在日本陆别津和南极洲Syowa站对HFC-23进行首次地面FTIR观测

M. Takeda, H. Nakajima, I. Murata, T. Nagahama, I. Morino, G. Toon, R. Weiss, J. Mühle, P. Krummel, P. Fraser, Hsiang J. Wang
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引用次数: 1

摘要

摘要我们开发了一种利用地基傅里叶变换红外光谱仪(FTIR)反演大气中HFC-23 (CHF3)丰度的方法,并分析了在日本陆别(43.5°N, 143.8°E)和南极洲Syowa站(69.0°S, 39.6°E)观测到的光谱。利用SFIT4检索程序进行FTIR检索,利用HFC-23 ν2和ν5振动-旋转过渡带重叠的1138.5 ~ 1148.0 cm−1和1154.0 ~ 1160.0 cm−1两个光谱窗口,避免了HFC-23的强H2O吸收特征。我们将O3、N2O、CH4、H2O、HDO、CFC-12 (CCl2F2)、HCFC-22 (CHClF2)、PAN (CH3C(O)OONO2)、HCFC-141b (CH3CCl2F)和HCFC-142b (CH3CClF2)作为干扰物。H2O、HDO和CH4的垂直剖面在HFC-23的反演中可能存在较大的不确定性,因此初步采用其他独立的光谱窗反演。每次HFC-23反演只有一条对对流层和平流层下层HFC-23敏感的垂直信息。反演误差主要是由于HFC-23、H2O、HDO和CH4丰度的光谱参数存在系统不确定性。为了比较ftir反演的HFC-23总柱数与AGAGE (Advanced Global Atmospheric Gases Experiment)提供的地表干空气摩尔分数,我们计算了ftir反演的HFC-23干空气柱平均摩尔分数(XHFC-23)。与AGAGE数据集相比,Rikubetsu和Syowa站点的ftir检索的XHFC-23具有负偏差。利用ftir检索的陆别县12月至2月的XHFC-23数据(DJF)数据得出的趋势为0.817±0.087 ppt(万亿分之一)年−1,这与AGAGE 12-box模式同期全球平均数据集(0.820±0.011 ppt年−1)的趋势很好地吻合。2007-2019年期间特立尼达海头(41.1°N, 124.2°W) AGAGE原位测量的趋势值(0.984±0.002 ppt)小于2007-2019年期间在特立尼达海头(41.1°N, 124.2°W)测量的趋势值(0.894±0.099 ppt)。Syowa站XHFC-23数据集2007-2016年的变化趋势为0.823±0.075 ppt(年−1),与Cape Grim(40.7°S, 144.7°E) AGAGE同期原位测量结果(0.874±0.002 ppt(年−1)一致。尽管两个站点的FTIR反演的XHFC-23存在系统偏差,但这些结果表明地面FTIR观测具有监测大气HFC-23趋势的能力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
First ground-based FTIR observations of HFC-23 at Rikubetsu, Japan, and Syowa Station, Antarctica
Abstract. We have developed a procedure for retrieving atmospheric abundances of HFC-23 (CHF3) with a ground-based Fourier transform infrared spectrometer (FTIR) and analysed the spectra observed at Rikubetsu, Japan (43.5° N, 143.8° E), and at Syowa Station, Antarctica (69.0° S, 39.6° E). The FTIR retrievals were carried out with the SFIT4 retrieval program, and the two spectral windows of 1138.5–1148.0 cm−1 and 1154.0–1160.0 cm−1 in the overlapping ν2 and ν5 vibrational-rotational transition bands of HFC-23 were used to avoid strong H2O absorption features. We considered O3, N2O, CH4, H2O, HDO, CFC-12 (CCl2F2), HCFC-22 (CHClF2), PAN (CH3C(O)OONO2), HCFC-141b (CH3CCl2F), and HCFC-142b (CH3CClF2) as interfering species. Vertical profiles of H2O, HDO, and CH4 are preliminarily retrieved with other independent spectral windows because these profiles may induce large uncertainties in the HFC-23 retrieval. Each HFC-23 retrieval has only one piece of vertical information with sensitivity to HFC-23 in the troposphere and the lower stratosphere. The retrieval errors mainly arise from the systematic uncertainties of the spectroscopic parameters used to obtain the HFC-23, H2O, HDO, and CH4 abundances. For comparison between FTIR-retrieved HFC-23 total columns and surface dry-air mole fractions provided by AGAGE (Advanced Global Atmospheric Gases Experiment), the FTIR-retrieved HFC-23 dry-air column-averaged mole fractions (XHFC-23) were calculated. The FTIR-retrieved XHFC-23 at Rikubetsu and Syowa Station have negative biases compared to AGAGE datasets. The trend derived from the FTIR-retrieved XHFC-23 data at Rikubetsu for December to February (DJF) data over the 1997–2010 period is 0.817 ± 0.087 ppt (parts per trillion) year−1, which is in good agreement with the trend derived from the annual global mean datasets of the AGAGE 12-box model for the same period (0.820 ± 0.011 ppt year−1). The trend of the FTIR-retrieved XHFC-23 data at Rikubetsu for DJF data over the 2007–2020 period is 0.894 ± 0.099 ppt year−1, which is smaller than the trend in the AGAGE in-situ measurements at Trinidad Head (41.1° N, 124.2° W) for the 2007–2019 period (0.984 ± 0.002 ppt year−1). The trend computed from the XHFC-23 datasets at Syowa Station over the 2007–2016 period is 0.823 ± 0.075 ppt year−1, which is consistent with that derived from the AGAGE in-situ measurements at Cape Grim (40.7° S, 144.7° E) for the same period (0.874 ± 0.002 ppt year−1). Although there are systematic biases on the FTIR-retrieved XHFC-23 at both sites, these results indicate that ground-based FTIR observations have the capability to monitor the trend of atmospheric HFC-23.
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