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激光外差光谱探测由于其光谱分辨率高、体积小、重量轻等优点近年来得到了快速的发展, 可用于大气温室气体垂直廓线测量和碳卫星地面定标等. 本文报道了利用3.939 µm带间级联激光器作为本振光源的测量大气N2O的激光外差系统, 自制高精度太阳跟踪仪收集太阳光作为激光外差的信号光源, 其跟踪精度达到7 arcsec, 激光外差系统的光谱分辨率达到0.004 cm–1, 测量了合肥地区(31.902°N, 117.167°E)大气N2O吸收光谱, 得到2838.336和2539.344 cm–1两个强吸收峰, 并对吸收信号进行波长标定, 得到了N2O分子的整层大气透过率谱, 信噪比为93. 将高分辨率光谱数据进行归一化处理和频率校正, 利用参考正向模型和最优估计算法得到N2O大气整层浓度廓线, 标准偏差体积分数为0.000031 × 10–6—0.0026 × 10–6, 对应相对误差范围为0.009%—0.83%. 研究结果表明, 所搭建的激光外差系统能够实现对大气中N2O的吸收光谱测量以及对N2O的廓线反演, 为长期观测大气N2O浓度提供保证.aser heterodyne spectroscopy detection has rapidly developed in recent years due to its high spectral resolution, small size, and light weight. It can be used to measure the atmospheric greenhouse gas vertical profile and calibrate the carbon satellite ground. This paper reports a laser heterodyne system for measuring atmospheric N2O, with a 3.939-µm interband cascade laser used as a local oscillator light source. A homemade high-precision solar tracker collects sunlight as a laser heterodyne signal source. The tracking accuracy reaches 7 arcsec, and the spectral resolution of the laser heterodyne system arrives at 0.004 cm–1. The atmospheric N2O absorption spectrum in Hefei area (31.902°N, 117.167°E) is measured, and two strong absorption peaks respectively at 288.336 and 2539.344 cm–1 are obtained. In addition, the wavelength calibration of the absorption signal, and the entire atmospheric transmittance spectrum of N2O molecules are obtained, and the signal-to-noise ratio is 93. The high-resolution spectrum data are normalized and frequency is corrected, and the N2O atmospheric concentration profile is obtained by using the reference forward model and the optimal estimation algorithm. The standard deviation of volume fraction is in a range of 0.000031—0.0026 ppm, and the corresponding relative error range is 0.009%—0.83%. The research results show that the laser heterodyne system built in this work can be used to measure the absorption spectrum of N2O in the atmosphere and realize the inversion of the N2O profile, which provides a guarantee for long-term observation of atmospheric N2O concentration.
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图 2 (a)太阳跟踪仪内部装置; (b)精跟踪模式下太阳光斑质心偏移量
Fig. 2. (a) Internal device of suntracker; (b) sunlight spot centroid offset in precision tracking mode.
图 3 系统结构原理图(LIA, 锁相放大器; PC, 电脑; DAQ, 数据采集卡; FL1, 2, 聚焦透镜1, 2; BS1, 2, 分束器1, 2)
Fig. 3. System structure schematic diagram. LIA, lock-in amplifier; PC, personal computer; DAQ, data acquisition card; FL1, 2, focus lens 1, 2; BS1, 2, beam splitter 1, 2.
图 5 (a) 射频信号功率谱; (b) 仪器函数
Fig. 5. (a) RF signal power spectrum; (b) instrument functions.
图 7 (a) N2O吸收的外差信号; (b) 激光器波数与注入电流的关系
Fig. 7. (a) Heterodyne signal absorbed by N2O; (b) the relationship between laser wavenumber and injection current.
图 8 实验所得N2O吸收光谱与模拟吸收光谱的对比
Fig. 8. Comparison of the N2O absorption spectrum obtained in the experiment and the simulation absorption spectrum.
图 10 LHR数据反演结果 (a) 实验和拟合LHR谱图; (b) 残差
Fig. 10. Inversion results of LHR data: (a) Experimental and fitted LHR spectrogram; (b) residual.
图 12 N2O的先验和反演的垂直浓度分布图(VMR表示体积混合比)
Fig. 12. Prior and inversion vertical concentration profiles of N2O. VMR, volume mixing ratio.
表 1 3.9 µm激光外差系统的参数设置
Table 1. Parameter setting of 3.9 µm laser heterodyne system.
参数 数值 太阳光传输效率 0.305 滤波带宽/MHz 60 太阳温度/K 5773 测量波长/m 3.939 积分时间/s 0.3 
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[1] 向亮, 高庆先, 周锁铨, 陈永立 2009 气候变化研究进展 5 278
Xiang L, Gao Q X, Zhou S Q, Chen Y L 2009 Adv. Clim. Change Res. 5 278
[2] 邵君宜, 林兆祥, 刘林美, 龚威 2017 物理学报 66 104206
Google Scholar
Shao J Y, Lin Z X, Liu L M, Gong W 2017 Acta Phys. Sin. 66 104206
Google Scholar
[3] 王薇, 刘文清, 张天舒 2014 光学学报 34 0130003
Google Scholar
Wang W, Liu W Q, Zhang T S 2014 Acta Opt. Sin. 34 0130003
Google Scholar
[4] Zhao Y J, Wexler A S, Hase F, Pan Y, Mitloehner F M 2016 J. Environ. Prot. Ecol. 7 1719
Google Scholar
[5] Clarke G B, Wilson E L, Miller J H, et al. 2014 Meas. Sci. Technol. 25 055204
Google Scholar
[6] Palmer P I, Wilson E L, Villanueva G L, et al. 2019 Atmos. Meas. Tech. 12 2579
Google Scholar
[7] Weidmann D, Tsai T R, Macleod N A, et al. 2011 Opt. Lett. 36 1951
Google Scholar
[8] Tsai T R, Rose R A, Weidmann D, et al. 2012 Appl. Opt. 51 8779
Google Scholar
[9] Wilson E L, McLinden M L, Miller J H, et al. 2013 Appl. Phys. B 114 385
Google Scholar
[10] Wilson E L, DiGregorio A J, Villanueva G, et al. 2019 Appl. Phys. B 125 211
Google Scholar
[11] Rodin A, Klimchuk A, Nadezhdinskiy A, et al. 2014 Opt. Express 22 13825
Google Scholar
[12] 谈图, 曹振松, 王贵师, 等 2015 光谱学与光谱分析 35 1516
Google Scholar
Tan T, Cao Z S, Wang G S, et al. 2015 Spectrosc. Spectral Anal. 35 1516
Google Scholar
[13] Wang J, Wang G, Tan T, et al. 2019 Opt. Express 27 9610
Google Scholar
[14] Parvitte B, Zéninari V, Thiébeaux C, et al. 2004 Spectrochim. Acta, Part A 60 1193
Google Scholar
[15] Gisi M, Hase F, Blumenstock T 2011 Atmos. Meas. Tech. 4 47
Google Scholar
[16] Siegman A E 1966 Appl. Opt. 5 1588
Google Scholar
[17] 张尚露, 黄印博, 卢兴吉, 曹振松, 戴聪明, 刘强, 高晓明, 饶瑞中, 王英俭 2019 光谱学与光谱分析 39 1317
Google Scholar
Zhang S L, Huang Y B, Lu X j, Cao Z S, Dai C M, Liu Q, Gao X M, Zhong R R, Wang Y J 2019 Spectrosc. Spectral Anal. 39 1317
Google Scholar
[18] Rodgers C D 2000 Inverse Methods for Atmospheric Sounding: Theory and Practise (1st Ed.) (Singapore: World Scientific Publishing)
[19] Rodgers C D 1990 J. Geophys. Res. 95 5587
Google Scholar
[20] Weidmann D, Reburn W J, Smith K M 2007 Appl. opt. 46 7162
Google Scholar
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