Weingartner, Ernest
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A novel measurement system for unattended, in situ characterization of carbonaceous aerosols
Carbonaceous aerosol is a relevant constituent of the atmosphere in terms of climate and health impacts. Nevertheless, measuring this component poses many challenges. There is currently no simple and sensitive commercial technique that can reliably capture its totality in an unattended manner, with minimal user intervention, for extended periods of time. To address this issue we have developed the fast thermal carbon totalizator (FATCAT). Our system captures an aerosol sample on a rigid metallic filter and subsequently analyses it by rapidly heating the filter directly, through induction, to a temperature around 800°C. The carbon in the filter is oxidized and quantified as CO2 in order to establish the total carbon (TC) content of the sample. The metallic filter is robust, which solves filter displacement or leakage problems, and does not require a frequent replacement like other measurement techniques. The limit of detection of our system using the 3σ criterion is TC =0.19 µg-C (micrograms of carbon). This translates to an average ambient concentration of TC =0.32 µg-C m^−3 and TC =0.16 µg-C m^−3 for sampling interval of 1 or 2 h respectively using a sampling flow rate of 10 L min^−1. We present a series of measurements using a controlled, well-defined propane flame aerosol as well as wood-burning emissions using two different wood-burning stoves. Furthermore, we complement these measurements by coating the particles with secondary organic matter by means of an oxidation flow reactor. Our device shows a good correlation (correlation coefficient, R^2>0.99) with well-established techniques, like mass measurements by means of a tapered element oscillating microbalance and TC measurements by means of thermal–optical transmittance analysis. Furthermore, the homogeneous fast-heating of the filter produces fast thermograms. This is a new feature that, to our knowledge, is exclusive of our system. The fast thermograms contain information regarding the volatility and refractoriness of the sample without imposing an artificial fraction separation like other measurement methods. Different aerosol components, like wood-burning emissions, soot from the propane flame and secondary organic matter, create diverse identifiable patterns.
Interdisziplinäre Perspektiven zur Bedeutung der Aerosolübertragung für das Infektionsgeschehen von SARS-CoV-2
Die Bedeutung der Aerosolübertragung für das Severe Acute Respiratory Syndrome Coronavirus Type 2 (SARS-CoV-2) wurde anfangs kontrovers diskutiert. Mit der Zeit haben sich zur Infektionsminderung jedoch neben Abstands- und Hygieneregeln auch aerosolphysikalisch begründete Maßnahmen wie das Tragen von Gesichtsmasken und Lüftung von Innenräumen als effektiv erwiesen. In einem interdisziplinären Workshop „Aerosol & SARS-CoV-2“ der Gesellschaft für Aerosolforschung (GAeF) in Kooperation mit der Deutschen Gesellschaft für Pneumologie und Beatmungsmedizin (DGP), dem Fachverband Allgemeine Lufttechnik im VDMA, der Gesellschaft für Virologie (GfV), der Gesundheitstechnischen Gesellschaft (GG) und der International Society for Aerosols in Medicine (ISAM) unter der Schirmherrschaft des Robert-Koch-Instituts (RKI) im März 2021 wurde der Forschungs- und Abstimmungsbedarf zu diesem Thema aufgegriffen. Wesentliche Grundlagen aus den verschiedenen Disziplinen sowie interdisziplinäre Perspektiven zur Aerosolübertragung von SARS-CoV-2 und zu infektionsmindernden Maßnahmen werden hier zusammengefasst. Abschließend werden offene Forschungsfragen und dringender Forschungsbedarf dargestellt.
Comparing black carbon and aerosol absorption measuring instruments – a new system using lab-generated soot coated with controlled amounts of secondary organic matter
We report on an inter-comparison of black-carbon- and aerosol-absorption-measuring instruments with laboratory-generated soot particles coated with controlled amounts of secondary organic matter (SOM). The aerosol generation setup consisted of a miniCAST 5201 Type BC burner for the generation of soot particles and a new automated oxidation flow reactor based on the micro smog chamber (MSC) for the generation of SOM from the ozonolysis of α-pinene. A series of test aerosols was generated with elemental to total carbon (EC / TC) mass fraction ranging from about 90 % down to 10 % and single-scattering albedo (SSA at 637 nm) from almost 0 to about 0.7. A dual-spot Aethalometer AE33, a photoacoustic extinctiometer (PAX, 870 nm), a multi-angle absorption photometer (MAAP), a prototype photoacoustic instrument, and two prototype photo-thermal interferometers (PTAAM-2λ and MSPTI) were exposed to the test aerosols in parallel. Significant deviations in the response of the instruments were observed depending on the amount of secondary organic coating. We believe that the setup and methodology described in this study can easily be standardised and provide a straightforward and reproducible procedure for the inter-comparison and characterisation of both filter-based and in situ black-carbon-measuring (BC-measuring) instruments based on realistic test aerosols.
A European aerosol phenomenology - 6. Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites
This paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σsp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σsp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intra-annual variability. At mountain sites, higher σsp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σsp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σsp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σsp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σsp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σsp are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.
Development of a waveguide-based interferometer for the measurement of trace substances
Photonic integration on a chip has the potential to develop new low-cost, high-performance sensing devices. A proof of concept of the sensing capabilities of a waveguide-based photothermal interferometer for the measurement of traces of light-absorbing substances (soot particles, gases) has been achieved. The measurement principle can also be extended to a wide range of other applications such as refractive index measurements, or vibration/distance sensors. A unique feature is that the waveguide technology allows for a passive operation of the interferometer, i.e., no quadrature point control is required.
A global study of hygroscopicity-driven light-scattering enhancement in the context of other in situ aerosol optical properties
The scattering and backscattering enhancement factors (f(RH) and fb(RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in Burgos et al. (2019) that compiles f(RH) and fb(RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f(RH) and fb(RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher f(RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb(RH) is consistently lower than f(RH) at all sites, with the difference between f(RH) and fb(RH) increasing for aerosol with higher f(RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM1 than PM10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω0, and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω0 and scattering Ångström exponent, αsp) to parameterize f(RH). The majority of sites (75 %) showed a consistent trend with ω0 (higher f(RH = 85 %) for higher ω0), while no clear pattern was observed between f(RH = 85 %) and αsp. This suggests that aerosol ω0 is more promising than αsp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω0 and f(RH) could serve as a constraint on global model simulations.
A dual-wavelength photothermal aerosol absorption monitor. Design, calibration and performance
There exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed the two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM-2λ), which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ∼ 1 µmol mol−1 NO2, whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 and 1064 nm, respectively, and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and CLAP suffer from cross sensitivity to scattering – this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100–500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.23–0.35 higher than the PTAAM-2λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements.
A single-beam photothermal interferometer for in situ measurements of aerosol light absorption
We have developed a novel single-beam photothermal interferometer and present here its application for the measurement of aerosol light absorption. The use of only a single laser beam allows for a compact optical set-up and significantly easier alignment compared to standard dual-beam photothermal interferometers, making it ideal for field measurements. Due to a unique configuration of the reference interferometer arm, light absorption by aerosols can be determined directly – even in the presence of light-absorbing gases. The instrument can be calibrated directly with light-absorbing gases, such as NO2, and can be used to calibrate other light absorption instruments. The detection limits (1σ) for absorption for 10 and 60 s averaging times were determined to be 14.6 and 7.4 Mm−1, respectively, which for a mass absorption cross section of 10 m2 g−1 leads to equivalent black carbon concentration detection limits of 1460 and 740 ng m−3, respectively. The detection limit could be reduced further by improvements to the isolation of the instrument and the signal detection and processing schemes employed.