基于量子级联激光器的气体光谱检测关键技术
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摘要
由于量子级联激光器（Quantum Cascade Laser：QCL）具有发射功率高、线宽窄、能在室温下工作等特点，基于量子级联激光器的气体光谱检测技术与装备已成为近年来的研究热点。
论文针对气体检测技术中存在的分辨率、灵敏度等问题，开展基于量子级联激光器的气体光谱检测系统关键技术研究。重点研究了基于量子级联激光器的气体光谱检测系统的光谱扫描理论与方法，并对不同温度下的脉冲内光谱扫描进行了模拟分析；研究了气体光谱检测系统的差分吸收光谱技术和基于F-P标准具的频率标定技术的相关理论与实现方法，设计并搭建了基于量子级联激光器的气体光谱检测系统，完成了该系统的性能测试与分析；以甲烷和甲醛为具体检测对象，基于HITRAN的JavaHAWKs和PGOPHER软件进行了相应吸收光谱的计算与模拟，完成了甲烷和甲醛红外吸收光谱的定性与定量检测，测试验证了基于量子级联激光器的气体光谱检测系统的主要性能；基于该系统，进行了甲醛的吸收强度、压力展宽效应、压力频移效应和光谱非线性效应的实验研究，获得了较满意的实验结果。
本论文主要研究工作是：
①论文分析了气体检测技术的研究现状、存在的科学与技术问题，提出了基于中红外量子级联激光器的气体检测系统结构与实现方法，确定了基于量子级联激光器的气体光谱检测系统方案；
②研究了量子级联激光器的气体光谱检测系统的光谱检测理论与方法，分析研究了基于脉冲电流调谐的量子级联激光器的光谱扫描理论与具体实现方法；
③基于气体分子的红外吸收光谱特性，研究了基于量子级联激光器的气体光谱检测的相关理论与方法；采用差分吸收光谱检测技术，解决了气体检测中存在的部分干扰等问题，提高了系统检测灵敏度与检测精度；基于F-P标准具的频率标定技术，解决了中红外波段气体检测系统中时域与频域标定的技术问题；
④提出了基于分布反馈式脉冲量子级联激光器的气体光谱检测系统的总体结构设计方案，搭建了系统实验平台，完成了系统波长范围、分辨率、重复性、稳定性和检测灵敏度等性能的测试分析；
⑤基于本论文搭建的气体检测系统，完成了甲烷和甲醛气体吸收光谱的采集；基于HITRAN的JavaHAWKs和PGOPHER软件对甲烷和甲醛气体吸收光谱进行了模拟，比较模拟光谱与实验光谱的吸收峰数目、位置以及相对吸收强度，完成了吸收光谱的定性分析；完成了甲烷和甲醛气体吸收光谱的采集和处理，基于Beer-Lambert定律的光谱积分面积的计算方法，获得了混合气体中甲烷和甲醛的浓度值，完成了两种气体的定量测试；
⑥基于本实验平台，对甲醛气体吸收光谱的“Rapid Passage”非线性效应、吸收强度、压力展宽和压力频移效应进行了相应参数分析，获得了比较满意的实验结果；
⑦进行论文研究工作的总结，提出了存在的问题与下一步工作思路。
Due to the characteristics of high output power, narrow line-width, roomtemperature operation and so on, Quantum Cascade Lasers (QCLs) have become theresearch focus in the fields of trace gas detection technology and instrumentalintegration system.
This thesis aimed at the issues existed in the gas detection technology andinstrument system researching, key technologies in gas spectroscopy detectiontechnology based on Quantum Cascade Laser were carried out. And also importantlyfocused on the fundamental theory of quantum cascade laser based spectrum scanningmethod by applying a pulse current to the QCL, and also different spectral ranges wereobtained by tuning the QCL operation temperatures; Research work of theory andrealization methods were also carried out by analysing differential optical absorptionspectroscopy and technology based on F-P etalon, then design and set-up the gasdetection experimental system based on quantum cascade laser, and measured thesystem stability and other characteristics; Take methane (CH4) and formaldehyde(H2CO) as the detection gases, firstly simulated their spectrum using HITRAN andPGOPHER, then calculated the relative parameters and results. Testing measurementsresults showed that the quantum cascade laser based gas spectroscopy detection systemhas a relatively high detection sensitivity and resolution. Absorption line intensity,pressure broadening and pressure induced frequency shift parameters of formaldehyde(H2CO) were measured using the system and good results were obtained.
The mainly research works in this thesis were:
①Gas detection technology status, existing matters were compared and analysedin this thesis and them gas spectroscopy detection system and realization method wereproposed, the research scheme was confirmed as pulsed distribute feedback quantumcascade laser based gas detection system and technology.
②Spectrum scanning theory and methods were researched based on distributefeedback quantum cascade laser, and analysis works were carried out by using pulsecurrent tuning method.
③Based on the molecular absorption specificity, fundamental knowledge andmethod were researched based on quantum cascade laser system; by utilizing the gasdetection technology, noise from the environment and other absorptive gases absorption were deducted, and then the sensitivity would be improved. Frequency calibration wasdone by analysing the F-P etalon signal recorded from the experimental system.
④Design scheme was proposed as distribute feedback quantum cascade laserbased gas spectroscopy detection, then each functional modal was tested and set-up,then the whole experimental system was done. Spectral range, resolution, absorbancerepetition, stability and detection limit were measured based on this system;
⑤Take methane (CH4) and formaldehyde (H2CO) as the detection gases, theirspectra were recorded and analysed, then compared with the HITRAN and PGOPHERsimulation, and spectrum parameters were calculated.
⑥Specially, detection work of H2CO was done by measuring its absorption lineintensity, pressure broadening coefficient, pressure induced frequency shift and theRapid Passage effect, and the corresponding results were calculated and analysed.
⑦The thesis conclusion was done, and then bring forward the existent matters andconsiderations for the future work.
论文针对气体检测技术中存在的分辨率、灵敏度等问题，开展基于量子级联激光器的气体光谱检测系统关键技术研究。重点研究了基于量子级联激光器的气体光谱检测系统的光谱扫描理论与方法，并对不同温度下的脉冲内光谱扫描进行了模拟分析；研究了气体光谱检测系统的差分吸收光谱技术和基于F-P标准具的频率标定技术的相关理论与实现方法，设计并搭建了基于量子级联激光器的气体光谱检测系统，完成了该系统的性能测试与分析；以甲烷和甲醛为具体检测对象，基于HITRAN的JavaHAWKs和PGOPHER软件进行了相应吸收光谱的计算与模拟，完成了甲烷和甲醛红外吸收光谱的定性与定量检测，测试验证了基于量子级联激光器的气体光谱检测系统的主要性能；基于该系统，进行了甲醛的吸收强度、压力展宽效应、压力频移效应和光谱非线性效应的实验研究，获得了较满意的实验结果。
本论文主要研究工作是：
①论文分析了气体检测技术的研究现状、存在的科学与技术问题，提出了基于中红外量子级联激光器的气体检测系统结构与实现方法，确定了基于量子级联激光器的气体光谱检测系统方案；
②研究了量子级联激光器的气体光谱检测系统的光谱检测理论与方法，分析研究了基于脉冲电流调谐的量子级联激光器的光谱扫描理论与具体实现方法；
③基于气体分子的红外吸收光谱特性，研究了基于量子级联激光器的气体光谱检测的相关理论与方法；采用差分吸收光谱检测技术，解决了气体检测中存在的部分干扰等问题，提高了系统检测灵敏度与检测精度；基于F-P标准具的频率标定技术，解决了中红外波段气体检测系统中时域与频域标定的技术问题；
④提出了基于分布反馈式脉冲量子级联激光器的气体光谱检测系统的总体结构设计方案，搭建了系统实验平台，完成了系统波长范围、分辨率、重复性、稳定性和检测灵敏度等性能的测试分析；
⑤基于本论文搭建的气体检测系统，完成了甲烷和甲醛气体吸收光谱的采集；基于HITRAN的JavaHAWKs和PGOPHER软件对甲烷和甲醛气体吸收光谱进行了模拟，比较模拟光谱与实验光谱的吸收峰数目、位置以及相对吸收强度，完成了吸收光谱的定性分析；完成了甲烷和甲醛气体吸收光谱的采集和处理，基于Beer-Lambert定律的光谱积分面积的计算方法，获得了混合气体中甲烷和甲醛的浓度值，完成了两种气体的定量测试；
⑥基于本实验平台，对甲醛气体吸收光谱的“Rapid Passage”非线性效应、吸收强度、压力展宽和压力频移效应进行了相应参数分析，获得了比较满意的实验结果；
⑦进行论文研究工作的总结，提出了存在的问题与下一步工作思路。
Due to the characteristics of high output power, narrow line-width, roomtemperature operation and so on, Quantum Cascade Lasers (QCLs) have become theresearch focus in the fields of trace gas detection technology and instrumentalintegration system.
This thesis aimed at the issues existed in the gas detection technology andinstrument system researching, key technologies in gas spectroscopy detectiontechnology based on Quantum Cascade Laser were carried out. And also importantlyfocused on the fundamental theory of quantum cascade laser based spectrum scanningmethod by applying a pulse current to the QCL, and also different spectral ranges wereobtained by tuning the QCL operation temperatures; Research work of theory andrealization methods were also carried out by analysing differential optical absorptionspectroscopy and technology based on F-P etalon, then design and set-up the gasdetection experimental system based on quantum cascade laser, and measured thesystem stability and other characteristics; Take methane (CH4) and formaldehyde(H2CO) as the detection gases, firstly simulated their spectrum using HITRAN andPGOPHER, then calculated the relative parameters and results. Testing measurementsresults showed that the quantum cascade laser based gas spectroscopy detection systemhas a relatively high detection sensitivity and resolution. Absorption line intensity,pressure broadening and pressure induced frequency shift parameters of formaldehyde(H2CO) were measured using the system and good results were obtained.
The mainly research works in this thesis were:
①Gas detection technology status, existing matters were compared and analysedin this thesis and them gas spectroscopy detection system and realization method wereproposed, the research scheme was confirmed as pulsed distribute feedback quantumcascade laser based gas detection system and technology.
②Spectrum scanning theory and methods were researched based on distributefeedback quantum cascade laser, and analysis works were carried out by using pulsecurrent tuning method.
③Based on the molecular absorption specificity, fundamental knowledge andmethod were researched based on quantum cascade laser system; by utilizing the gasdetection technology, noise from the environment and other absorptive gases absorption were deducted, and then the sensitivity would be improved. Frequency calibration wasdone by analysing the F-P etalon signal recorded from the experimental system.
④Design scheme was proposed as distribute feedback quantum cascade laserbased gas spectroscopy detection, then each functional modal was tested and set-up,then the whole experimental system was done. Spectral range, resolution, absorbancerepetition, stability and detection limit were measured based on this system;
⑤Take methane (CH4) and formaldehyde (H2CO) as the detection gases, theirspectra were recorded and analysed, then compared with the HITRAN and PGOPHERsimulation, and spectrum parameters were calculated.
⑥Specially, detection work of H2CO was done by measuring its absorption lineintensity, pressure broadening coefficient, pressure induced frequency shift and theRapid Passage effect, and the corresponding results were calculated and analysed.
⑦The thesis conclusion was done, and then bring forward the existent matters andconsiderations for the future work.
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