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介绍了基于近紫外发光二极管LED (中心波长约372 nm,半高宽13 nm) 光源的非相干宽带腔增强吸收光谱技术,同时用于探测痕量气体HONO和NO2. LED出射光经准直后耦合进入长度为70 cm,由两块高反射率镜片组成的高精密光学腔内. 分别测量了氮气消光谱和氦气消光谱,通过两者瑞利散射截面的差异而引起光谱强度的变化来标定镜片反射率.在360390 nm反演波段内,镜片反射率在390 nm处最大且为0.99962, 对应测量NO2/HONO混合物时的最大光程约1.71 km,并利用最小二乘拟合反演出了HONO和NO2的浓度值.当光谱采集时间为1000 s时, HONO和NO2的探测灵敏度(1) 分别为0.6 ppbv和1.9 ppbv.实验结果表明,该技术为实现大气痕量气体的高灵敏度在线监测提供了另一种可能的途径.
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关键词:
- 大气光学 /
- 非相干宽带腔增强吸收光谱技术 /
- 近紫外发光二极管 /
- HONO探测
An application of incoherent broadband cavity enhanced absorption spectroscopy with a near-ultraviolet LED (peak 372 nm and FWHM is 13 nm) to simultaneously detecting HONO and NO2 is described. The light emitted from the LED is collimated and then coupled into an 70 cm long high finesse cavity formed with two high reflectivity mirrors. The spectra are respectively recorded when the cell is filled with He and then N2, and the mirror reflectivity is determined from the change in transmitted intensity due to the difference in Rayleigh scattering cross-section between He and N2. The maximum of mirror reflectivity is 0.99962 at 390 nm in a spectral region of 360-390 nm, and corresponding maximum of light path length is about 1.71 km when NO2/HONO mixture is measured. The concentrations of HONO and NO2 are obtained using least-squares fit. Detection sensitivity (1) of 0.6 ppbv for HONO and 1.9 ppbv for NO2 are achieved using an acquisition time of 1000 s. The experimental results demonstrate the possible application of this technology to in situ monitoring the trace gases in the atmosphere.-
Keywords:
- atmospheric optics /
- incoherent broadband cavity enhanced absorption spectroscopy /
- near-ultraviolet LED /
- detection of HONO
[1] Ehhalt D H 1994 Sci. Total Environ. 143 1
[2] Alicke B, Platt U,Stutz J 2002 J. Geophys. Res-Atmos. 107 8196
[3] Rohrer F, Bohn B, Brauers T, Bruning D, Johnen F J, Wahner A, Kleffmann J 2005 Atmos. Chem. Phys. 5 2189
[4] Calvert J G, Yarwood G, Dunker A M 1994 Res. Chem. Intermed. 20 463
[5] Goodman A L, Underwood G M, Grassian V H 1999 J. Phys. Chem. A 103 7217
[6] Kleffmann J, Becker K H, Wiesen P 1998 Atmos. Environ. 32 2721
[7] Stutz J, Oh H J, Whitlow S I, Anderson C, Dibbb J E, Flynn J H, Rappenglueck B, Lefer B 2010 Atmos. Environ. 44 4090
[8] 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
[9] 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]
[10] Stutz J, Alicke B, Ackermann R, Geyer A, Wang S H, White A B, Williams E J, Spicer C W, Fast J D 2004 J. Geophys. Res-Atmos. 109 D03307
[11] Wang S H, Ackermann R, Spicer C W, Fast J D, Schmeling M, Stutz J 2003 Geophys. Res. Lett. 30 49
[12] Febo A, Perrino C, Allegrini I 1996 Atmos. Environ. 30 3599
[13] Platt U, Stutz J 2008 Differential Optical Absorption Spectroscopy: Principles and Applications (Berlin: Springer) p597
[14] 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]
[15] Romanini D, Kachanov A A, Sadeghi N, Stoeckel F 1997 Chem. Phys. Lett. 264 316
[16] Paul B, Scherer J J, Okeefe A, Saykally R J 1997 Laser Focus World 33 71
[17] Gianfrani L, Fox R W, Hollberg L 1999 J. Opt. Soc. Am. B 16 2247
[18] Provencal R, Gupta M, Owano T G, Baer D S, Ricci K N, O'Keefe A, Podolske J R 2005 Appl. Opt. 44 6712
[19] Wang L M, Zhang J S 2000 Environ. Sci. Technol. 34 4221
[20] Kasyutich V L, Martin P A, Holdsworth R J 2006 Meas. Sci. Technol. 17 923
[21] Fiedler S E, Hese A, Ruth A A 2003 Chem. Phys. Lett. 371 11
[22] Washenfelder R A, Langford A O, Fuchs H, Brown S S 2008 Atmos. Chem. Phys. 8 7779
[23] Vaughan S, Gherman T, Ruth A A, Orphal J 2008 Phys. Chem. Chem. Phys. 10 4471
[24] Gherman T, Venables D S, Vaughan S, Orphal J, Ruth A A 2008 Environ. Sci. Technol. 42 890
[25] Wu T, Zhao W, Chen W, Zhang W, Gao X 2009 Appl. Phys. B Lasers O 94 85
[26] Venables D S, Gherman T, Orphal J, Wenger J C, Ruth A A 2006 Environ. Sci. Technol. 40 6758
[27] Triki M, Cermak P, Mejean G, Romanini D 2008 Appl. Phys. B Lasers O 91 195
[28] Fiedler S E, Hese A, Ruth A A 2005 Rev. Sci. Instrum. 76 023107
[29] Ball S M, Langridge J M, Jones R L 2004 Chem. Phys. Lett. 398 68
[30] Langridge J M, Ball S M, Shillings A J L, Jones R L 2008 Rev. Sci. Instrum. 79 123110
[31] Langridge J M, Laurila T, Watt R S, Jones R L, Kaminski C F, Hult J 2008 Opt. Express 16 10178
[32] Langridge J M, Ball S M, Jones R L 2006 Analyst 131 916
[33] Thalman R, Volkamer R 2010 Atmos. Meas. Tech. 3 1797
[34] Shardanand S, Rao A D P 1977 NASA Technical Note (Wallops Island: Wallops Flight Center)
[35] Naus H, Ubachs W 2000 Opt. Lett. 25 347
[36] Platt U, Meinen J, Poehler D, Leisner T 2009 Atmos. Meas. Tech. 2 713
[37] Voigt S, Orphal J, Burrows J P 2002 J. Photoch. Photobio. A 149 1
[38] Stutz J, Kim E S, Platt U, Bruno P, Perrino C, Febo A 2000 J. Geophys. Res-Atmos. 105 14585
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[1] Ehhalt D H 1994 Sci. Total Environ. 143 1
[2] Alicke B, Platt U,Stutz J 2002 J. Geophys. Res-Atmos. 107 8196
[3] Rohrer F, Bohn B, Brauers T, Bruning D, Johnen F J, Wahner A, Kleffmann J 2005 Atmos. Chem. Phys. 5 2189
[4] Calvert J G, Yarwood G, Dunker A M 1994 Res. Chem. Intermed. 20 463
[5] Goodman A L, Underwood G M, Grassian V H 1999 J. Phys. Chem. A 103 7217
[6] Kleffmann J, Becker K H, Wiesen P 1998 Atmos. Environ. 32 2721
[7] Stutz J, Oh H J, Whitlow S I, Anderson C, Dibbb J E, Flynn J H, Rappenglueck B, Lefer B 2010 Atmos. Environ. 44 4090
[8] 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
[9] 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]
[10] Stutz J, Alicke B, Ackermann R, Geyer A, Wang S H, White A B, Williams E J, Spicer C W, Fast J D 2004 J. Geophys. Res-Atmos. 109 D03307
[11] Wang S H, Ackermann R, Spicer C W, Fast J D, Schmeling M, Stutz J 2003 Geophys. Res. Lett. 30 49
[12] Febo A, Perrino C, Allegrini I 1996 Atmos. Environ. 30 3599
[13] Platt U, Stutz J 2008 Differential Optical Absorption Spectroscopy: Principles and Applications (Berlin: Springer) p597
[14] 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]
[15] Romanini D, Kachanov A A, Sadeghi N, Stoeckel F 1997 Chem. Phys. Lett. 264 316
[16] Paul B, Scherer J J, Okeefe A, Saykally R J 1997 Laser Focus World 33 71
[17] Gianfrani L, Fox R W, Hollberg L 1999 J. Opt. Soc. Am. B 16 2247
[18] Provencal R, Gupta M, Owano T G, Baer D S, Ricci K N, O'Keefe A, Podolske J R 2005 Appl. Opt. 44 6712
[19] Wang L M, Zhang J S 2000 Environ. Sci. Technol. 34 4221
[20] Kasyutich V L, Martin P A, Holdsworth R J 2006 Meas. Sci. Technol. 17 923
[21] Fiedler S E, Hese A, Ruth A A 2003 Chem. Phys. Lett. 371 11
[22] Washenfelder R A, Langford A O, Fuchs H, Brown S S 2008 Atmos. Chem. Phys. 8 7779
[23] Vaughan S, Gherman T, Ruth A A, Orphal J 2008 Phys. Chem. Chem. Phys. 10 4471
[24] Gherman T, Venables D S, Vaughan S, Orphal J, Ruth A A 2008 Environ. Sci. Technol. 42 890
[25] Wu T, Zhao W, Chen W, Zhang W, Gao X 2009 Appl. Phys. B Lasers O 94 85
[26] Venables D S, Gherman T, Orphal J, Wenger J C, Ruth A A 2006 Environ. Sci. Technol. 40 6758
[27] Triki M, Cermak P, Mejean G, Romanini D 2008 Appl. Phys. B Lasers O 91 195
[28] Fiedler S E, Hese A, Ruth A A 2005 Rev. Sci. Instrum. 76 023107
[29] Ball S M, Langridge J M, Jones R L 2004 Chem. Phys. Lett. 398 68
[30] Langridge J M, Ball S M, Shillings A J L, Jones R L 2008 Rev. Sci. Instrum. 79 123110
[31] Langridge J M, Laurila T, Watt R S, Jones R L, Kaminski C F, Hult J 2008 Opt. Express 16 10178
[32] Langridge J M, Ball S M, Jones R L 2006 Analyst 131 916
[33] Thalman R, Volkamer R 2010 Atmos. Meas. Tech. 3 1797
[34] Shardanand S, Rao A D P 1977 NASA Technical Note (Wallops Island: Wallops Flight Center)
[35] Naus H, Ubachs W 2000 Opt. Lett. 25 347
[36] Platt U, Meinen J, Poehler D, Leisner T 2009 Atmos. Meas. Tech. 2 713
[37] Voigt S, Orphal J, Burrows J P 2002 J. Photoch. Photobio. A 149 1
[38] Stutz J, Kim E S, Platt U, Bruno P, Perrino C, Febo A 2000 J. Geophys. Res-Atmos. 105 14585
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