Department of Earth and Planetary Sciences, University of California, Berkeley, CA 94720;
College of Chemistry, University of California, Berkeley, CA 94720.
Proc Natl Acad Sci U S A. 2018 Sep 4;115(36):8931-8936. doi: 10.1073/pnas.1807532115. Epub 2018 Aug 20.
The hydroxyl radical (OH) is the primary oxidant in the troposphere, and the impact of its fluctuations on the methane budget has been disputed in recent years, however measurements of OH are insufficient to characterize global interannual fluctuations relevant for methane. Here, we use a 6,000-y control simulation of preindustrial conditions with a chemistry-climate model to quantify the natural variability in OH and internal feedbacks governing that variability. We find that, even in the absence of external forcing, maximum OH changes are 3.8 ± 0.8% over a decade, which is large in the context of the recent methane growth from 2007-2017. We show that the OH variability is not a white-noise process. A wavelet analysis indicates that OH variability exhibits significant feedbacks with the same periodicity as the El Niño-Southern Oscillation (ENSO). We find intrinsically generated modulation of the OH variability, suggesting that OH may show periods of rapid or no change in future decades that are solely due to the internal climate dynamics (as opposed to external forcings). An empirical orthogonal function analysis further indicates that ENSO is the dominant mode of OH variability, with the modulation of OH occurring primarily through lightning [Formula: see text] La Niña is associated with an increase in convection in the Tropical Pacific, which increases the simulated occurrence of lightning and allows for more OH production. Understanding this link between OH and ENSO may improve the predictability of the oxidative capacity of the troposphere and assist in elucidating the causes of current and historical trends in methane.
羟基自由基 (OH) 是平流层中的主要氧化剂,近年来,其波动对甲烷预算的影响一直存在争议,然而,OH 的测量不足以描述与甲烷相关的全球年际波动。在这里,我们使用化学-气候模型对工业化前条件进行了 6000 年的控制模拟,以量化 OH 的自然变异性和控制这种变异性的内部反馈。我们发现,即使在没有外部强迫的情况下,OH 的最大变化在十年内也达到了 3.8%±0.8%,这在 2007-2017 年甲烷增长的背景下是很大的。我们表明,OH 变异性不是一个白噪声过程。小波分析表明,OH 变异性与厄尔尼诺-南方涛动(ENSO)具有相同的周期性,存在显著的反馈。我们发现 OH 变异性存在内在的调制,这表明 OH 在未来几十年可能会出现快速变化或无变化的时期,这仅仅是由于内部气候动力(而不是外部强迫)。经验正交函数分析进一步表明,ENSO 是 OH 变异性的主要模式,OH 的调制主要通过闪电[公式:见正文]拉尼娜现象与热带太平洋中对流的增加有关,这增加了模拟闪电的发生,并允许更多的 OH 产生。了解 OH 和 ENSO 之间的这种联系可能会提高平流层氧化能力的可预测性,并有助于阐明甲烷当前和历史趋势的原因。