Multi-harmonic detection in wavelength modulation spectroscopy systems

Two multi-harmonic detection methods for wavelength modulation spectroscopy (WMS) systems are presented and compared. The two possibilities discussed in this paper are: simultaneous curve fitting of multiple harmonic spectra, and reconstruction of the transmission from harmonic coefficients. The optimum number of harmonics is four and 25 harmonics, respectively. Compared with standard single-harmonic curve fitting, the methods give about a factor of 3 better performance than standard second-harmonic curve fitting. Concluding, multi-harmonic detection is better than single-harmonic detection and should be used if the system bandwidth is high enough to allow for proper detection of the higher harmonics.     

基于波长调制技术的激光器调制特性研究

在流场诊断技术中,可调谐半导体吸收光谱技术（TDLAS）成为主要的诊断技术之一,其可实现非接触、原位检测。波长调制（WMS）和直接吸收(DA)是两种最常用的TDLAS气体传感方法,在目标含量很低或者极端流场环境下,波长调制技术呈现出更多的优势,检测灵敏度与直接吸收相比可以提高1～2个数量级。在近红外波长调制技术应用领域,分布反馈式（DFB）半导体激光器成为流场诊断技术的光源选择之一,无论利用谐波信号（或者归一化谐波信号）的线型拟合,还是选择谐波信号的峰值来反演流场参数,吸收模型的准确建立均十分重要。在模型建立时,激光器频率-时间响应以及光强-时间响应的准确表示尤为重要。为解决吸收模型准确建立问题,提出了一种准确测量激光器调制参数的完整方法,通过实验测量了用于探测水汽吸收的1 392和1 469 nm激光器的调制特性,研究了分布反馈式激光器的调制参数随调制幅度,调制频率以及工作温度的变化。根据该方法得到的调制参数,建立吸收模型,测得常温下空气中水汽浓度为1.97%,直接吸收方法测得浓度为1.99%,验证了该测量方法的准确性。研究表明,调制深度随调制幅度的增加线性增加,随调制频率的增加非线性单调减小,随工作温度的升高线性增加;激光器的出光强度和频率同时被调制,强度变化超前频率变化的相位,随调制幅度的变化不明显,随调制频率的增加单调增加,随工作温度的升高单调减小;归一化一次谐波振幅和二次振幅均随调制幅度的增加而增加,随调制频率的增加而减小,随工作温度的变化不明显。在吸收光谱应用领域,波长调制技术发挥的作用愈加重要,调制系数与谐波信号的峰值息息相关,在波长调制技术应用时,选取适当的调制参数,有利于得到合适的谐波信号,可通过改变调制幅度、调制频率、工作温度得到最优调制系数。研究了近红外分布反馈式半导体激光器的调制特性,该方法同样适用于不同封装和不同波段激光器调制特性的研究,利于推广吸收光谱技术在各领域的应用。     

Optical pathlength saturation signatures in wavelength modulation spectroscopy signals of atmospheric molecular oxygen

We discuss experimental and theoretical results of absorption features of the oxygen A-band transitions in the optically thick regime when synchronous detection at higher harmonics (N≥2), using wavelength modulation spectroscopy (WMS), is performed. We show that the absorption saturation effects demonstrate a distinctive feature which results in suppression of the line-center lobes of the harmonic signals. These effects depend on the optical pathlength as well as on the modulation index. The rich structure of WMS signals, especially at higher detection orders, is central to the technique’s advantages in resolving spectra congested with highly disparate oscillator-strength lines. The effect of pathlength saturation on this structure is investigated.     

Self-calibration wavelength modulation spectroscopy for acetylene detection based on tunable diode laser absorption spectroscopy

The expressions of the second harmonic(2f) signal are derived on the basis of absorption spectral and lock-in theories.A parametric study indicates that the phase shift between the intensity and wavelength modulation makes a great contribution to the 2f signal.A self-calibration wavelength modulation spectroscopy(WMS) method based on tunable diode laser absorption spectroscopy(TOLAS) is applied,combining the advantages of ambient pressure,temperature suppression,and phase-shift influences elimination.Species concentration is retrieved simultaneously from selected 2f signal pairs of measured and reference WMS-2f spectra.The absorption line of acetylene(C_2H_2) at 1530.36 nm near-infrared is selected to detect C_2H_2 concentrations in the range of 0-400 ppmv.System sensitivity,detection precision and limit are markedly improved,demonstrating that the self-calibration method has better detecting performance than the conventional WMS.     

CO在1. 578 μ m的可调谐二极管激光光谱信号小波去噪研究

研究了一氧化碳(CO)近红外波段直接吸收和波长调制信号去噪处理算法。从HATRAN数据库中得到CO气体的吸收信号作为仿真数据,提取直接吸收信号、1-f和2-f解调信号作为原始信号,研究了不同小波基以及不同的分解层数对叠加高斯白噪声的光谱信号去噪的效果。最后利用基长为0.95 m有效光程为55.1 m的Herriott型多光程池对CO在1.578 μm处的第二泛频带P(4)吸收谱线信号进行测量和信号处理,与原始信号相比,经过信号处理过的直接吸收、1-f和2-f解调信号的信噪比都提高1～2个数量级;通过选择不同小波基和优化小波变换层数,增加了系统的抗干扰能力。     

Wavelength-modulation-spectroscopy for real-time, in situ NO detection in combustion gases with a 5.2 μm quantum-cascade laser

A mid-infrared absorption strategy with calibration-free wavelength-modulation-spectroscopy (WMS) has been developed and demonstrated for real-time, in situ detection of nitric oxide in particulate-laden combustion-exhaust gases up to temperatures of 700 K. An external-cavity quantum-cascade laser (ECQCL) near 5.2 μm accessed the fundamental absorption band of NO, and a wavelength-scanned, 1f-normalized WMS with second-harmonic detection (WMS-2f/1f) strategy was developed. Due to the external-cavity laser architecture, large nonlinear intensity modulation (IM) was observed when the wavelength was modulated by injection-current modulation, and the IM indices were also found to be strongly wavelength-dependent as the center wavelength was scanned with piezoelectric tuning of the cavity. A quantitative model of the 1f-normalized WMS-2f signal was developed and validated under laboratory conditions. A sensor was subsequently designed, built and demonstrated for real-time, in situ measurements of NO across a 3 m path in the particulate-laden exhaust of a pulverized-coal-fired power plant boiler. The 1f-normalized WMS-2f method proved to have better noise immunity for non-absorption transmission, than wavelength-scanned direct absorption. A 0.3 ppm-m detection limit was estimated using the R15.5 transition near 1927 cm⁻¹ with 1 s averaging. Mid-infrared QCL-based NO absorption with 1f-normalized WMS-2f detection shows excellent promise for practical sensing in the combustion exhaust.     

Wavelength modulation spectroscopy based on quasi-continuous-wave diode lasers

A modified wavelength modulation spectroscopy（WMS）based on the self-heating effect of the tunable diode laser when driven in quasi-continuous-wave（QCW）mode is investigated.A near-infrared distributed feedback（DFB）diode laser working at the QCW mode is employed as the QCW light source,and CO2 is selected as the target gas.The characteristic of the QCW second harmonic（2f）line profile is analyzed through a comparison with that of the traditional CW WMS with the same system.A noise-equivalent absorbance of 3.2×10-5 Hz-1/2 for CO2 at 1.58μm is obtained with 18-m optical path.The QCW WMS lowers the dependence on lasers and expands selectivity,thus verifying the feasibility of the method.     

Absorption linewidth inversion with wavelength modulation spectroscopy

For absorption linewidth inversion with wavelength modulation spectroscopy(WMS), an optimized WMS spectral line fitting method was demonstrated to infer absorption linewidth effectively, and the analytical expressions for relationships between Lorentzian linewidth and the separations of first harmonic peak-to-valley and second harmonic zero-crossing were deduced. The transition of CO_2 centered at 4991.25 cm~(-1) was used to verify the optimized spectral fitting method and the analytical expressions. Results showed that the optimized spectra fitting method was able to infer absorption accurately and compute more than 10 times faster than the commonly used numerical fitting procedure. The second harmonic zero-crossing separation method calculated an even 6 orders faster than the spectra fitting without losing any accuracy for Lorentzian dominated cases. Additionally, linewidth calculated through second harmonic zero-crossing was preferred for much smaller error than the first harmonic peak-to-valley separation method. The presented analytical expressions can also be used in on-line optical sensing applications, electron paramagnetic resonance, and further theoretical characterization of absorption lineshape.     

连续和准连续调制激光吸收光谱的软件锁相解调比较研究

根据对激光器施加的调制信号是否连续,波长调制光谱分为连续和准连续调制激光吸收光谱技术。为了深入的比较研究这两种方案,设计准连续调制谱专用的软件锁相放大器,将准连续调制信号因间断产生的无效信号滤除后,再对吸收信号解调得到二次谐波信号。与连续激光调制谱软件解调的二次谐波信号进行了比较,结果表明,参数相同,准连续调制谱比连续调制谱的信噪比提高5%、检测限降低11.3%。在滤除无效信号后,准连续调制谱也可以解调出标准的二次谐波信号,因此有望用于与气体线型相关的研究中。该工作为选取更加适用的激光调制谱技术,提供了准确依据。     

中红外痕量乙烷传感器设计与稳定性分析

根据乙烷气体分子在3.3 μm处的基频吸收特性,使用中心波长为3.337 μm室温连续带间级联激光器(ICL)和有效光程为54.6 m密集光斑多通气体吸收气室(600 mL)研制了基于波长调制光谱技术(WMS)的乙烷传感器。详细介绍了基于WMS和二次谐波(2f)探测技术的光谱吸收法气体检测原理,给出了目标乙烷气体吸收线的遴选细节。此项技术的使用减小了光功率漂移对系统的影响,使得系统最低检测下限(MDL)和稳定性能得到提升。结合原理框图,通过光学和电学两个模块分别详细介绍了乙烷传感系统设计方案,描述了自主研制的软、硬件单元和商用仪器的使用及其型号供他人参考,并给出传感器光学配置实物图。而且,为匹配激光波长调制与基于压力的吸收线宽,对气压和调制深度进行优化,研究了调制幅度对应2f信号峰值及调制幅度与调制深度的关系,最终确定最优气压和调制深度分别为100 Torr和0.074 cm-1,对应的调制信号幅度为~0.026 V。此外,基于优化后的气压和调制深度,使用136.8 nmol·mol-1 乙烷标准气体进行了系统灵敏度估算。详细介绍了ICL扫描调制信号、锁相放大及数据采集单元的参数设置,并给出示波器记录的扫描调制信号及2f信号波形图片。通过对比DAQ采集的2f信号和背景噪声信号,估算系统最低检测下限为33 nmol·mol-1。最后,使用9个不同浓度乙烷标准气体(20～400 nmol·mol-1)分别进行~5 min系统标定测试,并列出了拟合曲线和拟合相关度等信息。而且,使用浓度为48 nmol·mol-1乙烷气体样品开展连续2 h系统稳定性测试并进行Allan-Werle 方差分析。结果显示,该系统工作稳定,积分时间为4 s时,乙烷气体检测灵敏度为~0.81 nmol·mol-1。通过增加系统积分时间至63 s,系统灵敏度可被提高至~0.36 nmol·mol-1。     

高功率超短脉冲激光系统中光谱增益窄化补偿的调制函数

设计了一种与高功率超短脉冲激光放大过程中获得的总增益、增益介质的带宽、激光带宽、脉冲中心波长等参数相关的调制函数,对激光放大过程中的光谱增益窄化进行补偿。此调制函数的优越性在于,对不同性能的激光系统,无需改变调制函数的形式就能适用。通过数值模拟的方法,讨论了在不同增益介质带宽、激光带宽、脉冲中心波长下的补偿效果。此调制函数在高功率超短脉冲激光系统中有良好的应用前景。     

CO2分子的近红外二极管激光吸收光谱灵敏探测

利用近红外二极管激光波长调制技术与二次谐波探测结合初步观测了CO2 分子在波长 1.5 7μm附近的吸收 ,获得了最小可探测吸收为 8.6× 10 -5(信噪比为 2 ) ,对应 5 0 0× 10 -6m-1的探测灵敏度。     

高功率超短脉冲激光系统中光谱增益窄化补偿的调制函数

 设计了一种与高功率超短脉冲激光放大过程中获得的总增益、增益介质的带宽、激光带宽、脉冲中心波长等参数相关的调制函数,对激光放大过程中的光谱增益窄化进行补偿。此调制函数的优越性在于,对不同性能的激光系统,无需改变调制函数的形式就能适用。通过数值模拟的方法,讨论了在不同增益介质带宽、激光带宽、脉冲中心波长下的补偿效果。此调制函数在高功率超短脉冲激光系统中有良好的应用前景。     

Cost-effective and dispersion-tolerant cascade modulation for millimeter-wave-over-fiber applications

In millimeter-wave-over-fiber (MWoF) feeder systems, the received millimeter-wave signals at the remote antennas (RAs) can suffer from signal fading by chromatic dispersion of optical fiber. This can be substantially mitigated by Mach-Zehnder modulator (MZM) based photonic up-conversion technique. In this technique, the data signals at intermediate frequency (IF) are frequency up-converted to millimeter-wave frequency by an MZM biased at its transmission null point. However, this scheme requires a costly, high-speed MZM, which will hinder the widespread of this technique for cost-sensitive MWoF applications. Hence, we propose and demonstrate a cost-effective way of reducing the cost of MWoF optical transmitters based on photonic up-conversion technique. We employ a dual wavelength source composed of a directly modulated laser and a polarimetric filter. This source is used to generate a millimeter-wave tone signal and to frequency up-convert the IF data signals to millimeter-wave frequency. The dual wavelength source is also shared with numerous RAs for further cost reduction. Our experimental demonstration performed with 30 Msymbol/s 16-quadrature amplitude modulation signals shows that we can transmit the 20 GHz millimeter-wave signals over 25 km standard single-mode fiber without any transmission penalty.     

紫外域多纵模高光谱分辨率激光雷达探测气溶胶的技术实现和系统仿真

多纵模高光谱分辨率激光雷达是一种新型的高光谱分辨率激光雷达.本文在研究典型高功率Nd:YAG脉冲激光器的多纵模模式及其在大气中传输的气溶胶米散射和瑞利散射光谱的基础上,设计紫外域多纵模高光谱分辨率激光雷达系统,采用窄带干涉滤光片滤除太阳背景光的影响,设计可调谐马赫-曾德尔干涉仪,分离提取多纵模激光回波中的气溶胶米散射和瑞利散射光谱,并利用马赫-曾德尔干涉仪双通道输出的互补性原理,精确反演气溶胶光学参量.系统仿真结果表明,所设计的紫外域多纵模高光谱分辨率激光雷达能够实现10 km高度内的气溶胶光学参量精细探测.     

可调谐二极管激光吸收光谱二次谐波信号的模拟与分析

可调谐二极管激光吸收光谱技术(TDLAS)作为近年来发展起来的一种气体检测技术,具有高分辨率、高灵敏度和快速测量等特点。波长调制光谱信号的二次谐波分量常作为检测信号,用于气体浓度信息的反演。利用MATLAB中的可视化建模仿真平台Simulink,模拟了基于TDLAS的波长调制光谱信号,利用锁相放大原理提取二次谐波分量。采用数字锁相,正交双通道结构实现锁相算法。通过比较不同调制系数下二次谐波信号的变化情况,分析了二次谐波信号与调制系数的关系,以便确定最佳参数,用于二次谐波的提取。     

Inline multi-harmonic calibration method for open-path atmospheric ammonia measurements

We demonstrate a real-time inline calibration method for an open-path ammonia sensor using a quantum cascade laser (QCL) at 9.06 μm. Ethylene (C₂H₄) has an absorption feature partially offset from the ammonia absorption feature, and the ethylene signal serves as a reference signal for ammonia concentration in real time. Spectroscopic parameters of ammonia and ethylene are measured and compared with the HITRAN database to ensure the accuracy of the calibration. Multiple harmonic wavelength modulation spectroscopy (WMS) signals are used to separate the ambient ammonia and reference ethylene absorption signals. The ammonia signal is detected with the second harmonic (2f), while it is calibrated simultaneously with a high-harmonic (6–12f) signal of ethylene. The interference of ambient ammonia absorption on the ethylene reference signal is shown to be negligible when using ultra high-harmonics (≥6f). This in situ calibration method yields a field precision of 3 % and accuracy of 20 % for open-path atmospheric ammonia measurements.     

Multi-mode absorption spectroscopy, MUMAS, using wavelength modulation and cavity enhancement techniques

Multi-mode absorption spectroscopy, MUMAS, has been combined with the techniques of wavelength modulation spectroscopy, WMS, and cavity enhanced absorption spectroscopy, CEAS, to record multiple molecular transitions using a single laser and a single detector. MUMAS signals were recorded using a multi-mode diode laser of the A-band $b^{1}\varSigma _{g}^{+}\leftarrow X^{3}\varSigma _{g}^{-}Multi-mode absorption spectroscopy, MUMAS, has been combined with the techniques of wavelength modulation spectroscopy, WMS, and cavity enhanced absorption spectroscopy, CEAS, to record multiple molecular transitions using a single laser and a single detector. MUMAS signals were recorded using a multi-mode diode laser of the A-band b¹\varSigma _g⁺? X³\varSigma _g^-b^{1}\varSigma _{g}^{+}\leftarrow X^{3}\varSigma _{g}^{-} of molecular oxygen at 760 nm. Direct MUMAS and WMS-MUMAS signals were recorded using a White cell for air and pure oxygen for pressures in the range 0 to 1 bar. CEAS-MUMAS signals were recorded with and without WMS in an open enhancement cavity containing laboratory air. Enhancement of the signal-to-noise ratio has been obtained demonstrating the potential for increased detection sensitivity for gas-sensing applications of MUMAS.     

准连续激光调制吸收光谱的解调方法研究

针对准连续激光调制吸收光谱谐波信号的解调,设计了一种专用的准连续软件锁相放大器,对采集的数据做有效性判断、 无效数据滤除、 数字相敏检测、 数字滤波等处理,实现了准连续激光调制吸收光谱的谐波信号解调。 构建气体检测实验系统,对准连续软件锁相放大器和商品化的高性能锁相放大器进行了对比实验,结果表明,使用准连续软件锁相放大器的Allan方差比后者小1个数量级、 检测限低2倍。 并能够解决小占空比时的信号失锁问题,具有小的信号波形失真。