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在Ru(0001)表面上,电子激发解吸与极性NH3共吸附的CF2Cl2过程中的负离子形成。

Negative ion formation in electron-stimulated desorption of CF2Cl2 coadsorbed with polar NH3 on Ru(0001).

作者信息

Solovev S, Kusmierek D O, Madey T E

机构信息

Department of Physics and Astronomy and Laboratory for Surface Modification, Rutgers, The State University of New Jersey, Piscataway, New Jersey 08854-8019, USA.

出版信息

J Chem Phys. 2004 Jan 8;120(2):968-78. doi: 10.1063/1.1630296.

Abstract

Photon-induced dissociation of CF2Cl2 (freon-12) in the stratosphere contributes substantially to atmospheric ozone depletion. We report recent results on dissociation and negative ion formation in electron-stimulated desorption (ESD) of CF2Cl2 on Ru(0001), when CF2Cl2 is coadsorbed with a polar molecule (NH3), for electron energies ranging from 50 to 300 eV. Two different time-of-flight methods are used in this investigation: (a) an ESD ion angular distribution detector with wide collection angle and (b) a quadrupole mass spectrometer with narrow collection angle and high mass resolution. Many negative ESD fragments are seen (F-, Cl-, FCl-, CF-, F2-, and Cl2-), whose intensities depend on the surface preparation. Using both detectors we observe a giant enhancement of Cl- and F- yields for ESD of CF2Cl2 coadsorbed with approximately 1 ML of NH3; this enhancement (>10(3) for Cl-) is specific to certain ions, and is attributed to an increased probability of dissociative electron attachment due to "trapped" low-energy secondary electrons, i.e., precursor states of the solvated electron in NH3. In further studies, the influence of polar NH3 spacer layers (1-10 ML) on ESD of top-layer CF2Cl2 is determined, and compared with thick films of condensed CF2Cl2. The magnitudes and energy dependences of the Cl- yields are different in these cases, due to several contributing factors.

摘要

平流层中光子诱导的二氟二氯甲烷(氟利昂 - 12)解离对大气臭氧层损耗有重大贡献。我们报告了近期关于在Ru(0001)表面上,当二氟二氯甲烷与极性分子(NH₃)共吸附时,电子能量在50至300 eV范围内的电子激发脱附(ESD)中解离和负离子形成的研究结果。本研究中使用了两种不同的飞行时间方法:(a)具有宽收集角的ESD离子角分布探测器,以及(b)具有窄收集角和高质量分辨率的四极质谱仪。观察到许多负ESD碎片(F⁻、Cl⁻、FCl⁻、CF⁻、F₂⁻和Cl₂⁻),其强度取决于表面处理。使用这两种探测器,我们观察到与约1 ML的NH₃共吸附的二氟二氯甲烷的ESD中Cl⁻和F⁻产率大幅提高;这种提高(Cl⁻的提高>10³)特定于某些离子,并且归因于由于“捕获”的低能二次电子,即NH₃中溶剂化电子的前驱态,导致解离电子附着概率增加。在进一步的研究中,确定了极性NH₃间隔层(1 - 10 ML)对顶层二氟二氯甲烷ESD的影响,并与凝聚态二氟二氯甲烷的厚膜进行了比较。由于几个促成因素,在这些情况下Cl⁻产率的大小和能量依赖性是不同的。

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