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We integrated Enviro-HIRLAM (Environment-High Resolution Limited Area Model) meteorological output into FLEXPART (FLEXible PARTicle dispersion model). A FLEXPART simulation requires meteorological input from a numerical weather prediction (NWP) model. The publicly available version of FLEXPART can utilize either ECMWF (European Centre for Medium-range Weather Forecasts) Integrated Forecast System (IFS) forecast or reanalysis NWP data, or NCEP (U.S. National Center for Environmental Prediction) Global Forecast System (GFS) forecast or reanalysis NWP data. The primary benefits of using Enviro-HIRLAM are that it runs at a higher resolution and accounts for aerosol effects in meteorological fields. We compared backward trajectories generated with FLEXPART using Enviro-HIRLAM (both with and without aerosol effects) to trajectories generated using NCEP GFS and ECMWF IFS meteorological inputs, for a case study of a heavy haze event which occurred in Beijing, China in November 2018. We found that results from FLEXPART were considerably different when using different meteorological inputs. When aerosol effects were included in the NWP, there was a small but noticeable difference in calculated trajectories. Moreover, when looking at potential emission sensitivity instead of simply expressing trajectories as lines, additional information, which may have been missed when looking only at trajectories as lines, can be inferred.

Abstract New particle formation (NPF) is a global phenomenon that significantly influences climate. NPF also contributes to haze, with pronounced negative impacts on human health. Theory and observations both show that nucleation is favored during clean days and inhibited during haze episodes due to a high pre‐existing condensation sink (CS). Here we show that the surprising occurrence of NPF during haze days in Beijing is associated with a high concentration of sulfuric acid dimers. With both field observations and model simulations, we demonstrate that downward mixing of sulfur dioxide (SO2) from the residual layer aloft enhances ground level SO2, which in turn elevates sulfuric acid dimer after rapid SO2 oxidation in the polluted air. Our results address a key gap between the source of SO2 and its atmospheric oxidation products during haze conditions in a megacity, Beijing, providing a missing link in a complete chain describing NPF in the polluted atmosphere.

Abstract The role of new particle formation (NPF) events and their contribution to haze formation through subsequent growth in polluted megacities is still controversial. To improve the understanding of the sources, meteorological conditions, and chemistry behind air pollution, we performed simultaneous measurements of aerosol composition and particle number size distributions at ground level and at 260 m in central Beijing, China, during a total of 4 months in 2015–2017. Our measurements show a pronounced decoupling of gas-to-particle conversion between the two heights, leading to different haze processes in terms of particle size distributions and chemical compositions. The development of haze was initiated by the growth of freshly formed particles at both heights, whereas the more severe haze at ground level was connected directly to local primary particles and gaseous precursors leading to higher particle growth rates. The particle growth creates a feedback loop, in which a further development of haze increases the atmospheric stability, which in turn strengthens the persisting apparent decoupling between the two heights and increases the severity of haze at ground level. Moreover, we complemented our field observations with model analyses, which suggest that the growth of NPF-originated particles accounted up to ∼60% of the accumulation mode particles in the Beijing–Tianjin–Hebei area during haze conditions. The results suggest that a reduction in anthropogenic gaseous precursors, suppressing particle growth, is a critical step for alleviating haze although the number concentration of freshly formed particles (3–40 nm) via NPF does not reduce after emission controls.

We characterized new particle formation (NPF) events in the urban background of Amman during August 2016−July 2017. The monthly mean of submicron particle number concentration was 1.2 × 104−3.7 × 104 cm−3 (exhibited seasonal, weekly, and diurnal variation). Nucleation mode (10−15 nm) concentration was 0.7 × 103−1.1 × 103 cm−3 during daytime with a sharp peak (1.1 × 103−1.8 × 103 cm−3) around noon. We identified 110 NPF events (≈34% of all days) of which 55 showed a decreasing mode diameter after growth. The NPF event occurrence was higher in summer than in winter, and events were accompanied with air mass back trajectories crossing over the Eastern Mediterranean. The mean nucleation rate (J10) was 1.9 ± 1.1 cm−3 s−1 (monthly mean 1.6−2.7 cm−3 s−1) and the mean growth rate was 6.8 ± 3.1 nm/h (4.1−8.8 nm/h). The formation rate did not have a seasonal pattern, but the growth rate had a seasonal variation (maximum around August and minimum in winter). The mean condensable vapor source rate was 4.1 ± 2.2 × 105 molecules/cm3 s (2.6−6.9 × 105 molecules/cm3 s) with a seasonal pattern (maximum around August). The mean condensation sink was 8.9 ± 3.3 × 10−3 s−1 (6.4−14.8 × 10−3 s−1) with a seasonal pattern (minimum around June and maximum in winter).

Organic aerosol (OA) is a major component of fine particulate matter (PM) affecting air quality, human health, and the climate. The bsorptive and reflective behavior of OA components contributes to determining particle optical properties and thus their effects on the radiative budget of the troposphere. There is limited knowledge on the influence of the molecular composition of OA on particle optical properties in the polluted urban environment. In this study, we characterized the molecular composition of oxygenated OA collected on filter samples in autumn of 2018 in Beijing, China, with a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO-CIMS). Three haze episodes occurred during our sampling period with daily maximum concentrations of OA of 50, 30, and 55 µg m[sup -3], respectively. We found that the signal intensities of dicarboxylic acids and sulfur-containing compounds increased during the two more intense haze episodes, while the relative contributions of wood-burning markers and other aromatic compounds were enhanced during the cleaner periods. We further assessed the optical properties of oxygenated OA components by combining the detailed chemical composition measurements with collocated particle light absorption measurements. We show that light-absorption enhancement (E[sub abs]) of black carbon (BC) was mostly related to more oxygenated OA (e.g. dicarboxylic acids), likely formed in aqueous-phase reactions during the intense haze periods with higher relative humidity, and speculate that they might contribute to lensing effects. Aromatics and nitro-aromatics (e.g. nitrocatechol and its derivatives) were mostly related to a high light absorption coefficient (b[sub abs]) consistent with light-absorbing (brown) carbon (BrC). Our results provide information on oxygenated OA components at the molecular level associated with BrC and BC particle light-absorption and can serve as a basis for further studies on the effects of anthropogenic OA on radiative forcing in the urban environment. [ABSTRACT FROM AUTHOR]

Despite the numerous studies investigating haze formation mechanism in China, it is still puzzling that intensive haze episodes could form within hours directly following relatively clean periods. Haze has been suggested to be initiated by the variation of meteorological parameters and then to be substantially enhanced by aerosol-radiation-boundary layer feedback. However, knowledge on the detailed chemical processes and the driving factors for extensive aerosol mass accumulation during the feedback is still scarce. Here, the dependency of the aerosol number size distribution, mass concentration and chemical composition on the daytime mixing layer height (MLH) in urban Beijing is investigated. The size distribution and chemical composition-resolved dry aerosol light extinction is also explored. The results indicate that the aerosol mass concentration and fraction of nitrate increased dramatically when the MLH decreased from high to low conditions, corresponding to relatively clean and polluted conditions, respectively. Particles having their dry diameters in the size of ~ 400-700 nm, and especially particle- phase ammonium nitrate and liquid water, contributed greatly to visibility degradation during the winter haze periods. The dependency of aerosol composition on the MLH revealed that ammonium nitrate and aerosol water content increased the most during low MLH conditions, which may have further triggered enhanced formation of sulphate and organic aerosol via heterogeneous reactions. As a result, more sulphate, nitrate and water soluble organics were formed, leading to an enhanced water uptake ability and increased light extinction by the aerosols. The results of this study contribute towards a more detailed understanding of the aerosol-chemistry-radiation-boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing. [ABSTRACT FROM AUTHOR]