Atmospheric new particle formation (NPF) is an important global phenomenon that is nevertheless sensitive to ambient conditions. According to both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (HSO) concentration to promote the formation of new particles and a low preexisting aerosol loading to minimize the sink of new particles. We investigated NPF in Shanghai and were able to observe both precursor vapors (HSO) and initial clusters at a molecular level in a megacity. High NPF rates were observed to coincide with several familiar markers suggestive of HSO-dimethylamine (DMA)-water (HO) nucleation, including sulfuric acid dimers and HSO-DMA clusters. In a cluster kinetics simulation, the observed concentration of sulfuric acid was high enough to explain the particle growth to ~3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result from the added contribution of condensing organic species. These findings will help in understanding urban NPF and its air quality and climate effects, as well as in formulating policies to mitigate secondary particle formation in China.

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Abstract. Long-term measurements of aerosol optical depths (AODs) at 440 nm and Ångström exponents (AE) between 440 and 870 nm made for CARSNET were compiled into a climatology of aerosol optical properties for China. Quality-assured monthly mean AODs are presented for 50 sites representing remote, rural, and urban areas. AODs were 0.14, 0.34, 0.42, 0.54, and 0.74 at remote stations, rural/desert regions, the Loess Plateau, central and eastern China, and urban sites, respectively, and the corresponding AE values were 0.97, 0.55, 0.82, 1.19, and 1.05. AODs increased from north to south, with low values (< 0.20) over the Tibetan Plateau and northwestern China and high AODs (> 0.60) in central and eastern China where industrial emissions and anthropogenic activities were likely sources. AODs were 0.20–0.40 in semi-arid and arid regions and some background areas in northern and northeastern China. AEs were > 1.20 over the southern reaches of the Yangtze River and at clean sites in northeastern China. In the northwestern deserts and industrial parts of northeast China, AEs were lower (< 0.80) compared with central and eastern regions. Dust events in spring, hygroscopic particle growth during summer, and biomass burning contribute the high AODs, especially in northern and eastern China. The AODs show decreasing trends from 2006 to 2009 but increased ~ 0.03 per year from 2009 to 2013.

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[1] Ozone and its precursors were measured from 15 June 2006 to 14 June 2007 at an urban site in Shanghai and used to characterize photochemical oxidant production in this region. During the observation period, ozone displays a seasonal variation with a maximum in spring. Observed nitrogen oxides (NOx) and carbon monoxide (CO) reached a maximum in winter and a minimum in summer. NOx and CO has a similar double-peak diurnal cycle, implying that they are largely of motor vehicle origin. Total nonmethane organic compounds (NMOC) concentrations averaged over the morning, and the 24-hour periods have a large day-to-day variation with no apparent seasonal cycle. Aromatics play a dominant role in contributing to total NMOC reactivity and ozone-forming potential. Anthropogenic NMOC of diverse sources are major components of total NMOC and consist mainly of moderate and low reactivity species. In contrast, relatively low levels of biogenic NMOC concentrations were observed in urban Shanghai. The early morning NMOC/NOx ratios are typically below 8:1 with an average of around 4:1, indicating that the sampling location is situated in a NMOC-limited regime. Model simulations confirm that potential photochemical ozone production in Shanghai is NMOC-sensitive. It is presently difficult to predict the impact of future human activities, such as the increase of automobiles and vegetation-covered landscapes and the reduction of aerosol on ozone pollution in the fast developing megacities of China, and additional studies are needed to better understand the highly nonlinear ozone problem.

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Abstract. Amines and amides are important atmospheric organic-nitrogen compounds but high time resolution, highly sensitive, and simultaneous ambient measurements of these species are rather sparse. Here, we present the development of a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) method, utilizing protonated ethanol as reagent ions to simultaneously detect atmospheric gaseous amines (C1 to C6) and amides (C1 to C6). This method possesses sensitivities of 5.6–19.4 Hz pptv−1 for amines and 3.8–38.0 Hz pptv−1 for amides under total reagent ion signals of  ∼  0.32 MHz. Meanwhile, the detection limits were 0.10–0.50 pptv for amines and 0.29–1.95 pptv for amides at 3σ of the background signal for a 1 min integration time. Controlled characterization in the laboratory indicates that relative humidity has significant influences on the detection of amines and amides, whereas the presence of organics has no obvious effects. Ambient measurements of amines and amides utilizing this method were conducted from 25 July to 25 August 2015 in urban Shanghai, China. While the concentrations of amines ranged from a few parts per trillion by volume to hundreds of parts per trillion by volume, concentrations of amides varied from tens of parts per trillion by volume to a few parts per billion by volume. Among the C1- to C6-amines, the C2-amines were the dominant species with concentrations up to 130 pptv. For amides, the C3-amides (up to 8.7 ppb) were the most abundant species. The diurnal and backward trajectory analysis profiles of amides suggest that in addition to the secondary formation of amides in the atmosphere, industrial emissions could be important sources of amides in urban Shanghai. During the campaign, photo-oxidation of amines and amides might be a main loss pathway for them in daytime, and wet deposition was also an important sink.

Developing red thermally activated delayed fluorescence (TADF) emitters,a ttainable for both high-efficient red organic light-emitting diodes (OLEDs) and non-doped deep red/near-infrared (NIR) OLEDs,ischallenging. Now,two red emitters,B PPZ-PXZ and mDPBPZ-PXZ, with twisted donor-acceptor structures were designed and synthesized to study molecular design strategies of high-efficiency red TADF emitters.B PPZ-PXZ employs the strictest molecular restrictions to suppress energy loss and realizes red emission with aphotoluminescence quantum yield (F PL )of100 AE 0.8 %and external quantum efficiency (EQE) of 25.2 %i nadoped OLED.Its non-doped OLED has an EQE of 2.5 %owingto unavoidable intermolecular p-p interactions.mDPBPZ-PXZ releases two pyridine substituents from its fused acceptor moiety.A lthough mDPBPZ-PXZ realizes al ower EQE of 21.7 %i nt he doped OLED,i ts non-doped device shows asuperior EQE of 5.2 %with adeep red/NIR emission at peak of 680 nm.