Recent observations suggest that a certain fraction of organic carbon (OC) aerosol effectively absorbs solar radiation, which is also known as brown carbon (BrC) aerosol. Despite much observational evidence of its presence, very few global modelling studies have been conducted because of poor understanding of global BrC emissions. Here we present an explicit global simulation of BrC in a global 3-D chemical transport model (GEOS-Chem), including global BrC emission estimates from primary (3.9 ± 1.7 and 3.0 ± 1.3 TgC yr⁻¹ from biomass burning and biofuel) and secondary (5.7 TgC yr⁻¹ from aromatic oxidation) sources. We evaluate the model by comparing the results with observed absorption by water-soluble OC in surface air in the United States, and with single scattering albedo observations at Aerosol Robotic Network (AERONET) sites all over the globe. The model successfully reproduces the seasonal variations of observed light absorption by water-soluble OC, but underestimates the magnitudes, especially in regions with high secondary source contributions. Our global simulations show that BrC accounts for 21 % of the global mean surface OC concentration, which is typically assumed to be scattering. We find that the global direct radiative effect of BrC is nearly zero at the top of the atmosphere, and consequently decreases the direct radiative cooling effect of OC by 16 %. In addition, the BrC absorption leads to a general reduction of NO₂ photolysis rates, whose maximum decreases occur in Asia up to −8 % (−17 %) on an annual (spring) mean basis. The resulting decreases of annual (spring) mean surface ozone concentrations are up to −6 % (−13 %) in Asia, indicating a non-negligible effect of BrC on photochemistry in this region.

The Himalayas and the Tibetan Plateau region (HTP), despite being a remote and sparsely populated area, is regularly exposed to polluted air masses with significant amounts of aerosols including black carbon. These dark, light-absorbing particles are known to exert a great melting potential on mountain cryospheric reservoirs through albedo reduction and radiative forcing. This study combines ground-based and satellite remote sensing data to identify a severe aerosol pollution episode observed simultaneously in central Tibet and on the southern side of the Himalayas during 13–19 March 2009 (pre-monsoon). Trajectory calculations based on the high-resolution numerical weather prediction model COSMO are used to locate the source regions and study the mechanisms of pollution transport in the complex topography of the HTP. We detail how polluted air masses from an atmospheric brown cloud (ABC) over South Asia reach the Tibetan Plateau within a few days. Lifting and advection of polluted air masses over the great mountain range is enabled by a combination of synoptic-scale and local meteorological processes. During the days prior to the event, winds over the Indo-Gangetic Plain (IGP) are generally weak at lower levels, allowing for accumulation of pollutants and thus the formation of ABCs. The subsequent passing of synoptic-scale troughs leads to southwesterly flow in the middle troposphere over northern and central India, carrying the polluted air masses across the Himalayas. As the IGP is known to be a hotspot of ABCs, the cross-Himalayan transport of polluted air masses may have serious implications for the cryosphere in the HTP and impact climate on regional to global scales. Since the current study focuses on one particularly strong pollution episode, quantifying the frequency and magnitude of similar events in a climatological study is required to assess the total impact.

This paper is an overview of the progress in sky radiometer technology and the development of the network called SKYNET. It is found that the technology has produced useful on-site calibration methods, retrieval algorithms, and data analyses from sky radiometer observations of aerosol, cloud, water vapor, and ozone. A formula was proposed for estimating the accuracy of the sky radiometer calibration constant F₀ using the improved Langley (IL) method, which was found to be a good approximation to observed monthly mean uncertainty in F₀, around 0.5 % to 2.4 % at the Tokyo and Rome sites and smaller values of around 0.3 % to 0.5 % at the mountain sites at Mt. Saraswati and Davos. A new cross IL (XIL) method was also developed to correct an underestimation by the IL method in cases with large aerosol retrieval errors. The root-mean-square difference (RMSD) in aerosol optical thickness (AOT) comparisons with other networks took values of less than 0.02 for λ≥500 nm and a larger value of about 0.03 for shorter wavelengths in city areas and smaller values of less than 0.01 in mountain comparisons. Accuracies of single-scattering albedo (SSA) and size distribution retrievals are affected by the propagation of errors in measurement, calibrations for direct solar and diffuse sky radiation, ground albedo, cloud screening, and the version of the analysis software called the Skyrad pack. SSA values from SKYNET were up to 0.07 larger than those from AERONET, and the major error sources were identified as an underestimation of solid viewing angle (SVA) and cloud contamination. Correction of these known error factors reduced the SSA difference to less than 0.03. Retrievals of other atmospheric constituents by the sky radiometer were also reviewed. Retrieval accuracies were found to be about 0.2 cm for precipitable water vapor amount and 13 DU (Dobson Unit) for column ozone amount. Retrieved cloud optical properties still showed large deviations from validation data, suggesting a need to study the causes of the differences. It is important that these recent studies on improvements presented in the present paper are introduced into the existing operational systems and future systems of the International SKYNET Data Center.

In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.

Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE), absorption Ångström exponent (AAE) and single scattering albedo (SSA) from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes.Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type) and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station.The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol), marine polluted (carbonaceous aerosol mixed with sea salt) and continental dust/biomass sites (dust and carbonaceous aerosol); however, current classification schemes perform poorly when predicting dominant aerosol type at remote marine and Arctic sites and at stations with more complex locations and topography where variable aerosol populations are not well represented by median optical properties. Although the aerosol classification methods presented here provide new ways to reduce ambiguity in typing schemes, there is more work needed to find aerosol typing methods that are useful for a larger range of geographic locations and aerosol populations.

Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.