The absorption Ångström exponent (AAE) is an important aerosol optical parameter used for aerosol characterization and apportionment studies. The AAE of black carbon (BC) particles is widely accepted to be 1.0, although observational estimates give quite a wide range of 0.6–1.3. With considerable uncertainties related to observations, a numerical study is a powerful method, if not the only one, to provide a better and more accurate understanding on BC AAE. This study calculates BC AAE using realistic particle geometries based on fractal aggregate and an accurate numerical optical model (namely the multiple-sphere T-matrix method), and considers bulk properties of an ensemble of BC particles following lognormal size distributions. At odds with the expectations, BC AAE is not 1.0, even when BC is assumed to have small sizes and a wavelength-independent refractive index. With a wavelength-independent refractive index, the AAE of fresh BC is approximately 1.05 and relatively insensitive to particle size. For BC with geometric mean diameters larger than 0.12 µm, BC AAE becomes smaller when BC particles are aged (compact structures or coated by other non-absorptive materials). For coated BC, we prescribe the coating fraction variation based on a laboratory study, where smaller BC cores are shown to develop larger coating fractions than those of bigger BC cores. For both compact and coated BC, the AAE is highly sensitive to particle size distribution, ranging from approximately 0.8 to even over 1.4 with wavelength-independent refractive index. When the refractive index is allowed to vary with wavelength, a feature with observational backing, the BC AAE may show an even wider range. For different BC morphologies, we derive simple empirical equations on BC AAE based on our numerical results, which can serve as a guide for the response of BC AAE to BC size and refractive index. Due to its complex influences, the effects of BC geometry is better to be discussed at certain BC properties, i.e., known size and refractive index.

Absorbing aerosols, like black carbon (BC), give rise to rapid adjustments, and the associated perturbation to the atmospheric temperature structure alters the cloud distribution. The level of scientific understanding of these rapid cloud adjustments—otherwise known as semi-direct effects (SDEs)—is considered low, with models indicating a likely negative (−0.44 to +0.1 Wm⁻²) forcing. Recent studies suggest this negative SDE is primarily driven by decreases in high-level clouds and enhanced longwave cooling. Here, we investigate the SDE using multiple models driven by observationally constrained fine-mode aerosol forcing without dust and sea salt. Unlike aerosol simulations, which yield a relatively vertically uniform aerosol atmospheric heating profile with significant upper-tropospheric heating, observation-based heating peaks in the lower-troposphere and then decays to zero in the mid-troposphere. We find a significant global annual mean decrease in low- and mid-level clouds, and weaker decreases in high-level clouds, which leads to a positive SDE dominated by shortwave radiation. Thus, in contrast to most studies, we find a robust positive SDE, implying cloud adjustments act to warm the climate system. Sensitivity tests with identical average, but vertically uniform observationally constrained aerosol atmospheric heating result in a negative SDE, due to enhanced longwave cooling as a result of large reductions in high-level clouds. Our results therefore suggest that model simulations lead to a negatively biased SDE, due to an aerosol atmospheric heating profile that is too vertically uniform.

Black carbon (BC) aerosols have often been assumed to be the only light-absorbing carbonaceous particles in the red and near-infrared spectral regions of solar radiation in the atmosphere. Here we report that tar balls (a specific type of organic aerosol particles from biomass burning) do absorb red and near-infrared radiation significantly. Tar balls were produced in a laboratory experiment, and their chemical and optical properties were measured. The absorption of these particles in the range between 470 and 950 nm was measured with an aethalometer, which is widely used to measure atmospheric aerosol absorption. We find that the absorption coefficient of tar balls at 880 nm is more than 10 % of that at 470 nm. The considerable absorption of red and infrared light by tar balls also follows from their relatively low absorption Ångström coefficient (and significant mass absorption coefficient) in the spectral range between 470 and 950 nm. Our results support the previous finding that tar balls may play an important role in global warming. Due to the non-negligible absorption of tar balls in the near-infrared region, the absorption measured in the field at near-infrared wavelengths cannot solely be due to soot particles.

Small aerosols are mostly anthropogenic, and the fine-mode aerosol optical depth (fAOD) can be used to infer anthropogenic aerosol amounts. We estimate AOD and fAOD globally on a monthly time scale from 2001 to 2010 by integrating monthly satellite-based (MODIS and MISR) and ground-based (AERONET) observations. For fAOD, three integration methods are developed to utilize global coverage by satellite data and maximize the influence of AERONET data. We evaluate each method by applying the method without a few randomly-chosen AERONET data and comparing its output with the few AERONET data. The best method of the three is based on integrating the Ångström exponent (AE) data from MODIS, MISR and AERONET, and its output is closer to AERONET fAOD accuracy than MODIS or MISR fAOD over both ocean and land. Using our integrated data, we find that the global 2001–2010 average of 500 nm AOD and fAOD is 0.17 and 0.089, respectively. Eastern China as a region shows the largest decadal-mean fAOD. The linear trend of global AOD or global fAOD from 2001 to 2010 is found to be slightly negative. This decreasing trend is particularly pronounced over the West (Western Europe and US/Canada combined) where AOD and fAOD reductions are about −20%. By contrast, fAOD in India and eastern China combined increased slightly. These results reflect the overall anthropogenic aerosol emission reduction in the West, and stagnating conditions in Asia. Moreover, our results in the West are consistent with the so-called surface brightening phenomenon in the recent decades.

There has been growing interest in the vertical structure of the recent Arctic warming. We investigated temperatures at the surface, 925, 700, 500 and 300 hPa levels in the Arctic (north of 70° N) using observations and four reanalyses: ERA-Interim, CFSR, MERRA and NCEP II. For the period 1979–2011, the layers at 500 hPa and below show a warming trend in all seasons in all the chosen reanalyses and observations. Restricting the analysis to the 1998–2011 period, however, all the reanalyses show a cooling trend in the Arctic-mean 500 hPa temperature in autumn, and this also applies to both observations and the reanalyses when restricting the analysis to the locations with available IGRA radiosoundings. During this period, the surface observations mainly representing land areas surrounding the Arctic Ocean reveal no summertime trend, in contrast with the reanalyses whether restricted to the locations of the available surface observations or not. In evaluating the reanalyses with observations, we find that the reanalyses agree better with each other at the available IGRA sounding locations than for the Arctic average, perhaps because the sounding observations were assimilated into reanalyses. Conversely, using the reanalysis data only from locations matching available surface (air) temperature observations does not improve the agreement between the reanalyses. At 925 hPa, CFSR deviates from the other three reanalyses, especially in summer after 2000, and it also deviates more from the IGRA radiosoundings than the other reanalyses do. The CFSR error in summer T925 is due mainly to underestimations in the Canadian-Atlantic sector between 120° W and 0°. The other reanalyses also have negative biases in this longitude band.

Aerosols directly affect the radiative balance of the Earth through the absorption and scattering of solar radiation. Although the contributions of absorption (heating) and scattering (cooling) of sunlight have proved difficult to quantify, the consensus is that anthropogenic aerosols cool the climate, partially offsetting the warming by rising greenhouse gas concentrations. Recent estimates of global direct anthropogenic aerosol radiative forcing (i.e., global radiative forcing due to aerosol–radiation interactions) are −0.35 ± 0.5 W m⁻², and these estimates depend heavily on aerosol simulation. Here, we integrate a comprehensive suite of satellite and ground-based observations to constrain total aerosol optical depth (AOD), its fine-mode fraction, the vertical distribution of aerosols and clouds, and the collocation of clouds and overlying aerosols. We find that the direct fine-mode aerosol radiative effect is −0.46 W m⁻² (−0.54 to −0.39 W m⁻²). Fine-mode aerosols include sea salt and dust aerosols, and we find that these natural aerosols result in a very large cooling (−0.44 to −0.26 W m⁻²) when constrained by observations. When the contribution of these natural aerosols is subtracted from the fine-mode radiative effect, the net becomes −0.11 (−0.28 to +0.05) W m⁻². This net arises from total (natural + anthropogenic) carbonaceous, sulfate and nitrate aerosols, which suggests that global direct anthropogenic aerosol radiative forcing is less negative than −0.35 W m⁻².