论文标题

使用具有明显强度变化的光源,用于基线不敏感的吸收光谱的曲线分析

Cepstral Analysis for Baseline-Insensitive Absorption Spectroscopy Using Light Sources with Pronounced Intensity Variations

论文作者

Goldenstein, Christopher S., Mathews, Garrett C., Cole, Ryan K., Makowiecki, Amanda S., Rieker, Gregory B.

论文摘要

该手稿提出了一种数据处理技术,该技术通过使用cepstral分析从基线光强度(IO)中的误差中隔离分子吸光度信号来提高吸收 - 光谱测量的准确性和精度。最近,曲线分析已与传统的吸收光谱仪一起使用,以创建一种时间域分子自由诱导衰减(M-FID)信号的修改形式,该信号可以独立于IO分析。但是,当基线强度和分子响应在时域中不能很好地分离时,无法对分子特征进行独立的分析,这在使用注射电流调节激光器(例如量子级联激光器)和其他具有明显强度调节的光源时是典型的。相反,此处介绍的方法适用于所有光源,因为它通过将模拟的M-FID信号拟合到时域中的M-FID信号的最小二乘确定气体性能。此方法对估计的IO中的错误不敏感,该误差随光学频率而缓慢变化,因此在时域迅速衰减。该方法提供的好处是通过用分布式反馈(DFB)量子cascade激光器(QCL)获得的扫描波长直接吸收测量值证明的。在CO的P(0,20)和P(1,14)的吸收转变时,在1 kHz的P(1,14)吸收过渡中扫描了DFB QCL的波长,以测量气体温度和浓度。使用新的基于M-FID的方法和两种传统方法处理测得的光谱,这些方法依赖于在光谱拟合程序中推断基线误差。基于M-FID的方法在所有情况下都表现出卓越的精度,并且测量精度比使用传统方法提供的测量精度比提供的精度高1.5至10倍。

This manuscript presents a data-processing technique which improves the accuracy and precision of absorption-spectroscopy measurements by isolating the molecular absorbance signal from errors in the baseline light intensity (Io) using cepstral analysis. Recently, cepstral analysis has been used with traditional absorption spectrometers to create a modified form of the time-domain molecular free-induction decay (m-FID) signal which can be analyzed independently from Io. However, independent analysis of the molecular signature is not possible when the baseline intensity and molecular response do not separate well in the time domain, which is typical when using injection-current-tuned lasers (e.g., quantum cascade lasers) and other light sources with pronounced intensity tuning. In contrast, the method presented here is applicable to all light sources since it determines gas properties by least-squares fitting a simulated m-FID signal to the measured m-FID signal in the time domain. This method is insensitive to errors in the estimated Io which vary slowly with optical frequency and, therefore, decay rapidly in the time domain. The benefits provided by this method are demonstrated via scanned-wavelength direct-absorption measurements acquired with a distributed-feedback (DFB) quantum-cascade laser (QCL). The wavelength of a DFB QCL was scanned across CO's P(0,20) and P(1,14) absorption transitions at 1 kHz to measure the gas temperature and concentration of CO. Measurements were acquired in a gas cell and in an ethylene-air flame at 1 atm. The measured spectra were processed using the new m-FID-based method and two traditional methods which rely on inferring the baseline error within the spectral-fitting routine. The m-FID-based method demonstrated superior accuracy in all cases and a measurement precision that was 1.5 to 10 times smaller than that provided using traditional methods.

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