NH<sub>3</sub> aliasing absorption spectra at 1103.4 cm<sup>–1</sup> based on continuous quantum cascade laser

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Abstract

Due to the important role of NH ₃in atmospheric aerosol chemistry, rapid and accurate inversion of ammonia concentration is very important for environmental issues. In this paper, a 9.05 μm continuous quantum cascade laser (QCL) is used as the light source at room temperature, and the scanned-wavelength direct-absorption tunable diode laser absorption spectroscopy (TDLAS) is used to study the spectral characteristics of the QCL at 1103.4 cm ^–1. A low-pressure experimental platform based on two-level temperature control was designed to measure the six aliasing absorption lines of ammonia at 1103.4 cm ^–1. The broadening of spectral line becomes smaller under the condition of reducing the pressure, and the aliasing spectra are separated. The line strength of each absorption line is calculated, and the measurement uncertainty is further analyzed. A method for accurate inversion of single-spectrum gas concentration by low-pressure separation was proposed for severely aliased spectra, and experimental verification was performed. By comparing the results with the HITRAN database, it is concluded that the experimental measured line strength of ammonia gas at 1103.4 cm ^–1has a deviation from the database of . The uncertainty of the line intensity measurement is mainly related to the separation and extraction of aliasing absorbance, which is about 2.42%–8.92%. The deviation between the inversion concentration and the actual value under the condition of extreme low pressure is between 1% and 3%, while the calculated deviation of the line intensity value in the 2.71%–4.71% HITRAN database is about 3% to 5%. The results above indicate that the experimental data are reliable. The non-separative aliasing spectral line method is used to invert the concentration at normal pressure, and the low-pressure separated single spectral line method is used to invert the concentration at low pressure. The results of the two are compared. The analysis results show that the low-pressure separation single-spectrum spectral line inversion concentration value has smaller deviation and higher accuracy from the original concentration. The study of this method provides reference for future inversion of gas concentrations inversion in the atmospheric environment and other fields.

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Corresponding author:Zhang Yu-Jun,yjzhang@aiofm.ac.cn

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同位素 Isotopologue	波数 ν/cm^–1	线强 S/(cm^–1/(molecule cm^–2))	空气展宽 γ_air/cm^–1·atm^–1	自展宽 γ_self/cm^–1·atm^–1	爱因斯坦系数 A/s^–1
¹⁴NH₃	1103.43047	7.119 × 10^–²⁰	0.0875	0.452	7.183
¹⁴NH₃	1103.43432	6.131 × 10^–²⁰	0.0933	0.521	5.263
¹⁴NH₃	1103.44122	1.514 × 10^–19	0.0818	0.388	8.654
¹⁴NH₃	1103.46978	7.756 × 10^–²⁰	0.0763	0.328	9.694
¹⁴NH₃	1103.47951	8.172 × 10^–²⁰	0.0994	0.595	2.877
¹⁴NH₃	1103.48575	7.824 × 10^–²⁰	0.071	0.274	10.32

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v₀/cm^–1	S_H/cm^–2atm^–1	S_M/cm^–2atm^–1	E/%
1103.43047	1.78339	1.70439	4.43
1103.43432	1.53589	1.46362	4.71
1103.44122	3.79275	3.6901	2.71
1103.46978	1.94297	1.87825	3.33
1103.47951	2.04718	1.97089	3.73
1103.48575	1.96001	1.88383	3.89

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	积分吸光度的不确定度 ΔA/%	压强的不确定度 ΔP/%	浓度的不确定度 Δm/%	光程的不确定度 ΔL/%	温度的不确定度 ΔT/%	线强的不确定度 ΔS/%
min	2.42	0.15	0.2	0.2	0.1	2.44
max	8.92	0.15	0.2	0.2	0.1	8.93

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实验气压/ torr	HITRAN数据库线强反演浓度m₁/ppm	实验测量线强反演浓度m₂/ppm	m₁与实际浓度偏差/%	m₂与实际浓度偏差/%
3.2	104.98	102.55	4.98	2.55
8.5	103.89	101.94	3.89	1.94
12.6	102.90	101.40	2.90	1.40
19.7	103.08	101.07	3.08	1.07
25.4	103.22	101.00	3.22	1.00
31.8	106.23	102.88	6.23	2.88
90.7	108.53	104.91	8.53	4.91
760	108.86	104.93	8.86	4.93

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压力P/torr	反演浓度 m₁,m₂/ppm	标气浓度m/ppm
压力P/torr	反演浓度 m₁,m₂/ppm	3.2	8.5	12.6	19.7	25.4	760
151.68	m₁	156.68	155.32	154.73	154.79	154.81	159.62
151.68	m₂	154.12	153.54	153.05	152.77	152.70	155.48
202.00	m₁	207.13	206.67	205.14	205.45	205.86	210.97
202.00	m₂	205.25	204.73	204.29	203.88	203.82	207.06
250.34	m₁	256.08	255.03	254.26	254.45	254.71	260.25
250.34	m₂	254.37	253.79	253.25	252.91	252.86	256.61
413.00	m₁	420.47	419.73	418.18	418.55	418.94	423.77
413.00	m₂	419.65	418.33	417.61	416.87	416.76	420.51

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Vol. 69, Issue 7 - 2020-04-05

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