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.

To understand the impact of firework-burning (FW) particles on air quality and human health during the winter haze period, 39 elements, 10 water-soluble ions and 8 fractions of carbonaceous species in atmospheric PM_2.5 in Nanjing were investigated during the 2014 Chinese Spring Festival (SF). Serious regional haze pollution persisted throughout the entire sampling period, with PM_2.5 averaging at 113 ± 69 μg m⁻³ and visibility at 4.8 ± 3.2 km. The holiday effect led to almost all the chemical species decreasing during the SF, except for Al, K, Ba and Sr which were related to FW. The source contributions of coal combustion, vehicle emission and road dust decreased dramatically, whereas FW contributed to about half of the PM_2.5 during the SF period. The intensive emission of FW particles on New Year's Eve accounted for 60.1% of the PM_2.5. Fireworks also obviously modified the chemical compositions of PM_2.5, with 39.3% contributed by increased organic matter, followed by steadily increased loadings of secondary inorganic ions. The aging processes of the FW particles lasted for about 4 days reflected by the variations of Ba, Sr, NH₄⁺, NO₃⁻, SO₄²⁻ and K⁺, characterized by heterogeneous reactions of SO₂ and NO_x on crustal materials directly from FW, the replacement of Cl⁻ by NO₃⁻ and SO₄²⁻, coating of NO₃⁻ and SO₄²⁻ on soot, formation of secondary organic aerosols and metal-catalyzed formation of NO₃⁻ and SO₄²⁻ at higher relative humidity. During aging, the main contributors to the extinction coefficient shifted from elemental carbon and organic matter to ammonium sulfate. The particles raised higher cancer risk of 1.62 × 10⁻⁶ by heavy metals (especially for Cd and As). This study provided detailed composition data and first comprehensive analysis of the aging processes of FW particles during the serious haze pollution period and their potential impact on human health.

Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM_2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM₁), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM₁ mass on average, accounting for 63–82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM₁ (6.4 m² g^-1) than during CPs (4.4 m² g^-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM_2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

Cloud droplet spectral relative dispersion is critical to parameterizations of cloud radiative properties, warm‐rain initiation, and aerosol‐cloud interactions in models; however, there is no consistent relationship between relative dispersion and volume‐mean radius in literature, which hinders improving relative dispersion parameterization and calls for physical explanation. Here we show, by analyzing aircraft observations of cumulus clouds during Routine AAF [Atmospheric Radiation Measurement (ARM) Aerial Facility] Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations, that the correlation between relative dispersion and volume‐mean radius changes from positive to negative as volume‐mean radius increases. With the new observation, we postulate that the sign of the correlation is determined by whether or not condensation (evaporation) occurs simultaneously with significant new activation (deactivation). The hypothesis is validated by simulations of both an adiabatic cloud parcel model and a parcel model accounting for entrainment‐mixing. A new quantity, first bin strength, is introduced to quantify this new observation. Theoretical analysis of truncated gamma and modified gamma size distributions further supports the hypothesis and reconciles the contrasting relationships between relative dispersion and volume‐mean radius, including the results in polluted fog observations. The results could shed new light on the so‐called “twilight zone” between cloudy and cloud‐free air, which in turn affects evaluation of aerosol‐cloud interactions and retrieval of aerosol optical depth.

The Moderate Resolution Imaging Spectroradiometer (MODIS) C6 L3, Clouds and the Earth's Radiant Energy System (CERES) Edition-4 L3 products, and the European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-Interim reanalysis data are employed to systematically study aerosol–cloud correlations over three anthropogenic aerosol regions and their adjacent oceans, as well as explore the effect of retrieval artifacts and underlying physical mechanisms. This study is confined to warm phase and single-layer clouds without precipitation during the summertime (June, July, and August). Our analysis suggests that cloud effective radius (CER) is positively correlated with aerosol optical depth (AOD) over land (positive slopes), but negatively correlated with aerosol index (AI) over oceans (negative slopes) even with small ranges of liquid water path (quasi-constant). The changes in albedo at the top of the atmosphere (TOA) corresponding to aerosol-induced changes in CER also lend credence to the authenticity of this opposite aerosol–cloud correlation between land and ocean. It is noted that potential artifacts, such as the retrieval biases of both cloud (partially cloudy and 3-D-shaped clouds) and aerosol, can result in a serious overestimation of the slope of CER–AOD/AI. Our results show that collision–coalescence seems not to be the dominant cause for positive slope over land, but the increased CER caused by increased aerosol might further increase CER by initializing collision–coalescence, generating a positive feedback. By stratifying data according to the lower tropospheric stability and relative humidity near cloud top, it is found that the positive correlations more likely occur in the case of drier cloud top and stronger turbulence in clouds, while negative correlations occur in the case of moister cloud top and weaker turbulence in clouds, which implies entrainment mixing might be a possible physical interpretation for such a positive CER–AOD slope.