光腔衰荡光谱法测量大气中的NO3和N2O5

本文应用基于二极管激光器的双路光腔衰荡光谱技术,分别对大气中NO₃和N₂O₅浓度进行监测. 通过使用实验室标准样校正有效吸收腔长比R_L和系统的总损耗系数?,并获得了NO₃有效吸收截面. 该装置在时间分辨率为1 s时,对NO₃的测量灵敏度达到1.1 pptv,N₂O₅被在线转换成NO₃,从而被另一路光腔衰荡光谱装置探测. 利用该装置,对合肥市区冬季夜间大气中的NO₃,N₂O₅浓度进行了实时监测. 通过对比一次大气快速清洁过程中氮氧化物、臭氧、PM_2.5等组分的浓度变化,讨论了大气环境下可能影响NO₃及N₂O₅浓度的因素.     

光外差腔衰荡光谱理论研究

提出了简化的光外差腔衰荡光谱技术，避免了通常腔衰荡光谱对衰荡时间的直接测量，同时消除了腔镜损耗的共模直流信号的测量.理论上其测量灵敏度可以达到量子噪声极限，而且技术实现相对简单，更适合于分子振转光谱研究.此外，还在理论上分析了该光谱技术具有的Gauss线型的一次微分光谱线型的特点，并讨论了一些实验参量对谱线强度和线型的影响，进而给出了最佳实验参量. 关键词： 光外差 腔衰荡光谱     

介质阻挡放电等离子体中OH自由基的光腔衰荡光谱原位诊断

研制了一套等效噪声吸收可达3×10^-9cm^-1的连续波光腔衰荡光谱装置。用该装置对介质阻挡放电等离子体中的OH自由基和水进行了原位定量测量,考察了OH自由基数密度随气压和放电电压以及放电频率的变化情况。实验结果表明,在(2.13~22.0)Χ10³Pa范围内,随着气压增加,OH自由基数密度在气压较低时增加;而在较高气压时由于H₂O的解离吸附作用使得体系中电子密度减小,OH自由基数密度随之减小。随放电电压和放电频率增加介质阻挡放电等离子体中电子密度和电子能量增加而导致OH数密度增加。     

强流离子源光腔衰荡光谱应用研究

强流离子源是托卡马克中性束注入器的核心部件,为了满足未来对高能量离子束中性化效率的要求,负离子源成为中性束注入系统的首选。光腔衰荡光谱(cavity ring-down spectroscopy,CRDS)是一种超高灵敏探测吸收光谱技术。在强流负离子源中,利用氢负离子的光致剥离过程,CRDS可以用来测量氢负离子的绝对积分密度。与激光光致剥离法与光学发射光谱法相比,CRDS具有不受电磁干扰、不依赖等离子体参数、测量精度高等优点。强流离子源负离子密度测量所用CRDS系统由激光器、光学谐振腔、光电探测器和数据采集系统四部分组成。本文根据CRDS测量氢负离子密度的原理,详细推导了氢负离子密度的计算方法,给出了氢负离子密度测算表达式;然后,结合强流离子源实验室应用的具体情况,分析了各部分装置的选择原则与注意事项;最后,介绍了CRDS技术在德国马克斯-普朗克等离子体物理研究所、日本国立聚变科学研究所、意大利Consorzio RFX研究所强流负离子源研究中的应用情况。实验结果表明,源腔气压、源功率等源参数会影响氢负离子密度;铯的注入可以将氢负离子密度从1016 m-3量级提高到1017 m-3量级;同时,日本NIFS的实验结果证明氢负离子密度与引出电流呈线性关系。     

光反馈腔衰荡光谱技术中的数据处理

在光反馈式腔衰荡光谱技术中,光谱数据的处理因一种特殊的光谱纹波现象而变得困难。以6 590.8~6 591.6 cm-1光谱范围内水汽分子的光反馈式腔衰荡光谱为基础,根据光谱纹波效应的特性分析结果,提出了一种简单的数据处理方法。利用该方法确定了6 590.871 cm-1处水汽分子吸收谱线的线宽约为0.100 3 cm-1,这与Hitran数据库提供的线宽结果仅有0.002 cm-1的误差,充分验证了该方法的有效性。     

线形C5H自由基A2Δ电子态的自选轨道分裂和寿命展宽

重新研究了C₅H和C₅D自由基A²Δ-X2Π电子吸收谱带. 利用乙炔/氦混合气脉冲直流放电产生的碳氢等离子体制备气相C5H和C5D自由基,利用光腔衰荡光谱记录碳氢等离子体束的直接吸收光谱. 与之前工作相比,实验光谱的波长校准得到了改进. 通过对实验光谱的分析,首次实验确定了C₅H自由基A²Δ电子态的自旋-轨道分裂常数为-0.7(3) cm^-1. 这为标识A2￠电子态的提供了有力的实验证据. 通过对谱带寿命展宽的分析,A²Δ电子态的寿命估测为1.6±0.3 ps.     

光纤腔衰荡光谱技术及其最新进展

阐述了腔衰荡光谱技术的基本原理及应用;从结构设计的角度考虑,归纳出光纤衰荡腔的三种基本结构,并对光纤腔衰荡光谱技术及其最新进展进行了评述;报道了我们采用脉冲光纤环衰荡光谱技术进行液体检测取得的最新进展;在总结光纤腔衰荡光谱技术优点的基础上,展望了其发展前景。     

基于半导体激光的光腔衰荡光谱装置测定水汽含量

搭建了一套基于光腔衰荡光谱技术的光学湿度计. 通过测量水分子在1.35和1.56 μm波段不同强度的吸收线,可测定水汽的相对含量,测量范围从10^-2到低至10^-12水平. 通过与商用冷镜式露点仪的对比测量,对该装置的定量精度进行了检验. 该系统所具备的高灵敏度使得水汽探测极限可达8 pptv     

光纤腔衰荡光谱技术及其最新进展

阐述了腔衰荡光谱技术的基本原理及应用;从结构设计的角度考虑,归纳出光纤衰荡腔的三种基本结构,并对光纤腔衰荡光谱技术及其最新进展进行了评述;报道了我们采用脉冲光纤环衰荡光谱技术进行液体检测取得的最新进展;在总结光纤腔衰荡光谱技术优点的基础上,展望了其发展前景.     

基于光腔衰荡光谱的宽范围水汽探测

介绍基于光腔衰荡光谱技术的光学湿度测量装置．该装置具有高真空兼容性,衰荡腔由低膨胀的殷钢制成,并利用其自身的自由光谱范围实现光谱的自标定．使用单个在1.39 μm的半导体激光器,实 现了从真空、高纯氦气中痕量水汽,一直到大气湿度的测量,可测量的水汽分压范围极大：0.1 μPa～1 kPa．该光学湿度计可用于作为基本水汽标准,以及测定低温下水(冰)的蒸气压．     

利用激光腔内共振衰减技术研究CH2CHO自由基的近紫外吸收光谱

利用激光腔内共振衰减技术 (CRDS) ,获取了CH2 CHO自由基的近紫外吸收光谱 .在此吸收光谱中 ,有一从 2 8786cm-1起始的振动 电子带 ,和一随能量而增加的宽吸收背景 .此CRDS吸收光谱和以前的低分辨吸收光谱相一致 ;其振动 电子吸收峰位置和在激光诱导荧光光谱及光解产物谱中的峰位置相吻合 .     

Absorption spectra of AsH2 radical in 435-510 nm by cavity ringdown spectroscopy

The absorption spectra of jet-cooled AsH₂ radicals were recorded in the wavelength range of 435-510 nm by cavity ringdown spectroscopy. The AsH₂ radicals were produced by pulsed DC discharge in a molecular beam of a mixture of AsH₃, SF₆, and argon. Seven vibronic bands with fine rotational structures have been identified and assigned as the , , and (n = 1-3) bands of the electronic transition. Based on the previous studies of AsH₂ radical, rotational assignments and rotational term values for each band were obtained, and the molecular parameters including vibrational constants, rotational constants, centrifugal distortion constants, and spin-rotation interaction constants were also determined.     

Ba原子吸收系数的光腔衰荡光谱测量

建立了一套脉冲激光腔衰荡光谱实验装置,并将光腔衰荡光谱技术用于原子束吸收光谱的测量,得到了Ba原子的6s6p^1P1←6s6s^1S0吸收线,进一步得出Ba原子在553．548nm附近的吸收系数,同时对吸收系数与原子炉温度的关系进行了分析,得到了较好的实验结果。     

用耦合簇方法及相关一致基研究PH$lt;sub$gt;2$lt;/sub$gt;($lt;i$gt;X$lt;/i$gt;$lt;sup$gt;2$lt;/sup$gt;$lt;i$gt;B$lt;/i$gt;$lt;sub$gt;1$lt;/sub$gt;)自由基的解析势能函数

利用耦合簇方法和Dunning等提出的系列相关一致基对PH₂自由基的基态结构进行优化, 并使用优选出的cc-pV5Z基组对其进行频率计算. 结果表明,平衡核间距R_P—H=0.14185 nm, 键角α_HPH=91.8624°, 离解能D_e（HP—H）=3.483 eV, 对称伸缩振动频率ν₁（a₁）=2399.9781 cm^-1, 弯曲振动频率ν₂（a₁）=1128.4213 cm^-1,反对称伸缩振动频率ν₃（b₂）=2407.8374 cm^-1. 在此基础上采用多体项展式理论导出了PH₂自由基的解析势能函数, 其等值势能图准确再现了PH₂自由基分子的平衡结构特征和动力学特征. 关键词： 2自由基')" href="#">PH₂自由基 多体项展式理论 解析势能函数     

基于光腔衰荡光谱的便携式呼气异戊二烯分析仪性能评估

呼气异戊二烯是一种内源性代谢产物,其含量与人体血液中的胆固醇水平存在关联.但人体呼气影响因素众多,寻找其与胆固醇水平诊断参数的定量相关性,需要对选取的特定人群进行有效的呼吸气体分析(实时、在线、高灵敏度、高选择性、高精度的大量呼气数据获取).光腔衰荡光谱(CRDS)是一种具有极高灵敏度、稳定性和选择性的光谱技术.采用目...     

High-resolution FTIR spectroscopy of the 3ν2 band of PH3

High-resolution Fourier transform spectrum of phosphine (PH₃) at room temperature has been recorded in the region of the 3ν₂ band (2730-3100 cm⁻¹) at an apodized resolution of 0.005 cm⁻¹. About 200 vibration-rotation transitions have been least squares fitted with an rms of 0.00039 cm⁻¹ after taking into account the ΔK = ±3 interaction.     

C2H2 Overtones Near 12300 cm-1 Revisited with a Very Sensitive Cavity Ring-down Spectrometer

利用单模连续的钛宝石激光器, 构建了一台光腔衰荡光谱仪, 其可探测的最小吸收可达1.8×10^-10/cm. 该光谱仪被用来记录C₂H₂分子在12240～12350 cm^-1的泛频光谱. 与在同一波段测量的已报到的CRDS和激光腔内吸收光谱仪结果比较,本测量同时具有更好的灵敏度和精度. 由此,获得了乙炔分子在12290.12、12311.82和12350.61 cm^-1附近高泛频谱带更准确的振转参数     

Collisional broadening and line intensities in the ν2 and ν4 bands of PH3

Using a tunable diode-laser spectrometer self-broadening coefficients and absolute intensities have been measured for 26 lines of PH₃ at 298 K in the QR branch of the ν₂ band and the PP and RP branches of the ν₄ band. The recorded lines with J values ranging from 2 to 14 and K from 0 to 11 are located in the spectral range 995-1093 cm⁻¹. Self-broadening coefficients have also been measured at 173.4 K for nine of these lines. The collisional widths and line strengths are obtained by fitting each spectral line with different theoretical profiles. The results obtained for the line intensities are in good agreement with recent measurements [J. Mol. Spectrosc. 215 (2002) 178]. The self-broadening coefficients are also calculated on the basis of a simple semiclassical model involving only the electrostatic interactions. A satisfactory agreement is obtained except for high J values or K values equal to J, for which the calculated results are notably underestimated. By comparing broadening coefficients at room and low temperatures, the temperature dependence of these broadenings has been determined both experimentally and theoretically.     

High sensitivity cw-cavity ringdown and Fourier transform absorption spectroscopies of CO2

The absorption spectrum of ¹³CO₂ has been recorded by cw-cavity ringdown spectroscopy with a new set up based on fibered DFB lasers. By using a series of 31 DFB lasers, the spectrum of carbon dioxide could be recorded in the 6130-6750 cm⁻¹ region with a typical sensitivity of 5 × 10⁻¹⁰ cm⁻¹. The spectrum has also been recorded between 4400 and 8500 cm⁻¹ with a Fourier transform spectrometer associated with a multi-pass cell (maximum path length of 105 m). The new observations obtained both by FTS and CRDS represent a significant extension of the available data. For instance, more than 4000 line positions were measured and assigned in the CRDS spectrum while only 232 line positions are listed in the HITRAN database. Altogether, the band by band analysis has led to the determination of the rovibrational parameters of 65, 7, and 24 bands for the ¹³C¹⁶O₂, ¹⁶O¹³C¹⁷O, and ¹⁶O¹³C¹⁸O isotopomers, respectively. As some observed line positions show significant deviations from the predictions of the effective Hamiltonian model, the new observed line positions were gathered with the data available in the literature to refine the set of effective Hamiltonian parameters of the ¹³C¹⁶O₂ isotopic species. The refined set of 96 effective Hamiltonian parameters reproduces more than 14 650 line positions of ¹³C¹⁶O₂ with an RMS=0.002 cm⁻¹. A detailed comparison with the line positions retrieved from Venus spectra and the line list provided by HITRAN is also presented and discussed.