Broadband cavity enhanced absorption spectroscopy for measuring atmospheric NO<sub>3</sub> radical

Duan Jun; Tang Ke; Qin Min; Wang Dan; Wang Mu-Di; Fang Wu; Meng Fan-Hao; Xie Pin-Hua; Liu Jian-Guo; Liu Wen-Qing

doi:10.7498/aps.70.20201066

Abstract

NO₃ radical is the most important oxidant in atmospheric chemistry at night, and it controls the oxidation and removal of various trace gas components in the atmosphere. The understanding of the chemical process of NO₃ radical is of great significance for studying the atmospheric pollution processes such as haze. The NO₃ radical has a low concentration and strong activity, so it is relatively difficult to measure accurately. We report here in this paper an instrument for unambiguously measuring NO₃ based on broadband cavity enhanced absorption spectroscopy (BBCEAS). To achieve the robust performance and system stability under diverse conditions, this BBCEAS instrument has been developed, with efficient sampling, and resistance against vibration and temperature change improved, and the BBCEAS instrument also has low-power consumption. The 660-nm-wavelemngth light-emitting diode (LED) is used as a light source of the BBCEAS system. The sampling gas path with low loss and suitable for domestic high-particle environment is designed. Through the LED light source test, the optimal working current and temperature can be obtained to achieve the acquisition of NO₃ absorption spectrum with high signal-to-noise ratio. Considering the fact that the water vapor absorption is an important interference factor for the measurement of NO₃ radical by BBCEAS, the daytime atmospheric measurement spectrum is used as a background spectrum, and participates in spectral fitting of NO₃ to reduce the effect of water vapor. The mirror reflectivity and effective cavity length are calibrated, and the Allan variance analysis is also carried out. The reflectance of the mirror can reach about 0.99993 at 662 nm (NO₃ absorption peak), and the corresponding theoretical effective optical path can reach more than 7 km, which can meet the measurement requirements of atmospheric NO₃ radicals. The detection limit (1σ) of 0.75 pptv for NO₃ is achieved with an acquisition time of 10 s and a total measurement error of about 16%. The atmospheric NO₃ radical observation is carried out in Hefei. During the observation period, the highest NO₃ concentration is 23.4 pptv, demonstrating the promising potential applications in in-situ, sensitive, accurate and fast simultaneous measurements of NO₃ in the future by using the developed broadband cavity enhanced absorption spectroscopy.

Keywords:

NO₃ /
BBCEAS /
high sensitivity

Authors and contacts

1.
Key Laboratory of Environmental Optics and Technology of Chinese Academy of Sciences, Anhui Institute of Optics and Fine Mechanics, HFIPS, Chinese Academy of Sciences, Hefei 230031, China
2.
School of Mathematics and Physics, Anhui University of Technology, Maanshan 243002, China
3.
School of Basic Medical Sciences, Anhui Medical University, Hefei 230032, China
4.
School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei 230026, China
5.
Center for Excellence in Regional Atmospheric Environment, Chinese Academy of Sciences, Xiamen 361021, China

Corresponding author: Qin Min, mqin@aiofm.ac.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2017YFC0209400), the National Natural Science Foundation of China (Grant Nos. 41705015, 41905130),Youth Science and Technology Talents Support Program (2020) by Anhui Association for Science and Technology (Grant No. RCTJ202002) and the Foundation of Director of Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, China (Grant No. AGHH201601)

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References

[1]	Levy H 1971 Science 173 141 Google Scholar
[2]	Wayne R P, Barnes I, Biggs P, Burrows J P, Canosamas C E, Hjorth J, Lebras G, Moortgat G K, Perner D, Poulet G, Restelli G, Sidebottom H 1991 Atmos. Environ. Part A 25 1
[3]	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 Google Scholar
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[5]	Platt U, Perner D, Winer A M, Harris G W, Pitts J N 1980 Geophys. Res. Lett. 7 89 Google Scholar
[6]	Wood E C, Wooldridge P J, Freese J H, Albrecht T, Cohen R C 2003 Environ. Sci. Technol. 37 5732 Google Scholar
[7]	Slusher D L, Huey L G, Tanner D J, Flocke F M, Roberts J M 2004 J. Geophys. Res. Atmos. 109 D19315 Google Scholar
[8]	Mihelcic D, Volzthomas A, Patz H W, Kley D 1990 J. Atmos. Chem. 11 271 Google Scholar
[9]	Wang D, Hu R, Xie P, Liu J, Liu W, Qin M, Ling L, Zeng Y, Chen H, Xing X, Zhu G, Wu J, Duan J, Lu X, Shen L 2015 J. Quant. Spectrosc. Radiat. Transfer 166 25
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[29]	Wu T, Coeur-Tourneur C, Dhont G, Cassez A, Fertein E, He X, Chen W 2014 J. Quant. Spectrosc. Radiat. Transfer 133 199 Google Scholar
[30]	Fiedler S E, Hese A, Ruth A A 2003 Chem. Phys. Lett. 371 284 Google Scholar
[31]	Lu X, Qin M, Xie P H, Duan J, Fang W, Ling L Y, Shen L L, Liu J G, Liu W Q 2016 Chin. Phys. B 25 024210 Google Scholar
[32]	Washenfelder R A, Langford A O, Fuchs H, Brown S S 2008 Atmos. Chem. Phys. 8 7779 Google Scholar
[33]	Shardanand, Rao A D P 1977 NASA Technical Note
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[35]	Yokelson R J, Burkholder J B, Fox R W, Talukdar R K, Ravishankara A R 1994 J. Phys. Chem. 98 13144 Google Scholar
[36]	Voigt S, Orphal J, Burrows J P 2002 J. Photochem. Photobiol., A 149 1 Google Scholar
[37]	Rothman L S, Jacquemart D, Barbe A, Benner D C, Birk M, Brown L R, Carleer M R, Chackerian C, Chance K, Coudert L H 2005 J. Quant. Spectrosc. Radiat. Transfer 96 139 Google Scholar
[38]	Qin M, Xie P, Su H, Gu J, Peng F, Li S, Zeng L, Liu J, Liu W, Zhang Y 2009 Atmos. Environ. 43 5731 Google Scholar

Cited By

图 1 基于红光LED的宽带腔增强吸收光谱系统示意图

Figure 1. The schematic diagram of broadband cavity enhanced absorption spectrometer based on red LED.

DownLoad: Full-Size Img PowerPoint

图 2 LED光源测试　(a) LED光谱随电流变化规律; (b) LED光谱随温度变化规律

Figure 2. Test of the LED light source: (a) LED spectrum changes with the current; (b) LED spectrum changes with temperature.

DownLoad: Full-Size Img PowerPoint

图 3 镜面反射率标定　(a)黑线是氮气谱, 红线是氦气谱; (b)蓝线为镜面反射率曲线

Figure 3. Calibrations of mirror reflectivity: (a) The black line is nitrogen spectrum, and the red line is helium spectrum; (b) the blue line is the derived curve of mirror reflectivity.

DownLoad: Full-Size Img PowerPoint

图 4 有效腔长标定　(a)NO₂光谱拟合结果(b) NO₂浓度时间序列

Figure 4. Calibration of effective cavity length: (a) Results of NO₂ spectral fitting; (b) time series of NO₂.

DownLoad: Full-Size Img PowerPoint

图 5 实测大气中NO₃的光谱反演实例　(a) 灰线是实测大气的吸收谱, 红线是拟合谱; (b) 灰线是NO₃的吸收谱, 红线是拟合谱, 反演浓度12.2 ± 0.61 pptv; (c) 灰线是NO₂的相对吸收谱, 红线是拟合谱; (d) 灰线是水汽的相对吸收谱, 红线是拟合谱; (e) 拟合残差谱, 标准偏差为8.7 × 10^–10

Figure 5. Spectral inversion example of NO_3: (a) The grey line is the absorption spectrum of the measured atmosphere, and the red line is the fitting spectrum; (b) the gray line is the absorption spectrum of NO₃ and the red line is the fitting spectrum, concentration of NO₃ is 12.2 ± 0.61 pptv; (c) the grey line is the relative absorption spectrum of NO₂, and the red line is the fitting spectrum; (d) the gray line is the relative absorption spectrum of water vapor, and the red line is the fitting spectrum; (e) the gray line is residual spectrum, and the standard deviation of residual spectrum is 8.7 × 10^–10.

DownLoad: Full-Size Img PowerPoint

图 6 检测限分析　(a) NO₃的Allan方差和标准方差随平均时间的变化曲线; (b) 4 s积分时间情况下的NO₃浓度统计图; (c) 4 s积分时间情况下的NO₃浓度时间序列

Figure 6. Analysis of detection limit: (a) Change curves of Allan variance and standard variance of NO₃ with average time; (b) statistical chart of NO₃ concentration with 4 s integration time; (c) time series of NO₃ concentration with 4 s integration time.

DownLoad: Full-Size Img PowerPoint

图 7 观测期间大气NO₃, O₃, NO₂, SO₂时间序列

Figure 7. Time series of Atmospheric NO₃, O₃, NO₂ and SO₂ during observation.

DownLoad: Full-Size Img PowerPoint

map

[1]	Levy H 1971 Science 173 141 Google Scholar
[2]	Wayne R P, Barnes I, Biggs P, Burrows J P, Canosamas C E, Hjorth J, Lebras G, Moortgat G K, Perner D, Poulet G, Restelli G, Sidebottom H 1991 Atmos. Environ. Part A 25 1
[3]	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 Google Scholar
[4]	Stutz J, Alicke B, Ackermann R, Geyer A, White A, Williams E 2004 J. Geophys. Res. Atmos. 109 D12306 Google Scholar
[5]	Platt U, Perner D, Winer A M, Harris G W, Pitts J N 1980 Geophys. Res. Lett. 7 89 Google Scholar
[6]	Wood E C, Wooldridge P J, Freese J H, Albrecht T, Cohen R C 2003 Environ. Sci. Technol. 37 5732 Google Scholar
[7]	Slusher D L, Huey L G, Tanner D J, Flocke F M, Roberts J M 2004 J. Geophys. Res. Atmos. 109 D19315 Google Scholar
[8]	Mihelcic D, Volzthomas A, Patz H W, Kley D 1990 J. Atmos. Chem. 11 271 Google Scholar
[9]	Wang D, Hu R, Xie P, Liu J, Liu W, Qin M, Ling L, Zeng Y, Chen H, Xing X, Zhu G, Wu J, Duan J, Lu X, Shen L 2015 J. Quant. Spectrosc. Radiat. Transfer 166 25
[10]	Wang H, Chen J, Lu K 2017 Atmos. Meas. Tech. 10 1465 Google Scholar
[11]	Wagner N L, Dube W P, Washenfelder R A, Young C J, Pollack I B, Ryerson T B, Brown S S 2011 Atmos. Meas. Tech. 4 1227 Google Scholar
[12]	Li Z, Hu R, Xie P, Wang H, Lu K, Wang D 2018 Sci. Total Environ. 613 131
[13]	Li Z, Hu R, Xie P, Hao C, Liu W 2018 Opt. Express 26 A433 Google Scholar
[14]	Ling L, Xie P, Qin M, Fang W, Jiang Y, Hu R, Zheng N 2013 Chin. Opt. Lett. 11 063001 Google Scholar
[15]	Ball S M, Langridge J M, Jones R L 2004 Chem. Phys. Lett. 398 68 Google Scholar
[16]	Langridge J M, Ball S M, Jones R L 2006 Analyst 131 916 Google Scholar
[17]	Kennedy O J, Ouyang B, Langridge J M, Daniels M J S, Bauguitte S, Freshwater R, McLeod M W, Ironmonger C, Sendall J, Norris O, Nightingale R, Ball S M, Jones R L 2011 Atmos. Meas. Tech. 4 1759 Google Scholar
[18]	Vaughan S, Gherman T, Ruth A A, Orphal J 2008 Phys. Chem. Chem. Phys. 10 4471 Google Scholar
[19]	Wu T, Chen W, Fertein E, Cazier F, Dewaele D, Gao X 2011 Appl. Phys. B 106 501
[20]	Gherman T, Venables D S, Vaughan S, Orphal J, Ruth A A 2007 Environ. Sci. Technol. 42 890
[21]	Min K E, Washenfelder R A, Dubé W P, Langford A O, Edwards P M, Zarzana K J, Stutz J, Lu K, Rohrer F, Zhang Y, Brown S S 2016 Atmos. Meas. Tech. 9 423 Google Scholar
[22]	Duan J, Qin M, Ouyang B, Fang W, Li X, Lu K, Tang K, Liang S, Meng F, Hu Z, Xie P, Liu W, Häsler R 2018 Atmos. Meas. Tech. 11 4531 Google Scholar
[23]	Thalman R, Volkamer R 2010 Atmos. Meas. Tech. 3 1797 Google Scholar
[24]	Liang S, Qin M, Xie P, Duan J, Fang W, He Y, Xu J, Liu J, Li X, Tang K, Meng F, Ye K, Liu J, Liu W 2019 Atmos. Meas. Tech. 12 2499 Google Scholar
[25]	Hoch D J, Buxmann J, Sihler H, Pöhler D, Zetzsch C, Platt U 2014 Atmos. Meas. Tech. 7 199 Google Scholar
[26]	Dorn H P, Apodaca R L, Ball S M, Brauers T, Brown S S, Crowley J N, Dubé W P, Fuchs H, Häseler R, Heitmann U, Jones R L, Kiendler-Scharr A, Labazan I, Langridge J M, Meinen J, Mentel T F, Platt U, Pöhler D, Rohrer F, Ruth A A, Schlosser E, Schuster G, Shillings A J L, Simpson W R, Thieser J, Tillmann R, Varma R, Venables D S, Wahner A 2013 Atmos. Meas. Tech. 6 1111 Google Scholar
[27]	Venables D S, Gherman T, Orphal J, Wenger J C, Ruth A A 2006 Environ. Sci. Technol. 40 6758 Google Scholar
[28]	Meinen J, Thieser J, Platt U, Leisner T 2010 Atmos. Chem. Phys. 10 3901 Google Scholar
[29]	Wu T, Coeur-Tourneur C, Dhont G, Cassez A, Fertein E, He X, Chen W 2014 J. Quant. Spectrosc. Radiat. Transfer 133 199 Google Scholar
[30]	Fiedler S E, Hese A, Ruth A A 2003 Chem. Phys. Lett. 371 284 Google Scholar
[31]	Lu X, Qin M, Xie P H, Duan J, Fang W, Ling L Y, Shen L L, Liu J G, Liu W Q 2016 Chin. Phys. B 25 024210 Google Scholar
[32]	Washenfelder R A, Langford A O, Fuchs H, Brown S S 2008 Atmos. Chem. Phys. 8 7779 Google Scholar
[33]	Shardanand, Rao A D P 1977 NASA Technical Note
[34]	Kern C, Trick S, Rippel B, Platt U 2006 Appl. Opt. 45 2077 Google Scholar
[35]	Yokelson R J, Burkholder J B, Fox R W, Talukdar R K, Ravishankara A R 1994 J. Phys. Chem. 98 13144 Google Scholar
[36]	Voigt S, Orphal J, Burrows J P 2002 J. Photochem. Photobiol., A 149 1 Google Scholar
[37]	Rothman L S, Jacquemart D, Barbe A, Benner D C, Birk M, Brown L R, Carleer M R, Chackerian C, Chance K, Coudert L H 2005 J. Quant. Spectrosc. Radiat. Transfer 96 139 Google Scholar
[38]	Qin M, Xie P, Su H, Gu J, Peng F, Li S, Zeng L, Liu J, Liu W, Zhang Y 2009 Atmos. Environ. 43 5731 Google Scholar

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Broadband cavity enhanced absorption spectroscopy for measuring atmospheric NO₃ radical

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Corresponding author: Qin Min, mqin@aiofm.ac.cn

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Broadband cavity enhanced absorption spectroscopy for measuring atmospheric NO3 radical

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Corresponding author: Qin Min, mqin@aiofm.ac.cn

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Broadband cavity enhanced absorption spectroscopy for measuring atmospheric NO₃ radical