New Aspects of Buffer Gas Effects in Resonant Spectrophones

R. Johnson, L. J. Thomas, R. Gerlach, N. Amer
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Abstract

In studies of gas phase photoacoustic spectroscopy, the gas whose spectrum is being investigated is generally one of several present in the sample, and often only in trace amounts. The response of the spectrophone is determined by the characteristics of the sample gas as a whole, and depends on the various thermal and molecular relaxational properties of the gases present. In particular, for an acoustically resonant spectrophone, important characteristics will include the sound velocity, heat capacity, thermal conductivity, viscosity, and the energies and relaxation times of the molecular vibrations. The sound velocity determines the resonant frequencies of the cavity, while the other parameters govern the loss mechanisms that determine the quality factors of the resonances, and also cause small shifts in the resonant frequencies. In an earlier study,1 the resonant frequencies and quality factors of acoustical resonances were determined for various buffer gases at atmospheric pressure, and the results were compared to theoretical predictions2 based on classical surface viscous and thermal losses. Significant discrepancies were observed for all non-noble gases.3 It is the goal of this work to investigate the pressure dependent behavior of the spectrophone, and to incorporate molecular relaxation effects into the theoretical interpretation of that behavior. We have made a number of extensions and improvements in experimental and analytical technique. The spectrophone used was a stainless steel cylinder polished to a 1/3 micron surface finish to guarantee well defined boundary layers whose losses could be calculated accurately from theory. The spectrophone and vacuum system were bakeable to reduce impurity effects due to outgassing. Whereas in the earlier experiment a large concentration of the optically absorbing component (9000 ppm of CH4) was used, we kept the absorber concentration small (50 ppm of C2H4) so as not to disturb the properties of the buffer gas. Use of an electro-optic modulator system allowed access to modes at much higher frequencies, thus enabling the study of lighter gases. We have measured the resonant frequency and quality factor as a function of pressure from atmopsheric pressure down to 10 torr or lower for each buffer gas. Data analysis consisted largely of nonlinear least squares curve fitting of the resonant response curves, which gave more accurate determinations of the resonant frequency and Q than the half power point method used in the previous experiment.
共振声谱仪中缓冲气体效应的新进展
在气相光声光谱的研究中,所研究的光谱气体通常是样品中存在的几种气体中的一种,而且往往只有微量。谱听器的响应是由样品气体作为一个整体的特性决定的,并且取决于存在的气体的各种热特性和分子弛豫特性。特别是,对于声共振光谱仪,重要的特性将包括声速、热容、导热性、粘度以及分子振动的能量和弛豫时间。声速决定了谐振腔的谐振频率,而其他参数决定了谐振腔的损耗机制,这些损耗机制决定了谐振腔的质量因素,也会引起谐振腔频率的微小变化。在早期的研究中,1确定了不同缓冲气体在常压下的共振频率和声共振的质量因子,并将结果与基于经典表面粘性和热损失的理论预测结果2进行了比较。在所有非惰性气体中都观察到显著的差异这项工作的目标是研究声谱仪的压力依赖行为,并将分子弛豫效应纳入该行为的理论解释。我们在实验和分析技术方面作了许多扩展和改进。所使用的声谱仪是一个不锈钢圆柱体,表面抛光到1/3微米,以保证边界层的定义良好,其损失可以从理论上准确计算出来。声谱仪和真空系统可烘烤,以减少放气对杂质的影响。在之前的实验中,我们使用了大浓度的光学吸收成分(9000 ppm的CH4),为了不影响缓冲气体的性质,我们将吸收剂浓度保持在小浓度(50 ppm的C2H4)。电光调制器系统的使用允许进入更高频率的模式,从而能够研究较轻的气体。我们测量了谐振频率和质量因子作为压力的函数,从大气压到10托或更低的每个缓冲气体。数据分析主要由谐振响应曲线的非线性最小二乘曲线拟合组成,与之前实验中使用的半功率点法相比,该方法可以更准确地确定谐振频率和Q。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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