Institut für Physikalische Chemie, Georg-August-Universität Göttingen, Tammannstraße 6, 37077 Göttingen, Germany.
J Chem Phys. 2017 Jul 7;147(1):013939. doi: 10.1063/1.4983307.
We describe a new instrument that uses ion imaging to study molecular beam-surface scattering and surface desorption kinetics, allowing independent determination of both residence times on the surface and scattering velocities of desorbing molecules. This instrument thus provides the capability to derive true kinetic traces, i.e., product flux versus residence time, and allows dramatically accelerated data acquisition compared to previous molecular beam kinetics methods. The experiment exploits non-resonant multiphoton ionization in the near-IR using a powerful 150-fs laser pulse, making detection more general than previous experiments using resonance enhanced multiphoton ionization. We demonstrate the capabilities of the new instrument by examining the desorption kinetics of CO on Pd(111) and Pt(111) and obtain both pre-exponential factors and activation energies of desorption. We also show that the new approach is compatible with velocity map imaging.
我们描述了一种新的仪器,该仪器使用离子成像来研究分子束-表面散射和表面解吸动力学,从而能够独立确定表面停留时间和解吸分子的散射速度。因此,该仪器提供了获得真实动力学轨迹的能力,即产物通量与停留时间的关系,并且与以前的分子束动力学方法相比,能够显著加速数据采集。该实验利用近红外区的非共振多光子电离,使用强大的 150-fs 激光脉冲,使检测比以前使用共振增强多光子电离的实验更通用。我们通过研究 CO 在 Pd(111)和 Pt(111)上的解吸动力学来演示新仪器的功能,并获得解吸的前指数因子和激活能。我们还表明,新方法与速度映射成像兼容。