Vertical profile of the clear-sky aerosol direct radiative effect in an Alpine valley, by the synergy of ground-based measurements and radiative transfer simulations

Atmospheric aerosols play an important role in Earth’s radiative balance, directly interacting with solar radiation or influencing cloud formation and properties. In order to assess their radiative impact, it is necessary to accurately characterise their optical properties, together with their spatial and vertical distribution. The information on aerosol vertical profile is often scarce, in particular in mountainous, complex terrains. This study presents the first attempt to evaluate the shortwave aerosol direct radiative effect in the Aosta Valley, a mountainous region in the Northwestern Italian Alps. Ground-based, remote sensing instruments (a sky radiometer and an Automated Lidar Ceilometer) are used to derive two descriptions of the aerosol properties and vertical distribution: a first, more accurate description, which includes the whole spectral information about the aerosol extinction coefficient, phase function and single scattering albedo; a second, more approximate one, which only relies on spectrally constant values of aerosol single scattering albedo and asymmetry factor. This information is used as input for radiative transfer simulations, which allow to estimate, in cloudless conditions, the shortwave aerosol direct radiative effect and the vertical profile of the instantaneous heating rates in the lower layers of the atmosphere. The simulations obtained with the two descriptions do not differ significantly: they highlight a strong surface dimming (between − 25 and − 50 W m− 2) due to the presence of aerosol, with a considerable radiative absorption inside the atmospheric column (around + 30 W m− 2), and an overall small cooling effect for the Earth-atmospheric system. The absorption of solar radiation within the atmospheric column due to aerosol leads to instantaneous heating rates up to 1.5 K day− 1 in the tropospheric layers below 6 km a.s.l. These results show that, in some conditions, the shortwave aerosol direct radiative effect can be considerable even in this Alpine environment, usually considered as relatively pristine (yearly average PM10 concentration about 20 μg m− 3).

Relative errors of derived multi-wavelengths intensive aerosol optical properties using CAPS_SSA, Nephelometer and TAP measurements

Aerosol intensive optical properties like the Ångström exponents for aerosol light extinction, scattering and absorption, or the single-scattering albedo are indicators for aerosol size distributions, chemical composition and radiative behaviour and contain also source information. The observation of these parameters requires the measurement of aerosol optical properties at multiple wavelengths which usually implies the use of several instruments. Our study aims to quantify the uncertainties of the determination of multiple-wavelengths intensive properties by an optical closure approach, using different test aerosols. In our laboratory study, we measured the full set of aerosol optical properties for a range of light-absorbing aerosols with different properties, mixed externally with ammonium sulphate to generate aerosols of controlled single-scattering albedo. The investigated aerosol types were: fresh combustion soot emitted by an inverted flame soot generator (SOOT, fractal aggregates), Aquadag (AQ, spherical shape), Cabot industrial soot (BC, compact clusters), and an acrylic paint (Magic Black, MB). One focus was on the validity of the Differential Method (DM: absorption = extinction minus scattering) for the determination of Ångström exponents for different particle loads and mixtures of light-absorbing aerosol with ammonium sulphate, in comparison to data obtained from single instruments. The instruments used in this study were two CAPS PMssa (Cavity Attenuated Phase Shift Single Scattering Albedo, λ = 450, 630 nm) for light extinction and scattering coefficients, one Integrating Nephelometer (λ = 450, 550, 700 nm) for light scattering coefficient and one Tricolour Absorption Photometer (TAP, λ = 467, 528, 652 nm) for filter-based light absorption coefficient measurement. Our key finding is that the coefficients of light absorption σap, scattering σsp and extinction σep from the Differential Method agree with data from single reference instruments, and the slopes of regression lines equal unity within the precision error. We found, however, that the precision error for the DM suppresses 100 % for σap values lower than 10–20 Mm−1 for atmospheric relevant single scattering albedo. This increasing uncertainty with decreasing σap yields an absorption Ångström exponent (AAE) that is too uncertain for measurements in the range of atmospheric aerosol loadings. We recommend using DM only for measuring AAE values for σap > 50 Mm−1. Ångström exponents for scattering and extinction are reliable for extinction coefficients from 20 up to 1000 Mm−1 and stay within 10 % deviation from reference instruments, regardless of the chosen method. Single-scattering albedo (SSA) values for 450 nm and 630 nm wavelengths agree with values from the reference method σsp (NEPH)/σep (CAPS PMSSA) with less than 10 % uncertainty for all instrument combinations and sampled aerosol types which fulfil the proposed goal for measurement uncertainty of 10 % proposed by Laj et al., 2020 for GCOS (Global Climate Observing System) applications.

Identifying Chemical Aerosol Signatures using Optical Suborbital Observations: How much can optical properties tell us about aerosol composition?

Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Analysis of Aerosol Optical Depth from Sun Photometer at Shouxian, China

We use two cloud screening methods—the clustering method and the multiplet method—to process the measurements of a sun photometer from March 2020 to April 2021 in Shouxian. The aerosol optical depth (AOD) and Angström parameters α and β are retrieved; variation characteristics and single scattering albedo are studied. The results show that: (1) The fitting coefficient of AOD retrieved by the two methods is 0.921, and the changing trend is consistent. The clustering method has fewer effective data points and days, reducing the overall average of AOD by 0.0542 (500 nm). (2) Diurnal variation of AOD can be divided into flat type, convex type, and concave type. Concave type and convex type occurred the most frequently, whereas flat type the least. (3) During observation, the overall average of AOD is 0.48, which is relatively high. Among them, AOD had a winter maximum (0.70), autumn and spring next (0.54 and 0.40), and a summer minimum (0.26). The variation trend of AOD and β is highly consistent, and the monthly mean of α is between 0.69 and 1.61, concerning mainly continental and urban aerosols. (4) Compared with others, the single scattering albedo in Shouxian is higher, reflecting strong scattering and weak aerosol absorption.

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.

Global maps of aerosol single scattering albedo using combined CERES-MODIS retrieval

Single Scattering Albedo (SSA) is a leading contributor to the uncertainty in aerosol radiative impact assessments. Therefore accurate information on aerosol absorption is required on a global scale. In this study, we have applied a multi-satellite algorithm to retrieve SSA using the concept of ‘critical optical depth.’ Global maps of SSA were generated following this approach using spatially and temporally collocated data from Clouds and the Earth’s Radiant Energy System (CERES) and Moderate Resolution Imaging Spectroradiometer (MODIS) sensors on board Terra and Aqua satellites. The method has been validated using the data from aircraft-based measurements of various field campaigns. The retrieval uncertainty is ±0.03 and depends on both the surface albedo and aerosol absorption. Global mean SSA estimated over land and ocean is 0.93 and 0.97, respectively. Seasonal and spatial distribution of SSA over various regions are also presented. The global maps of SSA, thus derived with improved accuracy, provide important input to climate models for assessing the climatic impact of aerosols on regional and global scales.