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 Angstrom 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.

Atmospheric aging promotes internal mixing of black carbon (BC), leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in situ at the Zeppelin Arctic station (78 degrees N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the polar region) project. Single-particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39 ngm(-3), while the rBC mass size distribution was of lognormal shape, peaking at an rBC mass-equivalent diameter (D-rBC) of around 240 nm. On average, the number fraction of particles containing a BC core with D-rBC > 80 nm was less than 5% in the size range (overall optical particle diameter) from 150 to 500 nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220 nm < D-rBC < 260 nm was 52 nm, resulting in a core-shell diameter ratio of 1.4, assuming a coated sphere morphology. Combining the aerosol absorption coefficient observed with an Aethalometer and the rBC mass concentration from the SP2, a mass absorption cross section (MAC) of 9.8 m(2) g(-1) was inferred at a wavelength of 550 nm. Consistent with direct observation, a similar MAC value (8.4m(2) g(-1) at 550 nm) was obtained indirectly by using Mie theory and assuming a coated-sphere morphology with the BC mixing state constrained from the SP2 measurements. According to these calculations, the lensing effect is estimated to cause a 54% enhancement of the MAC compared to that of bare BC particles with equal BC core size distribution. Finally, the ARTDECO radiative transfer model was used to estimate the sensitivity of the radiative balance to changes in light absorption by BC as a result of a varying degree of internal mixing at constant total BC mass. The clear-sky noontime aerosol radiative forcing over a surface with an assumed wavelength-dependent albedo of 0.76-0.89 decreased, when ignoring the absorption enhancement, by -0.12 Wm(-2) compared to the base case scenario, which was constrained with mean observed aerosol properties for the Zeppelin site in Arctic spring. The exact magnitude of this forcing difference scales with environmental conditions such as the aerosol optical depth, solar zenith angle and surface albedo. Nevertheless, our investigation suggests that the absorption enhancement due to internal mixing of BC, which is a systematic effect, should be considered for quantifying the aerosol radiative forcing in the Arctic region.