Abstract. Aerosol hygroscopicity is crucial for understanding roles of aerosol particles in atmospheric chemistry and aerosol climate effects. Light-scattering enhancement factor f (RH, λ) is one of the parameters describing aerosol hygroscopicity, which is defined as f (RH, λ) = σ sp (RH, λ)/σ sp (dry, λ), where σ sp (RH, λ) or σ sp (dry, λ) represents σ sp at wavelength λ under certain relative humidity (RH) or dry conditions. Traditionally, an overall hygroscopicity parameter κ can be retrieved from measured f (RH, λ), hereinafter referred to as κ f (RH) , by combining concurrently measured particle number size distribution (PNSD) and mass concentration of black carbon. In this paper, a new method is proposed to directly derive κ f (RH) based only on measurements from a three-wavelength humidified nephelometer system. The advantage of this newly proposed approach is that κ f (RH) can be estimated without any additional information about PNSD and black carbon. This method is verified with measurements from two different field campaigns. Values of κ f (RH) estimated from this new method agree very well with those retrieved by using the traditional method: all points lie near the 1 : 1 line and the square of correlation coefficient between them is 0.99. The verification results demonstrate that this newly proposed method of deriving κ f (RH) is applicable at different sites and in seasons of the North China Plain and might also be applicable in other regions around the world.

Abstract. The hygroscopicity of organic aerosol (OA) is important for investigation of its climatic and environmental impacts. However, the hygroscopicity parameter κOA remains poorly characterized, especially in the relatively polluted environment on the North China Plain (NCP). Here we conducted simultaneous wintertime measurements of bulk aerosol chemical compositions of PM2.5 and PM1 and bulk aerosol hygroscopicity of PM10 and PM1 on the NCP using a capture-vaporizer time-of-flight aerosol chemical speciation monitor (CV-ToF-ACSM) and a humidified nephelometer system which measures the aerosol light-scattering enhancement factor f(RH). A method for calculating κOA based on f(RH) and bulk aerosol chemical-composition measurements was developed. We found that κOA varied in a wide range with significant diurnal variations. The derived κOA ranged from almost 0.0 to 0.25, with an average (±1σ) of 0.08 (±0.06) for the entire study. The derived κOA was highly correlated with f44 (fraction of m∕z 44 in OA measured by CV-ToF-ACSM), an indicator of the oxidation degree of OA (R=0.79), and the relationship can be parameterized as κOA=1.04×f44-0.02 (κOA=0.3×O:C-0.02, based on the relationship between the f44 and O∕C ratio for CV-ToF-ACSM). On average, κOA reached the minimum (0.02) in the morning near 07:30 local time (LT) and then increased rapidly, reaching the peak value of 0.16 near 14:30 LT. The diurnal variations in κOA were highly and positively correlated with those of mass fractions of oxygenated OA (R=0.95), indicating that photochemical processing played a dominant role in the increase in κOA in winter on the NCP. Results in this study demonstrate the potential wide applications of a humidified nephelometer system together with aerosol composition measurements for investigating the hygroscopicity of OA in various environments and highlight that the parameterization of κOA as a function of OA aging processes needs to be considered in chemical transport models for better evaluating the impacts of OA on cloud formation, atmospheric chemistry, and radiative forcing.

Abstract. The study of atmospheric nitrous acid (HONO), which is the primary source of OH radicals, is crucial with respect to understanding atmospheric photochemistry and heterogeneous chemical processes. Heterogeneous NO2 chemistry under haze conditions has been identified as one of the missing sources of HONO on the North China Plain, and also produces sulfate and nitrate. However, controversy exists regarding the various proposed HONO production mechanisms, mainly regarding whether SO2 directly takes part in the HONO production process and what roles NH3 and the pH value play. In this paper, never before seen explosive HONO production was reported and evidence was found – for the first time in field measurements during fog (usually with 4< pH <6) and haze episodes under high relative humidity (pH ≈4) – that NH3 was the key factor that promoted the hydrolysis of NO2, leading to the explosive growth of HONO and nitrate under both high and relatively lower pH conditions. The results also suggest that SO2 plays a minor or insignificant role in HONO formation during fog and haze events, but was indirectly oxidized upon the photolysis of HONO via subsequent radical mechanisms. Aerosol hygroscopicity significantly increased with rapid inorganic secondary aerosol formation, further promoting HONO production as a positive feedback. For future photochemical and aerosol pollution abatement, it is crucial to introduce effective NH3 emission control measures, as NH3-promoted NO2 hydrolysis is a large daytime HONO source, releasing large amounts of OH radicals upon photolysis, which will contribute largely to both atmospheric photochemistry and secondary aerosol formation.

Abstract. Water condensed on ambient aerosol particles plays significant roles in atmospheric environment, atmospheric chemistry and climate. Before now, no instruments were available for real-time monitoring of ambient aerosol liquid water contents (ALWCs). In this paper, a novel method is proposed to calculate ambient ALWC based on measurements of a three-wavelength humidified nephelometer system, which measures aerosol light scattering coefficients and backscattering coefficients at three wavelengths under dry state and different relative humidity (RH) conditions, providing measurements of light scattering enhancement factor f(RH). The proposed ALWC calculation method includes two steps: the first step is the estimation of the dry state total volume concentration of ambient aerosol particles, Va(dry), with a machine learning method called random forest model based on measurements of the “dry” nephelometer. The estimated Va(dry) agrees well with the measured one. The second step is the estimation of the volume growth factor Vg(RH) of ambient aerosol particles due to water uptake, using f(RH) and the Ångström exponent. The ALWC is calculated from the estimated Va(dry) and Vg(RH). To validate the new method, the ambient ALWC calculated from measurements of the humidified nephelometer system during the Gucheng campaign was compared with ambient ALWC calculated from ISORROPIA thermodynamic model using aerosol chemistry data. A good agreement was achieved, with a slope and intercept of 1.14 and −8.6 µm3 cm−3 (r2 = 0.92), respectively. The advantage of this new method is that the ambient ALWC can be obtained solely based on measurements of a three-wavelength humidified nephelometer system, facilitating the real-time monitoring of the ambient ALWC and promoting the study of aerosol liquid water and its role in atmospheric chemistry, secondary aerosol formation and climate change.

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SummaryAnalyses of genome variations with high-throughput assays have improved our understanding of genetic basis of crop domestication and identified the selected genome regions, but little is known about that of modern breeding, which has limited the usefulness of massive elite cultivars in further breeding. Here we deploy pedigree-based analysis of an elite rice, Huanghuazhan, to exploit key genome regions during its breeding. The cultivars in the pedigree were resequenced with 7.69 depth on average, and 2.1 million high-quality single nucleotide polymorphisms (SNPs) were obtained. Tracing the derivation of genome blocks with pedigree and information on SNPs revealed the chromosomal recombination during breeding, which showed that 26.22% of Huanghuazhan genome are strictly conserved key regions. These major effect regions were further supported by a QTL mapping of 260 recombinant inbred lines derived from the cross of Huanghuazhan and a very dissimilar cultivar, Shuanggui 36, and by the genome profile of eight cultivars and 36 elite lines derived from Huanghuazhan. Hitting these regions with the cloned genes revealed they include numbers of key genes, which were then applied to demonstrate how Huanghuazhan were bred after 30 years of effort and to dissect the deficiency of artificial selection. We concluded the regions are helpful to the further breeding based on this pedigree and performing breeding by design. Our study provides genetic dissection of modern rice breeding and sheds new light on how to perform genomewide breeding by design.

Water vapor supersaturation, as one of the most important environmental parameters during the formation of clouds or fogs, cannot be directly measured, and few studies have been carried out to estimate it in the ambient activation process. In this study, a new method to estimate the water vapor supersaturation based on the inverse application of κ‐Köhler theory is proposed. Aerosol hygroscopic parameter κ, dry particle size distributions, and wet droplet size distributions were employed and a comparison of predicted droplet number concentration with the measurement results was made to obtain the effective supersaturation during the activation process. Using this method, we acquired the supersaturations varying from 0.01% to 0.05% in a fog episode observed in the North China Plain. In this fog episode, both hydrated unactivated droplets and activated droplets play a part in the total detected droplet number concentrations with the unactivated droplets' ratio decreasing with size. The sensitivity study was also made to evaluate the effects of droplet and aerosol hygroscopic measurement errors on the supersaturation ratio estimation. Water vapor supersaturation obtained with this method can be regarded as an effective value and can be further applied to cloud analysis in the future. This method is only based on conventional measurements of aerosol and droplets and does not rely on any other data, which makes it flexible and easy to perform. Calculated supersaturations and critical diameters can also deepen the understanding of ambient activation process and corresponding interactions between aerosol and droplet characteristics.

Abstract. Light detection and ranging (lidar) measurements have been widely used to profile the ambient aerosol extinction coefficient (σ ext ). The particle extinction-to-backscatter ratio (lidar ratio, LR), which strongly depends on the aerosol dry particle number size distribution (PNSD) and aerosol hygroscopicity, is introduced to retrieve the σ ext profile from elastic-backscatter lidar signals. Conventionally, a constant column-integrated LR that is estimated from aerosol optical depth is used by the retrieving algorithms. In this paper, the influences of aerosol PNSD, aerosol hygroscopic growth and relative humidity (RH) profiles on the variation in LR are investigated based on the datasets from field measurements in the North China Plain (NCP). Results show that LR has an enhancement factor of 2.2 when RH reaches 92 %. Simulation results indicate that both the magnitude and vertical structures of the σ ext profiles by using the column-related LR method are significantly biased from the original σ ext profile. The relative bias, which is mainly influenced by RH and PNSD, can reach up to 40 % when RH at the top of the mixed layer is above 90 %. A new algorithm for retrieving σ ext profiles and a new scheme of LR enhancement factor by RH in the NCP are proposed in this study. The relative bias between the σ ext profile retrieved with this new algorithm and the ideal true value is reduced to below 13 %.