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Fourier transform infrared time series of tropospheric HCN in eastern China: seasonality, interannual variability, and source attribution

机译:傅里叶变换红外时间序列在中国东部的对流层HCN:季节性,年际变异性和源归因

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We analyzed seasonality and interannual variability of tropospheric hydrogen cyanide (HCN) columns in densely populated eastern China for the first time. The results were derived from solar absorption spectra recorded with a ground-based high-spectral-resolution Fourier transform infrared (FTIR) spectrometer in Hefei (31°54′N, 117°10′E) between 2015 and 2018. The tropospheric HCN columns over Hefei, China, showed significant seasonal variations with three monthly mean peaks throughout the year. The magnitude of the tropospheric HCN column peaked in May, September, and December. The tropospheric HCN column reached a maximum monthly mean of (9.8±0.78)×1015moleculescm?2 in May and a minimum monthly mean of (7.16±0.75)×1015moleculescm?2 in November. In most cases, the tropospheric HCN columns in Hefei (32°N) are higher than the FTIR observations in Ny-?lesund (79°N), Kiruna (68°N), Bremen (53°N), Jungfraujoch (47°N), Toronto (44°N), Rikubetsu (43°N), Izana (28°N), Mauna Loa (20°N), La Reunion Maido (21°S), Lauder (45°S), and Arrival Heights (78°S) that are affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Enhancements of tropospheric HCN column were observed between September?2015 and July?2016 compared to the same period of measurements in other years. The magnitude of the enhancement ranges from 5% to 46% with an average of 22%. Enhancement of tropospheric HCN (ΔHCN) is correlated with the concurrent enhancement of tropospheric CO (ΔCO), indicating that enhancements of tropospheric CO and HCN were due to the same sources. The GEOS-Chem tagged CO simulation, the global fire maps, and the potential source contribution function (PSCF) values calculated using back trajectories revealed that the seasonal maxima in May are largely due to the influence of biomass burning in Southeast Asia (SEAS) (41±13.1%), Europe and boreal Asia (EUBA) (21±9.3%), and Africa (AF) (22±4.7%). The seasonal maxima in September are largely due to the influence of biomass burnings in EUBA (38±11.3%), AF (26±6.7%), SEAS (14±3.3%), and North America (NA) (13.8±8.4%). For the seasonal maxima in December, dominant contributions are from AF (36±7.1%), EUBA (21±5.2%), and NA (18.7±5.2%). The tropospheric HCN enhancement between September?2015 and July 2016 at Hefei (32°N) was attributed to an elevated influence of biomass burnings in SEAS, EUBA, and Oceania (OCE) in this period. In particular, an elevated number of fires in OCE in the second half of 2015 dominated the tropospheric HCN enhancement between September and December?2015. An elevated number of fires in SEAS in the first half of 2016 dominated the tropospheric HCN enhancement between January and July?2016.
机译:我们第一次分析了对流层富含氰化氢(HCN)柱的季节性和际变化。结果源自记录的太阳能吸收光谱,其在2015年至2018之间的合肥(31°54'n,117°10'e)中的地基高光谱分辨率傅里叶变换红外(FTIR)光谱仪。对流层HCN柱在中国合肥,全年三月平均峰值显示出显着的季节性变化。 Troposheric HCN专栏的大小在5月,9月和12月达到了峰值。 Troposheric HCN专栏的最大每月平均值(9.8±0.78)×1015moleculescm?2月2日和最低月平均值(7.16±0.75)×1015moleculescm?2月2日。在大多数情况下,合肥(32°N)中的对流层HCN柱高于NY-?Lesund(79°N),Kiruna(68°N),不来梅(53°N),Jungfraujoch(47°)中的FTIR观察n),多伦多(44°N),Rikubetsu(43°N),Izana(28°N),Mauna Loa(20°N),La Reunion Maido(21°S),Lauder(45°S)和到达隶属于网络的高度(78°S),用于检测大气组成变化(NDACC)。在9月份之间观察到了对流层HCN柱的增强2015年和7月 - 2016年相比,与其他几年同期的测量期相比。增强幅度为5%至46%,平均为22%。对流层HCN(ΔHCN)的增强与对流层CO(ΔCo)的并发增强相关,表明对流层CO和HCN的增强是由于相同的来源。使用后轨迹计算的Geos-Chem标记的CO模拟,全球火地图和潜在的源贡献功能(PSCF)值表明,季节性最大值可能在很大程度上是由于生物量在东南亚(SEA)的影响力( 41±13.1%),欧洲和北方亚洲(EUBA)(21±9.3%)和非洲(AF)(22±4.7%)。 9月份的季节性最大值主要是由于Euba中生物质燃烧的影响(38±11.3%),AF(26±6.7%),海洋(14±3.3%)和北美(NA)(13.8±8.4%) )。对于12月的季节性最大值,主导贡献来自AF(36±7.1%),EUBA(21±5.2%)和NA(18.7±5.2%)。 2015年9月(2016年7月,Hefei(32°N)之间的对流层HCN增强归因于此期间海洋,埃巴和大洋洲(Oceia(OCE)对生物量燃烧的升高。特别是2015年下半年在2015年9月至12月之间的对流层HCN增强率升高的OCE升高的火灾数量。 2016年上半年海洋中海域的火灾数量升高为2016年1月至7月至7月之间的对流层HCN增强。
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