Joint size and fall velocity distributions of raindrops were measured with a Particle Size and Velocity (PARSIVEL) precipitation particle disdrometer in a field experiment conducted during July and August 2007 at a semiarid continental site located in Guyuan, Ningxia Province, China (368N, 1068169E). Data from both stratiform and convective clouds are analyzed. Comparison of the observed raindrop size distributions shows that the increase of convective rain rates arises from the increases of both drop concentration and drop diameter while the increase of the rain rate in the stratiform clouds is mainly due to the increase of median and large drop concentration. Another striking contrast between the stratiform and convective rains is that the size distributions from the stratiform (convective) rains tend to narrow (broaden) with increasing rain rates. Statistical analysis of the distribution pattern shows that the observed size distributions from both rain types can be well described by the gamma distribution. Examination of the raindrop fall velocity reveals that the difference in air density leads to a systematic change in the drop fall velocity while organized air motions (updrafts and downdrafts), turbulence, drop breakup, and coalescence likely cause the large spread of drop fall velocity, along with additional systematic deviation from terminal velocity at certain raindrop diameters. Small (large) drops tend to have superterminal (subterminal) velocities statistically, with the positive deviation from the terminal velocity of small drops being much larger than the negative deviation of large drops.

Severe haze events during which particulate matter (PM) increases quickly from tens to hundreds of microgram per cubic meter in 1–2 days frequently occur in China. Although it has been known that PM is influenced by complex interplays among emissions, meteorology, and physical and chemical processes, specific mechanisms remain elusive. Here, a new positive feedback mechanism between planetary boundary layer (PBL), relative humidity (RH), and secondary PM (SPM) formation is proposed based on a comprehensive field experiment and model simulation. The decreased PBL associated with increased PM increases RH by weakening the vertical transport of water vapor; the increased RH in turn enhances the SPM formation through heterogeneous aqueous reactions, which further enhances PM, weakens solar radiation, and decreases PBL height. This positive feedback, together with the PM-Radiation-PBL feedback, constitutes a key mechanism that links PM, radiation, PBL properties (e.g. PBL height and RH), and SPM formation, This mechanism is self-amplifying, leading to faster PM production, accumulation, and more severe haze pollution.

h i g h l i g h t sHeterogeneous aqueous reactions during haze events was investigated. The conversion of gas-phase of S and N to particle-phase was analyzed. Relationships were given between conversion ratio of S, N with RH and O 3 . Evolution of aerosol composition and particle size were analyzed. a b s t r a c tThe effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM 2.5 ), nitrate (NO 3 ), sulfate (SO 4 ), ammonium (NH 4 )], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO 2 ), and ozone (O 3 )], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (N ratio ) and S from SO 2 to sulfate (S ratio ) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO 2 to their corresponding particle phases in the late haze period. Further analysis shows that N ratio and S ratio increased with increasing RH, with N ratio and S ratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60e80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of N ratio and S ratio to O 3 : the conversion ratios increase with decreasing O 3 concentration when O 3 concentration is lower than <15 ppb but increased with increasing O 3 when O 3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO 2 and NOx, accelerated the formation of secondary inorganic aerosols, and led to rapid increase of the PM 2.5 concentration.

Fog poses a severe environmental problem in the North China Plain, China, which has been witnessing increases in anthropogenic emission since the early 1980s. This work first uses the WRF/Chem model coupled with the local anthropogenic emissions to simulate and evaluate a severe fog event occurring in North China Plain. Comparison of the simulations against observations shows that WRF/Chem well reproduces the general features of temporal evolution of PM2.5 mass concentration, fog spatial distribution, visibility, and vertical profiles of temperature, water vapor content, and relative humidity in the planetary boundary layer throughout the whole period of the fog event. Sensitivity studies are then performed with five different levels of anthropogenic emission as model inputs to systematically examine the comprehensive impacts of aerosols on fog microphysical, macrophysical, radiative, and dynamical properties. The results show that as aerosol concentration increases, fog droplet number concentration and liquid water content all increase nonlinearly; but effective radius decreases. Macrophysical properties (fog fraction, fog duration, fog height, and liquid water path) also increase nonlinearly with increasing aerosol concentration, with rates of changes smaller than microphysical properties. Further analysis reveals distinct aerosol effects on thermodynamic and dynamical conditions during different stages of fog evolution: increasing aerosols invigorate fog formation and development by enhancing longwave‐induced instability, fog droplet condensation accompanying latent heat release, and thus turbulence, but delay fog dissipation by reducing surface solar radiation, surface sensible, and latent heat fluxes, and thus suppressing turbulence during the dissipation stage.

Wet scavenging of black carbon (BC) has been subject to large uncertainty, which importantly determines its atmospheric lifetime and indirect forcing impact on cloud microphysics. This study reveals the complex BC‐hydrometeor interactions in mixed‐phase clouds via single particle measurements in the real‐world environment, by capturing precipitation processes throughout cloud formation, cold rain/graupel, and subsequent snow events at a mountain site influenced by anthropogenic sources in wintertime. We found highly efficient BC wet scavenging during cloud formation, with large and thickly coated BC preferentially incorporated into droplets. During snow processes, BC core sizes in the interstitial phase steadily increased. A mechanism was proposed whereby the BC mass within each droplet was accumulated through droplet collision, leading to larger BC cores, which were then released back to the interstitial air through the Wegener‐Bergeron‐Findeisen processes when ice dominated. These results provide fundamental basis for constraining BC wet scavenging.

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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.Plain Language Summary The width of cloud droplet size distribution is critical to aerosol-cloud interactions and warm rain initiation. Relative dispersion represents the relative width of cloud droplet size distribution. Current parameterizations of relative dispersion often relate relative dispersion to volume-mean radius. Based on aircraft observations of cumulus clouds, it is found that relative dispersion is positively correlated with volume-mean radius when volume-mean radius is small, and the correlation becomes negative when volume-mean radius increases. A hypothesis is raised by relating the relationship between the two quantities to microphysical processes (activation, condensation, evaporation, and deactivation) and is substantiated with an adiabatic parcel model, a parcel model considering entrainment-mixing, and theoretical analysis. The results may promote the studies on the zone between cloudy and cloud-free air, which in turn affects evaluation of aerosol-cloud interactions.

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