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Emissions of biogenic volatile organic compounds and subsequent formation of secondary organic aerosols in a Larix kaempferi forest

机译：落叶松森林中生物挥发性有机化合物的排放及随后形成的次级有机气溶胶

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We conductedsimultaneous measurements of concentrations and above-canopy fluxes ofisoprene and α-pinene, along with their oxidation products in aerosolsin a (Japanese larch) forest in summer 2012.Vertical profiles of isoprene showed the maximum concentration near theforest floor with a peak around noon, whereas oxidation products of isoprene,i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), showed higherconcentrations near the canopy level of the forest. The vertical profilesuggests large emissions of isoprene near the forest floor, likely due to (a fern species), and the subsequentreaction within the canopy. The concentrations of α-pinene also showedhighest values near the forest floor, with maximums in the early morning andlate afternoon. The vertical profiles of α-pinene suggest its largeemissions from soil and litter in addition to emissions from leaves at the forest site. Isoprene and its oxidation products inaerosols exhibited similar diurnal variations within the forest canopy,providing evidence of secondary organic aerosol (SOA) formation via oxidationof isoprene most likely emitted from the forest floor. Although highabundance of α-pinene was observed in the morning, its oxidationproducts in aerosols showed peaks in daytime, due to a time lag between theemission and atmospheric reactions of α-pinene to form SOA. Positivematrix factorization (PMF) analysis indicated that anthropogenic influence isthe most important factor contributing to the elevated concentrations ofmolecular oxidation products of isoprene- (> 64 %) andα-pinene-derived SOA (> 57 %). The combination of the measuredfluxes and vertical profiles of biogenic volatile organic compounds (BVOCs)suggests that the inflow of anthropogenic precursors/aerosols likely enhancedthe formation of both isoprene SOA and α-pinene SOA within the forestcanopy even when the BVOC flux was relatively low. This study highlights theimportance of intra-canopy processes that promote biogenic SOA formation inthe presence of significant inflow of oxidants together with anthropogenicaerosols and their precursors.
机译：我们于2012年夏季同时测量了异戊二烯和α-concentrations烯的浓度和冠层以上通量，以及它们在氧化层中的氧化产物。日本的异戊二烯垂直剖面显示出林底附近的最大浓度，正午时有一个峰值，异戊二烯的氧化产物，即甲基丙烯醛（MACR）和甲基乙烯基酮（MVK），在森林冠层附近表现出较高的浓度。垂直剖面表明，可能是由于（蕨类植物）以及冠层内部的后续反应，导致林底附近大量异戊二烯排放。在森林底层附近，α-pine烯的浓度也显示最高值，在清晨和傍晚时最大。 α-pine烯的垂直剖面表明，除森林部位的叶片排放外，α-pine烯的排放量很大。气溶胶中的异戊二烯及其氧化产物在森林冠层内表现出相似的昼夜变化，提供了通过氧化最有可能从林地散发出的异戊二烯形成二次有机气溶胶（SOA）的证据。尽管在早晨观察到了高含量的α-pine烯，但由于排放和α-to烯形成SOA的大气反应之间存在时间差，因此其气溶胶中的氧化产物在白天显示出峰值。正矩阵分解（PMF）分析表明，人为影响是导致异戊二烯-（> 64％）和α-pine烯-SOA（> 57％）分子氧化产物浓度升高的最重要因素。测得的通量和生物挥发性有机化合物（BVOC）的垂直剖面的组合表明，即使BVOC通量相对较低，人为前体/气溶胶的流入也可能会促进森林冠层中异戊二烯SOA和α-pine烯SOA的形成。这项研究突出了冠层内部工艺的重要性，这种工艺在大量氧化剂与人为气溶胶及其前体一起流入的情况下，促进了生物源SOA的形成。

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