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用于气相动力学实验的光纤耦合激光诱导解吸源的设计与表征

Design and characterization of an optical-fiber-coupled laser-induced desorption source for gas-phase dynamics experiments.

作者信息

Milešević Dennis, Popat Divya, Gellersen Paul, Liu Zhihao, Stimson Joseph, Robertson Patrick, Green Andrew, Vallance Claire

机构信息

Department of Chemistry, University of Oxford, Chemistry Research Laboratory, 12 Mansfield Rd., Oxford OX1 3TA, United Kingdom.

出版信息

Rev Sci Instrum. 2023 Nov 1;94(11). doi: 10.1063/5.0170080.

Abstract

Preparation of neutral non-volatile molecules intact in the gas phase for mass spectrometry or chemical dynamics experiments remains a challenge for many classes of molecules. Here, we report the design and characterization of a fiber-coupled laser-based thermal desorption source capable of preparing intact neutral molecules at high molecular densities in the gas phase for use in velocity-map imaging experiments. Within this source, the sample is deposited onto a thin tantalum foil. Irradiation of the foil from the reverse side by a focused laser beam leads to highly localized heating of the sample, resulting in desorption of a plume of molecules into the gas phase. The fiber-coupled design simplifies the alignment of the desorption laser beam, and the ability to rotate the foil relative to the fixed laser beam allows the sample to be continually refreshed under vacuum. We use 118 nm photoionization of three test molecules-uracil, adenine, and phenylalanine-to characterize the source and to demonstrate various aspects of its performance. These include the dependence of the velocity-map imaging performance on the size of the interaction region and the dependence of the laser-induced desorption source emission on desorption laser power and heating time. Signal levels recorded in these measurements are comparable to those we typically obtain in similar experiments using a pulsed supersonic molecular beam, and we, therefore, believe that the source has considerable potential for use in a wide range of chemical dynamics and other experiments.

摘要

对于许多种类的分子而言,在气相中制备完整的中性非挥发性分子用于质谱分析或化学动力学实验仍然是一项挑战。在此,我们报告了一种基于光纤耦合激光的热解吸源的设计与表征,该热解吸源能够在气相中以高分子密度制备完整的中性分子,用于速度成像实验。在这个源中,样品被沉积在一张薄钽箔上。通过聚焦激光束从箔片的背面进行照射会导致样品高度局部加热,从而使一团分子解吸进入气相。光纤耦合设计简化了解吸激光束的对准,并且相对于固定激光束旋转箔片的能力使得样品能够在真空下持续更新。我们使用三种测试分子——尿嘧啶、腺嘌呤和苯丙氨酸——的118纳米光电离来表征该源,并展示其性能的各个方面。这些方面包括速度成像性能对相互作用区域大小的依赖性以及激光诱导解吸源发射对解吸激光功率和加热时间的依赖性。在这些测量中记录的信号水平与我们通常在使用脉冲超声分子束的类似实验中获得的信号水平相当,因此,我们认为该源在广泛的化学动力学和其他实验中具有相当大的应用潜力。

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