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Spring and summer contrast in new particle formation over nine forest areas in North America

机译:北美地区九个森林地区春季和夏季形成新的颗粒形成对比

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摘要

Recent laboratory chamber studies indicate a significant role forhighly oxidized low-volatility organics in new particle formation (NPF), butthe actual role of these highly oxidized low-volatility organics inatmospheric NPF remains uncertain. Here, particle size distributions (PSDs)measured in nine forest areas in North America are used to characterize theoccurrence and intensity of NPF and to evaluate model simulations using anempirical formulation in which formation rate is a function of theconcentrations of sulfuric acid and low-volatility organics fromalpha-pinene oxidation (Nucl-Org), and using an ion-mediated nucleationmechanism (excluding organics) (Nucl-IMN). On average, NPF occurred on~ 70 % of days during March for the four forest sites withspringtime PSD measurements, while NPF occurred on only ~ 10 % of days in July for all nine forest sites. Both Nucl-Org and Nucl-IMNschemes capture the observed high frequency of NPF in spring, but theNucl-Org scheme significantly overpredicts while the Nucl-IMN schemeslightly underpredicts NPF and particle number concentrations in summer.Statistical analyses of observed and simulated ultrafine particle numberconcentrations and frequency of NPF events indicate that the scheme withoutorganics agrees better overall with observations. The two schemes predictquite different nucleation rates (including their spatial patterns),concentrations of cloud condensation nuclei, and aerosol first indirectradiative forcing in North America, highlighting the need to reduce NPFuncertainties in regional and global earth system models.
机译:最近的实验室研究表明,高氧化低挥发性有机物在新颗粒形成(NPF)中起着重要作用,但这些高氧化低挥发性有机物在大气NPF中的实际作用仍不确定。在这里,使用北美9个森林地区测得的粒径分布(PSDs)来表征NPF的发生和强度,并使用经验公式评估模型模拟,其中形成速率是硫酸和低挥发性有机物浓度的函数由α-pine烯氧化(Nucl-Org),并使用离子介导的成核机理(不包括有机物)(Nucl-IMN)。平均而言,对四个森林站点进行春季PSD测量后,NPF发生在3月的约70%的日子中,而对于所有9个森林站点,NPF发生在7月的仅约10%的天中。 Nucl-Org和Nucl-IMN方案都捕获了春季观测到的NPF的高频率,但Nucl-Org方案明显超额预测,而Nucl-IMN方案则略微低估了夏季的NPF和颗粒数浓度。 NPF事件的发生频率表明,没有有机物的计划在总体上与观察结果更吻合。这两种方案预测了北美的成核速率(包括其空间模式),云凝结核的浓度以及气溶胶的首次间接辐射强迫将有很大不同,这凸显了减少区域和全球地球系统模型中NPF不确定性的必要性。

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