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Uptake of nitric acid, ammonia, and organics in orographic clouds: mass spectrometric analyses of droplet residual and interstitial aerosol particles

机译：地形云中硝酸，氨和有机物的吸收：液滴残留和间隙气溶胶颗粒的质谱分析

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Concurrent in situ analyses of interstitial aerosol andcloud droplet residues have been conducted at the Schmücke mountain siteduring the Hill Cap Cloud Thuringia campaign in central Germany in Septemberand October 2010. Cloud droplets were sampled from warm clouds (temperaturesbetween −3 and +16 °C) by a counterflow virtual impactor andthe submicron-sized residues were analyzed by a compact time-of-flight aerosolmass spectrometer (C-ToF-AMS), while the interstitial aerosol composition wasmeasured by an high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). During cloud-free periods, the submicron out-of-cloud aerosol was analyzed using both instruments, allowing for intercomparison between the two instruments. Further instrumentation included black carbon measurements and optical particle counters for the aerosol particles as well as optical sizinginstrumentation for the cloud droplets. The results show that, under cloudconditions, on average 85 % of the submicron aerosol mass partitioned intothe cloud liquid phase. Scavenging efficiencies of nitrate, ammonium,sulfate, and organics ranged between 60 and 100 %, with nitrate having, ingeneral, the highest values. For black carbon, the scavenging efficiency wasmarkedly lower (about 24 %). The nitrate and ammonium mass fractions werefound to be markedly enhanced in cloud residues, indicating uptake ofgaseous nitric acid and ammonia into the aqueous phase. This effect wasfound to be temperature dependent: at lower temperatures, the nitrate andammonium mass fractions in the residues were higher. Also, the oxidationstate of the organic matter in cloud residues was found to be temperaturedependent: the O : C ratio was lower at higher temperatures. A possibleexplanation for this observation is a more effective uptake and/or higherconcentrations of low-oxidized water-soluble volatile organic compounds,possibly of biogenic origin, at higher temperatures. Organic nitrates wereobserved in cloud residuals as well as in the out-of-cloud aerosol, but noindication of a preferred partitioning of organic nitrates into the aqueousphase or into the gas phase was detected. Assuming the uptake of nitric acidand ammonia in cloud droplets will be reversible, it will lead to aredistribution of nitrate and ammonium among the aerosol particles, leadingto more uniform, internally mixed particles after several cloud passages.
机译：2010年9月至2010年10月在德国中部的Hill Cap Cloud图林根州运动期间，在Schmücke山区对间隙气溶胶和云滴残留物进行了原位分析。用紧凑型飞行时间气溶胶质谱仪（C-ToF-AMS）分析了逆流虚拟撞击器和亚微米级残留物，同时通过高分辨率飞行时间气溶胶质谱仪（HR）测量了间质气溶胶成分-ToF-AMS）。在无云期间，使用这两种仪器分析了亚微米云雾气溶胶，从而可以在这两种仪器之间进行比较。进一步的仪器包括黑碳测量和用于气溶胶粒子的光学粒子计数器以及用于云滴的光学定径仪器。结果表明，在云条件下，平均有85％的亚微米气溶胶物质分配到云液相中。硝酸盐，铵，硫酸盐和有机物的清除效率介于60％至100％之间，其中硝酸盐通常具有最高的值。对于黑碳，清除效率明显较低（约24％）。发现硝酸盐和铵的质量分数在云状残留物中显着增强，表明气态硝酸和氨被吸收到水相中。发现该影响与温度有关：在较低温度下，残留物中的硝酸盐和铵质量分数较高。同样，发现云残留物中有机物的氧化态与温度有关：在较高的温度下，O 3：C比较低。该观察的可能解释是在较高温度下更有效地吸收和/或更高浓度的低氧化水溶性挥发性有机化合物（可能是生物来源的）。在云层残留物和云雾中观察到有机硝酸盐，但未发现有机硝酸盐在水相或气相中的优选分配。假设云滴中硝酸和氨的吸收是可逆的，这将导致硝酸盐和铵在气溶胶颗粒之间的分布，从而在经过几次云之后形成更均匀的内部混合颗粒。

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