Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range.
Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range.
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DOI：
10.1073/pnas.1807604115
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发表时间：
2018-09-11
影响因子：
11.1
通讯作者：
Winkler PM
中科院分区：
文献类型：
--
作者：
Stolzenburg D;Fischer L;Vogel AL;Heinritzi M;Schervish M;Simon M;Wagner AC;Dada L;Ahonen LR;Amorim A;Baccarini A;Bauer PS;Baumgartner B;Bergen A;Bianchi F;Breitenlechner M;Brilke S;Buenrostro Mazon S;Chen D;Dias A;Draper DC;Duplissy J;El Haddad I;Finkenzeller H;Frege C;Fuchs C;Garmash O;Gordon H;He X;Helm J;Hofbauer V;Hoyle CR;Kim C;Kirkby J;Kontkanen J;Kürten A;Lampilahti J;Lawler M;Lehtipalo K;Leiminger M;Mai H;Mathot S;Mentler B;Molteni U;Nie W;Nieminen T;Nowak JB;Ojdanic A;Onnela A;Passananti M;Petäjä T;Quéléver LLJ;Rissanen MP;Sarnela N;Schallhart S;Tauber C;Tomé A;Wagner R;Wang M;Weitz L;Wimmer D;Xiao M;Yan C;Ye P;Zha Q;Baltensperger U;Curtius J;Dommen J;Flagan RC;Kulmala M;Smith JN;Worsnop DR;Hansel A;Donahue NM;Winkler PM
气溶胶颗粒可以通过气体到颗粒的转化而形成和生长，最终成为云滴的种子，影响全球气候。植物排放的挥发性有机化合物在大气中被氧化，所得产物推动颗粒生长。我们通过控制良好的实验室设置在较宽的对流层温度范围内测量氧化生物蒸气的颗粒生长。虽然较高的温度会导致反应速率增加和高度氧化的分子浓度增加，但较低的温度允许额外但氧化程度较低的物质凝结。我们测量了整个研究温度范围内的快速增长，表明有机物在整个对流层气溶胶的增长中发挥着重要作用。我们的发现将有助于提高全球气溶胶模型的预测。大气蒸气中气溶胶颗粒的成核和生长构成了全球云凝结核（CCN）的主要来源。达到 CCN 尺寸的新形成颗粒的比例对颗粒生长速率高度敏感，特别是对于 10 nm 的颗粒尺寸，其中较大气溶胶颗粒的凝结损失最大。最近的结果表明，生物挥发性有机化合物的一些氧化产物是颗粒形成和初始生长的主要贡献者。然而，氧化有机物是否有助于对流层温度范围内的颗粒生长仍然是一个悬而未决的问题，有机物生长的定量质量平衡尚未在任何温度下得到证实。在这里，在欧洲核研究组织 (CERN) 的宇宙室外液滴 (CLOUD) 室内进行的大气条件下进行的实验表明，有机颗粒在 C 到 C 的范围内快速生长。温度降低时，自氧化程度较低，但所有氧化分子的挥发性降低得到了补偿。这通过颗粒相成分测量得到证实，显示在低温下相对较少含氧产品的吸收增强。我们可以使用完全基于从两个互补质谱仪获得的氧化有机分子的实验测量气相光谱的气溶胶生长模型来重现测量的生长速率。我们表明，生长速率对颗粒曲率敏感，这解释了广泛的大气观测结果，即颗粒生长速率在个位数纳米尺寸范围内增加。我们的结果表明，有机蒸气可以促进颗粒在对流层温度范围内从分子簇尺寸开始的生长。
Aerosol particles can form and grow by gas-to-particle conversion and eventually act as seeds for cloud droplets, influencing global climate. Volatile organic compounds emitted from plants are oxidized in the atmosphere, and the resulting products drive particle growth. We measure particle growth by oxidized biogenic vapors with a well-controlled laboratory setup over a wide range of tropospheric temperatures. While higher temperatures lead to increased reaction rates and concentrations of highly oxidized molecules, lower temperatures allow additional, but less oxidized, species to condense. We measure rapid growth over the full temperature range of our study, indicating that organics play an important role in aerosol growth throughout the troposphere. Our finding will help to sharpen the predictions of global aerosol models. Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes 10 nm, where coagulation losses to larger aerosol particles are greatest. Recent results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from C to C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We show that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.
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影响因子：
5.2
作者：
Donahue, N. M.;Trump, E. R.;Riipinen, I.
通讯作者：
Riipinen, I.
影响因子：
56.9
作者：
Bianchi, F.;Trostl, J.;Baltensperger, U.
通讯作者：
Baltensperger, U.
影响因子：
4.4
作者：
Kulmala, M;Kerminen, VM;O'Dowd, CD
通讯作者：
O'Dowd, CD
影响因子：
4.4
作者：
Murphy, B. N.;Julin, J.;Ekman, A. M. L.
通讯作者：
Ekman, A. M. L.
影响因子：
6.3
作者：
Pierce, J. R.;Adams, P. J.
通讯作者：
Adams, P. J.