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    The effect of rapid relative humidity changes on fast filter-based aerosol-particle light-absorption measurements: Uncertainties and correction schemes
    (Katlenburg-Lindau : Copernicus, 2019) Düsing, Sebastian; Wehner, Birgit; Müller, Thomas; Stöcker, Almond; Wiedensohler, Alfred
    Measuring vertical profiles of the particle light-absorption coefficient by using absorption photometers may face the challenge of fast changes in relative humidity (RH). These absorption photometers determine the particle light-absorption coefficient due to a change in light attenuation through a particle-loaded filter. The filter material, however, takes up or releases water with changing relative humidity (RH in %), thus influencing the light attenuation. A sophisticated set of laboratory experiments was therefore conducted to investigate the effect of fast RH changes (dRH/dt) on the particle light-absorption coefficient (σabs in Mm-1) derived with two absorption photometers. The RH dependence was examined based on different filter types and filter loadings with respect to loading material and areal loading density. The Single Channel Tricolor Absorption Photometer (STAP) relies on quartz-fiber filter, and the microAeth® MA200 is based on a polytetrafluoroethylene (PTFE) filter band. Furthermore, three cases were investigated: clean filters, filters loaded with black carbon (BC), and filters loaded with ammonium sulfate. The filter areal loading densities (ρ∗) ranged from 3.1 to 99.6 mg m-2 in the case of the STAP and ammonium sulfate and 1.2 to 37.6 mg m-2 in the case the MA200. Investigating BC-loaded cases, M8 scroll mrow miBCm 15pt was in the range of 2.9 to 43.0 and 1.1 to 16.3 mg m-2 for the STAP and MA200, respectively.

    Both instruments revealed opposing responses to relative humidity changes ("RH) with different magnitudes. The STAP shows a linear dependence on relative humidity changes. The MA200 is characterized by a distinct exponential recovery after its filter was exposed to relative humidity changes. At a wavelength of 624 nm and for the default 60 s running average output, the STAP reveals an absolute change in σabs per absolute change of RH ("σabsĝ•"RH) of 0.14 Mm-1 %-1 in the clean case, 0.29 Mm-1 %-1 in the case of BC-loaded filters, and 0.21 Mm-1 %-1 in the case filters loaded with ammonium sulfate. The 60 s running average of the particle light-absorption coefficient at 625 nm measured with the MA200 revealed a response of around -0.4 Mm-1 %-1 for all three cases. Whereas the response of the STAP varies over the different loading materials, in contrast, the MA200 was quite stable. The response was, for the STAP, in the range of 0.17 to 0.24 Mm-1 %-1 and, in the case of ammonium sulfate loading and in the BC-loaded case, 0.17 to 0.62 Mm-1 %-1. In the ammonium sulfate case, the minimum response shown by the MA200 was -0.42 with a maximum of -0.36 Mm-1 %-1 and a minimum of -0.42 and maximum -0.37 Mm-1 %-1 in the case of BC.

    A linear correction function for the STAP was developed here. It is provided by correlating 1 Hz resolved recalculated particle light-absorption coefficients and RH change rates. The linear response is estimated at 10.08 Mm-1 s-1 %-1. A correction approach for the MA200 is also provided; however, the behavior of the MA200 is more complex. Further research and multi-instrument measurements have to be conducted to fully understand the underlying processes, since the correction approach resulted in different correction parameters across various experiments. However, the exponential recovery after the filter of the MA200 experienced a RH change could be reproduced. However, the given correction approach has to be estimated with other RH sensors as well, since each sensor has a different response time. And, for the given correction approaches, the uncertainties could not be estimated, which was mainly due to the response time of the RH sensor. Therefore, we do not recommend using the given approaches. But they point in the right direction, and despite the imperfections, they are useful for at least estimating the measurement uncertainties due to relative humidity changes.

    Due to our findings, we recommend using an aerosol dryer upstream of absorption photometers to reduce the RH effect significantly. Furthermore, when absorption photometers are used in vertical measurements, the ascending or descending speed through layers of large relative humidity gradients has to be low to minimize the observed RH effect. But this is simply not possible in some scenarios, especially in unmixed layers or clouds. Additionally, recording the RH of the sample stream allows correcting for the bias during post-processing of the data. This data correction leads to reasonable results, according to the given example in this study. © Author(s) 2019.

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    Nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) for investigating hygroscopic properties of sub-10nm aerosol nanoparticles
    (Katlenburg-Lindau : Copernicus, 2020) Lei, Ting; Ma, Nan; Hong, Juan; Tuch, Thomas; Wang, Xin; Wang, Zhibin; Pöhlker, Mira; Ge, Maofa; Wang, Weigang; Mikhailov, Eugene; Hoffmann, Thorsten; Pöschl, Ulrich; Su, Hang; Wiedensohler, Alfred; Cheng, Yafang
    Interactions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physicochemical properties of nanoparticles, however, is restricted by the limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Besides maintaining accurate and stable sheath and aerosol flow rates (1 %), high accuracy of the differential mobility analyzer (DMA) voltage (0:1 %) in the range of 0-50V is crucial for achieving accurate sizing and small sizing offsets between the two DMAs (1:4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (0:1 K). We also tested and discussed different ways of preventing predeliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size effect on the deliquescence and efflorescence relative humidity (DRH and ERH, respectively) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size dependence of DRH and ERH between 20 and 6 nm nanoparticles. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
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    Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations
    (Katlenburg-Lindau : Copernicus, 2022) Romshoo, Baseerat; Pöhlker, Mira; Wiedensohler, Alfred; Pfeifer, Sascha; Saturno, Jorge; Nowak, Andreas; Ciupek, Krzysztof; Quincey, Paul; Vasilatou, Konstantina; Ess, Michaela N.; Gini, Maria; Eleftheriadis, Konstantinos; Robins, Chris; Gaie-Levrel, François; Müller, Thomas
    Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.