基于地基高分辨率太阳吸收光谱观测大气中硝酸的时空分布
(2.中国科学院合肥物质科学研究院安徽光学精密机械研究所环境光学与技术重点实验室, 安徽合肥 230031)
(3.中国科学技术大学地球和空间科学学院, 安徽合肥 230026)
(4.School of Chemistry,University of Wollongong,Wollongong, New South Wales 2522,Australia)
【摘要】利用高分辨率傅里叶变换红外光谱(FTIR)技术探测合肥地区大气硝酸(HNO3)的浓度,基于最优估算法由中红外太阳吸收光谱反演出HNO3的垂直廓线和柱总量。获得了2017年大气HNO3的垂直廓线和柱总量的时间序列,分析了HNO3的季节变化、浓度探测敏感性高度、反演平均核和自由度等特征。不同季节大气HNO3的垂直廓线表明,HNO3在20~30km的大气平流层浓度较高,在对流层浓度较低。HNO3的柱浓度显示出明显的季节变化,春季出现最大值,冬季出现最小值,季节变化幅值为9.82×1015 molecule/cm2。为了对地基FTIR的观测进行比对,选取Aura MLS卫星数据产品与地基测量数据进行比对。比对结果表明,地基遥感观测与卫星数据显示出的季节变化一致;尽管卫星偏柱量整体小于地基遥感的柱总量,但两者的相关系数为0.83,表明两者具有较好的一致性。地基观测结果验证了地基FTIR技术观测大气中HNO3时空分布的可靠性和准确性。
【关键词】 大气光学; 傅里叶变换红外光谱技术; 硝酸; 垂直廓线; 柱浓度;
【DOI】
【基金资助】
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References
[1] Batchelor R L,Strong K,Lindenmaier R,et al.A new Bruker IFS 125HR FTIR spectrometer for the Polar Environment Atmospheric Research Laboratory at Eureka, Nunavut,Canada:measurements and comparison with the existing Bomem DA8spectrometer[J]. Journal of Atmospheric and Oceanic Technology,2009,26(7):1328-1340.
[2] Brasseur G P,Solomon S.Aeronomy of the middle atmosphere:chemistry and physics of the stratosphere and mesosphere[M].Dordrecht:Springer,2005:327-358.
[3] Solomon S.Stratospheric ozone depletion:a review of concepts and history[J].Reviews of Geophysics,1999,37(3):275-316.
[4] Schaap M,van Loon M,ten Brink H M,et al.Secondary inorganic aerosol simulations for Europe with special attention to nitrate[J].Atmospheric Chemistry and Physics,2004,4(3):857-874.
[5] Kou X W,Zhou B,Liu X C,et al.Measurement of trace NH3concentration in atmosphere by cavity ringdown spectroscopy[J].Acta Optica Sinica,2018,38(11):1130001.
[6] Arden Pope III C,Ezzati M,Dockery D W.Fine particulate air pollution and life expectancies in the United States:the role of influential observations[J].Journal of the Air&Waste Management Association,2013,63(2):129-132.
[7] Murcray D G,Kyle T G,Murcray F H,et al.Nitric acid and nitric oxide in the lower stratosphere[J].Nature,1968,218(5136):78-79.
[8] Lado-Bordowsky O, Amat G. Laboratory and atmospheric measurements of HNO3to determine the amount of this constituent in the Earths atmosphere[J].Applied Optics,1979,18(20):3400-3403.
[9] Loewenstein M, Starr W L, Murcray D G.Stratospheric NO and HNO3 observations in the northern hemisphere for three seasons[J].Geophysical Research Letters,1978,5(6):531-534.
[10] Louisnard N,Fergant G,Girard A,et al.Infrared absorption spectroscopy applied to stratospheric profiles of minor constituents[J].Journal of Geophysical Research:Oceans,1983,88(C9):5365-5376.
[11] Rinsland C P,Goldman A,Murcray F J,et al.Infrared measurements of atmospheric gases above Mauna Loa,Hawaii,in February 1987[J].Journal of Geophysical Research,1988,93(D10):12607-12626.
[12] Russell III J M,Farmer C B,Rinsland C P,et al.Measurements of odd nitrogen compounds in the stratosphere by the ATMOS experiment on Spacelab3[J].Journal of Geophysical Research,1988,93(D2):1718-1736.
[13] Neuman J A,Gao R S,Fahey D W,et al.In situ measurements of HNO3,NOy,NO,and O3in the lower stratosphere and upper troposphere[J].Atmospheric Environment,2001,35(33):5789-5797.
[14] Wespes C, Emmons L, Edwards D P,et al.Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft,groundbased,satellite observations and MOZART-4model:source attribution and partitioning[J].Atmospheric Chemistry and Physics,2012,12(1):237-259.
[15] Johansson S,Woiwode W,Hpfner M,et al.Airborne limb-imaging measurements of temperature,HNO3,O3,ClONO2,H2O and CFC-12during the Arctic winter 2015/2016:characterization,in situ validation and comparison to Aura/MLS[J]. Atmospheric Measurement Techniques,2018,11(8):4737-4756.
[16] Wespes C,Hurtmans D,Clerbaux C,et al.Global distributions of nitric acid from IASI/MetOP measurements[J]. Atmospheric Chemistry and Physics,2009,9(20):7949-7962.
[17] Ronsmans G,Langerock B,Wespes C,et al.First characterization and validation of FORLI-HNO3vertical profiles retrieved from IASI/Metop[J].Atmospheric Measurement Techniques,2016,9(9):4783-4801.
[18] Griffin D,Walker K A,Conway S,et al.Multi-year comparisons of ground-based and space-borne Fourier transform spectrometers in the high Arctic between2006 and 2013[J]. Atmospheric Measurement Techniques,2017,10(9):3273-3294.
[19] Fiorucci I,Muscari G,Froidevaux L,et al.Groundbased stratospheric O3 and HNO3 measurements at thule,Greenland:an intercomparison with aura MLS observations[J]. Atmospheric Measurement Techniques,2013,6(9):2441-2453.
[20] Rinsland C P,Zander R,Demoulin P.Ground-based infrared measurements of HNO3 total column abundances:long-term trend and variability[J].Journal of Geophysical Research,1991,96(D5):9379-9389.
[21] Wood S W,Batchelor R L,Goldman A,et al.Ground-based nitric acid measurements at Arrival Heights,Antarctica,using solar and lunar Fourier transform infrared observations[J]. Journal of Geophysical Research,2004,109(D18):D18307.
[22] Vigouroux C,de Mazière M,Errera Q,et al.Comparisons between ground-based FTIR and MIPAS N2O and HNO3 profiles before and after assimilation in BASCOE[J].Atmospheric Chemistry and Physics,2007,7(2):377-396.
[23] Fu D, Walker K A, Mittermeier R L,et al.Simultaneous trace gas measurements using two Fourier transform spectrometers at Eureka,Canada during spring 2006,and comparisons with the ACEFTS[J].Atmospheric Chemistry and Physics,2011,11(11):5383-5405.
[24] Shan C G,Wang W,Liu C,et al.Detection of stable isotopic ratio of atmospheric CO2 based on Fourier transform infrared spectroscopy[J].Acta Physica Sinica,2017,66(22):220204.
[25] Wang W,Tian Y,Liu C,et al.Investigating the performance of a greenhouse gas observatory in Hefei,China[J]. Atmospheric Measurement Techniques,2017,10(7):2627-2643.
[26] Rodgers C D.Retrieval of atmospheric temperature and composition from remote measurements of thermal radiation[J].Reviews of Geophysics,1976,14(4):609-624.
[27] Rodgers C D.Inverse methods for atmospheric sounding-theory and practice[M]. Series on atmospheric, oceanic and planetary physics.Singapore:World Scientific Publishing Co. Pte.Ltd.,2000,2:103-121.
[28] Rothman L S,Gordon I E,Barbe A,et al.The HITRAN 2008molecular spectroscopic database[J].Journal of Quantitative Spectroscopy and Radiative Transfer,2009,110(9/10):533-572.
[29] Hase F,Blumenstock T,Paton-Walsh C.Analysis of the instrumental line shape of high-resolution Fourier transform IR spectrometers with gas cell measurements and new retrieval software[J].Applied Optics,1999,38(15):3417-3422.
[30] Hase F.Improved instrumental line shape monitoring for the ground-based, high-resolution FTIR spectrometers of the Network for the Detection of Atmospheric Composition Change[J].Atmospheric Measurement Techniques,2012,5(3):603-610.
[31] Keppel-Aleks G,Wennberg P O,Schneider T.Sources of variations in total column carbon dioxide[J].Atmospheric Chemistry and Physics,2011,11(8):3581-3593.
[32] Livesey N J,van Snyder W,Read W G,et al.Retrieval algorithms for the EOS Microwave Limb Sounder(MLS)[J].IEEE Transactions on Geoscience and Remote Sensing,2006,44(5):1144-1155.
[33] Livesey N J,Read W G,Wagner P A,et al.Version4.2×Level 2data quality and description document,Rev.B[J].Jet Propulsion Laboratory,2015.
[34] Rohrer F,Berresheim H.Strong correlation between levels of tropospheric hydroxyl radicals and solar ultraviolet radiation[J].Nature,2006,442(7099):184-187.
[35] Chen L, Wang S G, Wang L L. Variation characteristics and influencing factors of NOx and ozone in autumn in Fukang region of Xinjiang[J].Journal of Arid Meteorology,2012,30(3):345-352.
[36] Sun Y W,Wang L Y.Gaseous pollutants levels and sources of NOx,SO2in heating period of spring and non-heating period of summer in Siping city[J].Liaoning Chemical Industry,2014,43(1):19-21,24.
[37] Austin J,Garcia R R,Russell III J M,et al.On the atmospheric photochemistry of nitric acid[J].Journal of Geophysical Research,1986,91(D5):5477-5485.
ISSN:0253-2239
CN: 31-1252/O4
Vol 40, No. 02, Pages 23-33
January 2020
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