Metz Ricardo B, Nicolas Christophe, Ahmed Musahid, Leone Stephen R
Department of Chemistry, University of Massachusetts Amherst, Massachusetts 01003, USA.
J Chem Phys. 2005 Sep 15;123(11):114313. doi: 10.1063/1.2032947.
Photoionization efficiency curves were measured for gas-phase FeO and CuO using tunable vacuum-ultraviolet radiation at the Advanced Light Source. The molecules are prepared using laser ablation of a metal-oxide powder in a novel high-repetition-rate source and are thermally moderated in a supersonic expansion. These measurements provide the first directly measured ionization energy for CuO, IE(CuO)=9.41 +/- 0.01 eV. The direct measurement also gives a greatly improved ionization energy for FeO, IE(FeO) = 8.56 +/- 0.01 eV. The ionization energy connects the dissociation energies of the neutral and cation, leading to a refined bond strength for the FeO cation: D0(Fe(+)-O)=3.52 +/- 0.02 eV. A dramatic increase in the photoionization cross section at energies of 0.36 eV above the threshold ionization energy is assigned to autoionization and direct ionization involving one or more low-lying quartet states of FeO+. The interaction between the sextet ground state and low-lying quartet states of FeO+ is key to understanding the oxidation of hydrogen and methane by FeO+, and these experiments provide the first experimental observation of the low-lying quartet states of FeO+.
利用先进光源的可调谐真空紫外辐射,测量了气相FeO和CuO的光电离效率曲线。这些分子是在一种新型高重复率源中通过激光烧蚀金属氧化物粉末制备的,并在超声速膨胀中进行热缓和。这些测量首次直接测得CuO的电离能,IE(CuO)=9.41±0.01 eV。直接测量还大大改进了FeO的电离能,IE(FeO)=8.56±0.01 eV。电离能连接中性分子和阳离子的离解能,从而得到FeO阳离子更精确的键强度:D0(Fe(+)-O)=3.52±0.02 eV。在高于阈值电离能0.36 eV的能量处,光电离截面急剧增加,这归因于自电离和涉及FeO+一个或多个低激发四重态的直接电离。FeO+的六重基态与低激发四重态之间的相互作用是理解FeO+氧化氢和甲烷的关键,这些实验首次对FeO+的低激发四重态进行了实验观测。