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中国物理学会期刊

    基于亚多普勒wm-NICE-OHMS的14CO2光谱测量技术理论研究

    Theoretical study of14CO2spectrum measurement technology based on sub-Doppler wm-NICE-OHMS

    CSTR: 32037.14.aps.74.20241482
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    • 14CO 2光谱检测在大气环境学和同位素定年等领域中具有重要应用, 但由于其自然丰度极低且光谱重叠干扰严重, 检测难度极大. 基于亚多普勒光谱的噪声免疫腔增强光外差分子光谱(NICE-OHMS)技术因其具有高的灵敏度和选择性, 有望成为下一代 14CO 2检测方法. 本文理论分析了亚多普勒NICE-OHMS光谱测量技术. 通过模拟真实大气光谱, 选择2209.108 cm –1处的 14CO 2跃迁线作为最佳测量目标, 建立了 14CO 2亚多普勒饱和吸收NICE-OHMS模型, 并与多普勒展宽光谱进行对比, 验证了波长调制(wm-)亚多普勒NICE-OHMS技术可有效抑制光谱重叠干扰, 实现高分辨率的 14CO 2光谱测量. 最终, 通过数值模拟分析了压强和调制系数等参数对信号幅度的影响, 确定了最佳实验条件, 为高灵敏 14CO 2光谱测量提供理论依据.

      The massive emission of greenhouse gases, particularly CO 2, has led to severe damage to the Earth’s ecological environment and poses a threat to human health. Many countries have therefore proposed policies to curb the greenhouse effect. Carbon monitoring is a critical prerequisite for realizing these goals, and tracking carbon emission sources can support the precise implementation and advancement of related policies more effectively. The contribution of fossil fuel combustion to greenhouse gas emissions can be inferred by detecting the abundance of 14C in carbon dioxide in a specific region. Conventional 14CO 2detection methods have significant drawbacks, including complicated operation, high cost and large equipment size. Laser absorption spectroscopy (LAS) offers advantages such as real-time, online in-situmeasurement and simple operation, making it suitable for the online detection of isotopes. Among the various LAS techniques, noise immunity cavity enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) is the most sensitive. This method integrates frequency modulation spectroscopy (FMS) into cavity enhanced spectroscopy (CES) to suppress the low-frequency noise while increasing the absorption paths, providing a minimum detectable absorption coefficient as low as 10 –13. Additionally, the accumulation of high intracavity laser power in NICE-OHMS can stimulate saturation absorption, which has a narrow spectral width that can mitigate spectral overlap. In this work, we model the spectral signals of 14CO 2at different locations and select the transition line of 14CO 2at 2209.108 cm –1as an optimal measurement target based on the principles of high-intensity and well-resolution. The theoretical analysis of the NICE-OHMS technique is then carried out, and theoretical simulations of a mixed sample of 14CO 2and its nearby interfering gases ( 13CO 2, 12CO 2, and N 2O), are performed under the simulated experimental conditions. The results of the simulation show that the Doppler broadened spectral signal of 14CO 2is covered by the other gases’ signals with a very low amplitude, which is adverse to the detection of 14CO 2. To eliminate the linear slope of the Doppler broadened signal and to further improve the signal-to-noise ratio, we perform 14CO 2spectral measurements by using wavelength-modulated NICE-OHMS (wm-NICE-OHMS). The results of the simulation show that the spectral lines are effectively separated, and the detection accuracy of the 14CO 2ratio is greatly improved. Finally, the effects of pressure and modulation index on the 14CO 2wm-NICE-OHMS signal are analyzed. The results show that when the pressure is 42 mTorr and the modulation index is 1.07, the signal amplitude of wm-NICE-OHMS reaches its maximum. This work lays a theoretical foundation for the high precision detection of 14CO 2in real-time environmental monitoring. The potential for large-scale application of wm-NICE-OHMS in carbon emission tracking is highlighted, providing a more cost-effective alternative to traditional detection methods. Furthermore, the technology is able to suppress spectral interference from other gases and achieve high resolution in 14CO 2measurements, which will greatly help monitor and reduce greenhouse gas emissions.

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