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首页> 外文期刊>Atmospheric chemistry and physics >Diurnal cycle and multi-decadal trend of formaldehyde in the remote atmosphere near 46A degrees aEuro N
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Diurnal cycle and multi-decadal trend of formaldehyde in the remote atmosphere near 46A degrees aEuro N

机译：欧亚N 46A度附近偏远大气中甲醛的昼夜循环和数十年趋势

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摘要

Only very few long-term records of formaldehyde (HCHO) exist that are suitable for trend analysis. Furthermore, many uncertainties remain as to its diurnal cycle, representing a large short-term variability superimposed on seasonal and inter-annual variations that should be accounted for when comparing ground-based observations to, e.g., model results. In this study, we derive a multi-decadal time series (January 1988-June 2015) of HCHO total columns from ground-based high-resolution Fourier transform infrared (FTIR) solar spectra recorded at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5A degrees aEuro-N, 8.0A degrees aEuro-E, 3580aEuro-maEuro-a. s. l. ), allowing for the characterization of the mid-latitudinal atmosphere for background conditions. First we investigate the HCHO diurnal variation, peaking around noontime and mainly driven by the intra-day insolation modulation and methane (CH4) oxidation. We also characterize quantitatively the diurnal cycles by adjusting a parametric model to the observations, which links the daytime to the HCHO columns according to the monthly intra-day regimes. It is then employed to scale all the individual FTIR measurements on a given daytime in order to remove the effect of the intra-day modulation for improving the trend determination and the comparison with HCHO columns simulated by the state-of-the-art GEOS-Chem v9-02 chemical transport model. Such a parametric model will be useful to scale the Jungfraujoch HCHO columns on satellite overpass times in the framework of future calibration/validation efforts of space-borne sensors. GEOS-Chem sensitivity tests suggest then that the seasonal and inter-annual HCHO column variations above Jungfraujoch are predominantly led by the atmospheric CH4 oxidation, with a maximum contribution of 25aEuro-% from the anthropogenic non-methane volatile organic compound precursors during wintertime. Finally, trend analysis of the so-scaled 27-year FTIR time series reveals a long-term evolution of the HCHO columns in the remote troposphere to be related to the atmospheric CH4 fluctuations and the short-term OH variability: +2.9aEuro-%aEuro-year(-1) between 1988 and 1995, -3.7aEuro-%aEuro-year(-1) over 1996-2002 and +0.8aEuro-%aEuro-year(-1) from 2003 onwards.
机译：仅存在很少的适合趋势分析的长期甲醛记录（HCHO）。此外，其昼夜周期还存在许多不确定性，这代表着将季节性和年际变化叠加在一起的较大的短期变化，在将地面观测结果与例如模型结果进行比较时应考虑这些变化。在这项研究中，我们从在少女峰（瑞士阿尔卑斯山）高空站记录的地面高分辨率傅里叶变换红外（FTIR）太阳光谱中得出HCHO总列的数十年时间序列（1988年1月至2015年6月） ，例如aEuro-N的46.5A度，eEuro-E的8.0A度，3580aEuro-maEuro-asl），从而可以对背景条件下的中纬度大气进行表征。首先，我们研究了HCHO的昼夜变化，该变化在中午左右达到峰值，并且主要受日间日照调制和甲烷（CH4）氧化的驱动。我们还通过调整观测值的参数模型来定量地描述昼夜周期，该模型根据日内日间制度将白天链接到HCHO列。然后将其用于在给定的白天缩放所有单独的FTIR测量值，以消除日内调制的影响，以改善趋势确定性以及与由最新GEOS- Chem v9-02化学品运输模型。在未来星载传感器的校准/验证工作的框架内，这种参数化模型将有助于在卫星越过时间上缩放少女峰HCHO色谱柱。然后，GEOS-Chem敏感性测试表明，少女峰上方的HCHO色谱柱季节和年度间变化主要是由大气中的CH4氧化引起的，在冬季，人为的非甲烷挥发性有机化合物前体的贡献最大为25aEuro％。最后，如此缩放后的27年FTIR时间序列的趋势分析显示，遥远对流层中HCHO柱的长期演变与大气CH4波动和短期OH变异性有关：+ 2.9aEuro-％ 1988年至1995年之间的aEuro-year（-1），1996-2002年之间的-3.7aEuro-％aEuro-year（-1）和2003年以来的+ 0.8aEuro-％aEuro-year（-1）。

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