A global study of hygroscopicity-driven light-scattering enhancement in the context of other in situ aerosol optical properties

Gloria Titos; Maria Burgos; Paul Zieger; Lucas Alados-Arboledas; Urs Baltensperger; Anne Jefferson; James Sherman; Ernest Weingartner; Bas Henzing; Krista Luoma; Colin O'Dowd; Alfred Wiedensohler; Elisabeth Andrews
2021 | Atmos. Chem. Phys. | 21 (13031-13050)
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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.

From a polar to a marine environment: has the changing Arctic led to a shift in aerosol light scattering properties?

2020 | Atmos. Chem. Phys. | 20 (13671-13686)
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The study of long-term trends in aerosol optical properties is an important task to understand the underlying aerosol processes influencing the change of climate. The Arctic, as the place where climate change manifests most, is an especially sensitive region of the world. Within this work, we use a unique long-term data record of key aerosol optical properties from the Zeppelin Observatory, Svalbard, to ask the question of whether the environmental changes of the last 2 decades in the Arctic are reflected in the observations. We perform a trend analysis of the measured particle light scattering and backscattering coefficients and the derived scattering Ångström exponent and hemispheric backscattering fraction. In contrast to previous studies, the effect of in-cloud scavenging and of potential sampling losses at the site are taken explicitly into account in the trend analysis. The analysis is combined with a back trajectory analysis and satellite-derived sea ice data to support the interpretation of the observed trends. We find that the optical properties of aerosol particles have undergone clear and significant changes in the past 2 decades. The scattering Ångström exponent exhibits statistically significant decreasing of between −4.9 % yr−1 and −6.5 % yr−1 (using wavelengths of λ=450 and 550 nm), while the particle light scattering coefficient exhibits statistically significant increasing trends of between 2.6 % yr−1 and 2.9 % yr−1 (at a wavelength of λ=550 nm). The magnitudes of the trends vary depending on the season. These trends indicate a shift to an aerosol dominated more by coarse-mode particles, most likely the result of increases in the relative amount of sea spray aerosol. We show that changes in air mass circulation patterns, specifically an increase in air masses from the south-west, are responsible for the shift in aerosol optical properties, while the decrease of Arctic sea ice in the last 2 decades only had a marginal influence on the observed trends.

A global model–measurement evaluation of particle light scattering coefficients at elevated relative humidity

Burgos, M. A.; Andrews, E.; Titos, G.; Benedetti, A.; Bian, H.; Buchard, V.; Curci, G.; Kipling, Z.; Kirkevåg, A.; Kokkola, H.; Laakso, A.; Letertre-Danczak, J.; Lund, M. T.; Matsui, H.; Myhre, G.; Randles, C.; Schulz, M.; van Noije, T.; Zhang, K.; Alados-Arboledas, L.; Baltensperger, U.; Jefferson, A.; Sherman, J.; Sun, J.; Weingartner, E.; Zieger, P.
2020 | Atmos. Chem. Phys. | 20 (10231-10258)
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The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f(RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f(RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f(RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f(RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided.

A global view on the effect of water uptake on aerosol particle light scattering

Burgos, M.; Andrews; E.; Titos, G.; Alados-Arboledas, L.; Baltensperger, U.; Day, D.; Jefferson, A.; Kalivitis, N.; Mihalopoulos, N.; Sherman, J.; Sun, J.; Weingartner, E.; Zieger, P.
2019 | Sci. Data | 6 (157) (1-19)
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A reference dataset of multi-wavelength particle light scattering and hemispheric backscattering coefficients for different relative humidities (RH) between RH = 30 and 95% and wavelengths between λ = 450 nm and 700 nm is described in this work. Tandem-humidified nephelometer measurements from 26 ground-based sites around the globe, covering multiple aerosol types, have been re-analysed and harmonized into a single dataset. The dataset includes multi-annual measurements from long-term monitoring sites as well as short-term field campaign data. The result is a unique collection of RH-dependent aerosol light scattering properties, presented as a function of size cut. This dataset is important for climate and atmospheric model-measurement inter-comparisons, as a means to improve model performance, and may be useful for satellite and remote sensing evaluation using surface-based, in-situ measurements.

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Geovetenskapens Hus,
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Arrheniuslaboratoriet, Svante Arrhenius väg 16, Stockholm (Unit for Toxicological Chemistry)

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