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二极管激光腔衰荡光谱测量大气NO3自由基

胡仁志 王丹 谢品华 凌六一 秦敏 李传新 刘建国

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二极管激光腔衰荡光谱测量大气NO3自由基

胡仁志, 王丹, 谢品华, 凌六一, 秦敏, 李传新, 刘建国

Diode laser cavity ring-down spectroscopy for atmospheric NO3 radical measurement

Hu Ren-Zhi, Wang Dan, Xie Pin-Hua, Ling Liu-Yi, Qin Min, Li Chuan-Xin, Liu Jian-Guo
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  • 本文介绍了基于外部调制二极管激光器(波长661.85 nm,线宽为0.3 nm)为光源的腔衰荡光谱技术探测环境大气中NO3自由基. 通过改变外部调制信号,优化二极管激光器的输出光谱,获得NO3自由基的有效吸收截面;探讨了大气中的其他气体成分(O3,NO2和水蒸气)对NO3自由基的测量干扰;考虑PFA管的壁碰撞损耗和过滤膜的损耗,初步量化本系统的NO3自由基进气效率约为70%. 当时间分辨率为7 s时,在实验室环境下,系统的探测限为2.0 pptv. 将本系统初步应用于夜间大气中NO3自由基的测量(2 h),获得了NO3自由基的浓度主要在17.951.7 pptv之间,平均浓度为36.3 pptv,实际的探测限为3.5 pptv;由于NO3自由基进气效率的不确定性等因素,系统的测量误差约为 8%(1). 实验结果表明,二极管激光腔衰荡光谱技术可实现大气中NO3自由基的高灵敏度在线探测.
    This article presents an external modulation diode laser (with wavelength 661.85 nm and line width 0.3 nm) cavity ring-down spectrometer for measurement of NO3 radical in the atmosphere. The output spectrum of the diode laser is optimized by changing the external modulation signal; the effective cross-section of the instrument is a convolution of the measured cross-section and the laser spectrum. Interference of other gases (O3, NO2, and water vapor)in NO3 radical detection has also been investigated. Considering the loss from the PFA tube wall collision and the membrane filtration, NO3 radical inlet transmission efficiencies of the system is about 70% through the preliminary quantitative analysis. When the time resolution is 7 s, the laboratory detection limit of the system is 2.0 pptv. This instrument was deployed in the night atmosphere to measure the NO3 radical. NO3 concentration varied from 17.9 to 51.7 pptv with an average level of 36.3 pptv. A typical detection sensitivity in the night atmosphere is 3.5 pptv. Because of the uncertainty in the inlet transmission efficiencies and other factors, the total uncertainty of the measured NO3 radicals is about 8%(1 ). Experimental results show that the diode laser cavity ring-down spectroscopy can achieve high sensitivity in insitu detection of NO3 radicals in the atmosphere.
    • 基金项目: 中国科学院战略性先导科技专项(B类)(批准号:XDB05040200)和国家自然科学基金(批准号:61108031,41275038,41305139)资助的课题.
    • Funds: Project supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB05040200), and the National Natural Science Foundation of China (Grant Nos. 61108031, 41275038, 41305139).
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    Qin M, Xie P H, Liu W Q, Li A, Dou K, Fang W, Liu H G, Zhang W J 2006 J Environ Sci-China 18 69

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    Wang Z R, Zhou B, Wang S S, Yang S N 2011 Acta Phys. Sin. 60 060703 (in Chinese) [王焯如, 周斌, 王珊珊, 杨素娜 2011 物理学报 60 060703]

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    Asaf D, Pedersen D, Matveev V, Peleg M, Kern C, Zingler J, Platt U, Luria M 2009 Environ. Sci. Technol. 43 9117

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    McLaren R, Wojtal P, Majonis D, McCourt J, Halla J D, Brook J 2010 Atmos. Chem. Phys. 10 4187

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    Li S W, Liu W Q, Xie P H, Qin M, YangY J 2012 Terr. Atmos. Ocean. Sci. 23 39

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    Wang S S, Shi C Z, Zhou B, Zhao H, Wang Z R, Yang S N, Chen L M 2013 Atmos. Environ. 70 401

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    Li S W, Liu W Q, Wang J T, Xie P H, Wang X D 2013 Spectrosc. Spect. Anal. 33 444 (in Chinese) [李素文, 刘文清, 王江涛, 谢品华, 汪徐德 2013 光谱学与光谱分析 33 444]

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    Geyer A, Ackermann R, Dubois R, Lohrmann B, Mller R, Platt U 2001 Atmos. Environ. 35 3619

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    Brown S S, Stark H, Ciciora S J, McLaughlin R J, Ravishankara A R 2002 Rev. Sci. Instrum. 73 3291

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    Dube W P, Brown S S, Osthoff H D, Nunley M R, Ciciora S J, Paris M W, McLaughlin R J, Ravishankara A R 2006 Rev. Sci. Instrum. 77 034101

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    Rothman L S, Gordon I E, Barber R J, Dothe H, Gamache R R, Goldman A, Perevalov V I, Tashkun S A, Tennyson J 2010 J. Quant. Spectrosc. Ra. 111 2139

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    Atkinson R, Baulch D L, Cox R A, Crowley J N, Hampson R F, Hynes R G, Jenkin M E, Rossi M J, Troe J 2004 Atmos. Chem. Phys. 4 1461

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    Wang D, Hu R Z, Xie P H, Qin M, Ling L Y, Duan J 2014 Spectrosc. Spect. Anal. (in Chinese, Accepted) [王丹, 胡仁志, 谢品华, 秦敏, 凌六一, 段俊 2014 光谱学与光谱分析]

    [32]

    Ling L Y, Qin M, Xie P H, Hu R Z, Fang W, Jiang Y, Liu J G, Liu W Q 2012 Acta Phys. Sin. 61 140703 (in Chinese)[凌六一, 秦敏, 谢品华, 胡仁志, 方武, 江宇, 刘建国, 刘文清 2012 物理学报 61 140703]

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  • [1]

    Vrekoussis M, Kanakidou M, Mihalopoulos N, Crutzen P J, Lelieveld J, Perner D, Berresheim H, Baboukas E 2004 Atmos. Chem. Phys. 4 169

    [2]

    Brown S S, Stutzb J 2012 Chem. Soc. Rev. 41 6405

    [3]

    Geyer, A, Alicke, B, Konrad S, Schmitz T, Stutz J, Platt U 2001 J. Geophys. Res. 106 8013

    [4]

    Platt U, Alicke B, Dubois R, Geyer A, Hofzumahaus A, Holland F, Martinez M, Mihelcic D, Klupfel T, Lohrmann B, Patz W, Perner D, Rohrer F, Schafer J, Stutz J 2002 J. Atmos. Chem. 42 359

    [5]

    Longfellow C A, Ravishankara A R, Hanson D R 2000 J. Geophys. Res. 105 24

    [6]

    Hao N, Zhou B, Chen L M 2006 Acta Phys. Sin. 55 1529 (in Chinese) [郝楠, 周斌, 陈立民 2006 物理学报 55 1529]

    [7]

    Qin M, Xie P H, Liu W Q, Li A, Dou K, Fang W, Liu H G, Zhang W J 2006 J Environ Sci-China 18 69

    [8]

    Wang Z R, Zhou B, Wang S S, Yang S N 2011 Acta Phys. Sin. 60 060703 (in Chinese) [王焯如, 周斌, 王珊珊, 杨素娜 2011 物理学报 60 060703]

    [9]

    Heintz F, Platt U, Flentje H, Dubois R 1996 J. Geophys. Res. 101 22891

    [10]

    Asaf D, Pedersen D, Matveev V, Peleg M, Kern C, Zingler J, Platt U, Luria M 2009 Environ. Sci. Technol. 43 9117

    [11]

    McLaren R, Wojtal P, Majonis D, McCourt J, Halla J D, Brook J 2010 Atmos. Chem. Phys. 10 4187

    [12]

    Li S W, Liu W Q, Xie P H, Qin M, YangY J 2012 Terr. Atmos. Ocean. Sci. 23 39

    [13]

    Wang S S, Shi C Z, Zhou B, Zhao H, Wang Z R, Yang S N, Chen L M 2013 Atmos. Environ. 70 401

    [14]

    Li S W, Liu W Q, Wang J T, Xie P H, Wang X D 2013 Spectrosc. Spect. Anal. 33 444 (in Chinese) [李素文, 刘文清, 王江涛, 谢品华, 汪徐德 2013 光谱学与光谱分析 33 444]

    [15]

    Li A, Xie P H, Liu C, Liu J G, Liu W Q 2007 Chin. Phys. Lett. 24 2859

    [16]

    Wang Y, Li A, Xie P H, Zeng Y, Wang R B, Chen H, Pei X, Liu J G, Liu W Q 2012 Chin. Phys. B 21 114211

    [17]

    Solomon S, Miller H L, Smith J P, Sanders R W, Mount G H, Schmeltekopf A L, Noxon J F 1989 J. Geophys. Res. 94 11041

    [18]

    Aliwell S R, Jones R L 1996 Geophys. Res. Lett. 23 2585

    [19]

    Shi P, Xie P H, Li A, Jiang Y, Wu F C, Qin M 2010 Acta Optica Sinica 30 3643 (in Chinese) [石鹏, 谢品华, 李昂, 江宇, 吴丰成, 秦敏 2010 光学学报 30 3643]

    [20]

    Geyer A, Ackermann R, Dubois R, Lohrmann B, Mller R, Platt U 2001 Atmos. Environ. 35 3619

    [21]

    Michelcic D, Klemp Musgen D, Patz H W, Volz-Thomas A 1993 J. Atmos. Chem. 16 313

    [22]

    Geyer A, Alicke B, Mihelcic D, Stutz J, Platt U 1999 J. Geophys. Res. 104 26097

    [23]

    Wood E C, Wooldridge P J, Freese J H, Albrecht T, Cohen R C 2003 Environ. Sci. Technol. 37 5732

    [24]

    Wood E C, Bertram T H, Wooldridge P J, Cohen R C 2005 Environ. Sci. Technol. 5 483

    [25]

    Ventrillard-Courtillot I, O’Brien E S, Kassi S, Méjean G, Romanini D 2010 Applied Physics B 101 661

    [26]

    Brown S S, Stark H, Ciciora S J, McLaughlin R J, Ravishankara A R 2002 Rev. Sci. Instrum. 73 3291

    [27]

    Dube W P, Brown S S, Osthoff H D, Nunley M R, Ciciora S J, Paris M W, McLaughlin R J, Ravishankara A R 2006 Rev. Sci. Instrum. 77 034101

    [28]

    Orphal J, Fellows C E, Flaud P M 2003 J. Geophys. Res. 108 4077

    [29]

    Rothman L S, Gordon I E, Barber R J, Dothe H, Gamache R R, Goldman A, Perevalov V I, Tashkun S A, Tennyson J 2010 J. Quant. Spectrosc. Ra. 111 2139

    [30]

    Atkinson R, Baulch D L, Cox R A, Crowley J N, Hampson R F, Hynes R G, Jenkin M E, Rossi M J, Troe J 2004 Atmos. Chem. Phys. 4 1461

    [31]

    Wang D, Hu R Z, Xie P H, Qin M, Ling L Y, Duan J 2014 Spectrosc. Spect. Anal. (in Chinese, Accepted) [王丹, 胡仁志, 谢品华, 秦敏, 凌六一, 段俊 2014 光谱学与光谱分析]

    [32]

    Ling L Y, Qin M, Xie P H, Hu R Z, Fang W, Jiang Y, Liu J G, Liu W Q 2012 Acta Phys. Sin. 61 140703 (in Chinese)[凌六一, 秦敏, 谢品华, 胡仁志, 方武, 江宇, 刘建国, 刘文清 2012 物理学报 61 140703]

    [33]

    Voigt S, Orphal J, Bogumil K, Burrows J P 2001 J. Photoch. Photobiol. A 43 1

    [34]

    Voigt S, Orphal J, Burrows J P 2002 J. Photoch. Photobio. A 49 1

    [35]

    Brown S S, Stark H, Ravishankara A R 2002 Appl. Phys. B 75 173

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出版历程
  • 收稿日期:  2014-01-06
  • 修回日期:  2014-02-20
  • 刊出日期:  2014-06-05

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