 %, and-11.1% to-1.2% per year for 10-30, 30-200, and 200-800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies. © 2020 Author(s)