Theory of electronic friction of adsorbates at metal surfaces: Methods and applications

金属表面吸附物的电子摩擦理论：方法与应用

• 批准号: 170440243
• 负责人: Professor Dr. Peter Saalfrank
• 金额: --
• 依托单位: Lehrstuhl für Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2010
• 资助国家: 德国
• 起止时间: 2009-12-31 至 2020-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/170440243?language=en
• 关键词: Theory; electronic; friction; adsorbates; metal

Electronic friction is a theoretical concept to treat non-adiabatic dynamics of atoms and molecules at metal surfaces in an approximate way. Non-adiabatic effects we have here in mind are due to the violation of the Born-Oppenheimer approximation, arising from the coupling of adsorbate modes to a continuum of metal excitations. Physical phenomena triggered by non-adiabaticity, which have already been considered in this project, are, among others: (i) The vibrational relaxation of vibrationally excited adsorbates and associated with it, the line broadening in vibrational spectroscopy. (ii) Energy transfer during and influences on, reactive and non-reactive molecule-surface scattering. (iii) Substrate-mediated femtochemistry at surfaces following excitation with ultrashort laser pulses. These phenomena are of general importance for spectroscopy, photochemistry, and energy transfer near metal surfaces.In this project the "Molecular Dynamics with Electronic Friction" (MDEF) method, in which classical equations of motion subject to frictional and fluctuating forces shall be further developed, and applied to selected examples of gas-surface dynamics. Planned methodological developments aim at including non-isotropic corrections and effects of surface atom motion for atomic, electronic friction coefficients, as well as the treatment of two time-dependent temperature baths (one for electrons and one for phonons) in "on the fly" AIMDEF ("Ab Initio MDEF") simulations.Applications concern non-trivial examples which are relevant for current experiments: (i) A systematic study of the vibrational relaxation of different atoms at surfaces and the role played by electronic and phononic relaxation channels. We also wish to study the dependence of these phenomena on the adsorption site, the type of metal, and surface structure. (ii) The vibrational relaxation and vibrational line broadening of frustrated translational modes of hydrocarbons adsorbed on "naked" and hydrogen-passivated, ruthenium surfaces shall be studied. (iii) The proposed phenomenon of "dynamic promotion" of a surface photoreaction shall be investigated for the example of laser-induced associative desorption of hydrogen and deuterium from a Ru(0001) surface. (iv) Finally, we aim at a deeper understanding of dynamical details during laser-driven femtochemistry of CO on Ru(0001), and their possible manipulation by variation of laser pulse parameters.

电子摩擦是以近似方式处理金属表面原子和分子非绝热动力学的理论概念。我们在这里想到的非绝热效应是由于吸附质模式与金属激发连续体的耦合而违反了玻恩-奥本海默近似。本项目已考虑的由非绝热性引发的物理现象包括：（i）振动激发吸附物的振动弛豫以及与之相关的振动光谱中的谱线展宽。 (ii) 反应性和非反应性分子表面散射期间的能量转移及其影响。 (iii)超短激光脉冲激发后表面的基底介导的飞秒化学。这些现象对于光谱学、光化学和金属表面附近的能量转移具有普遍重要性。在该项目中，“电子摩擦分子动力学”（MDEF）方法将进一步发展受摩擦力和脉动力影响的经典运动方程，并应用于气体表面动力学的选定示例。计划的方法开发旨在包括非各向同性校正和表面原子运动对原子、电子摩擦系数的影响，以及“动态”中两个随时间变化的温度浴（一个用于电子，一个用于声子）的处理AIMDEF（“Ab Initio MDEF”）模拟。应用涉及与当前实验相关的重要示例：（i）系统研究表面不同原子的振动弛豫以及电子和电子所起的作用声子弛豫通道。我们还希望研究这些现象对吸附位点、金属类型和表面结构的依赖性。 (ii) 应研究吸附在“裸露”和氢钝化钌表面上的碳氢化合物受挫平移模式的振动弛豫和振动谱线展宽。 (iii) 所提出的表面光反应“动态促进”现象应以激光诱导氢和氘从 Ru(0001) 表面缔合解吸为例进行研究。 (iv) 最后，我们的目标是更深入地了解 Ru(0001) 上 CO 的激光驱动飞秒化学过程中的动力学细节，以及通过改变激光脉冲参数对其进行可能的操纵。

项目成果

Femtosecond laser induced desorption of H2, D2, and HD from Ru(0001): Dynamical promotion and suppression studied with ab initio molecular dynamics with electronic friction

• DOI: 10.1103/physrevb.95.125439
• 发表时间: 2017-03-29
• 期刊: PHYSICAL REVIEW B
• 影响因子: 3.7
• 作者: Juaristi, J. I.;Alducin, M.;Saalfrank, P.
• 通讯作者: Saalfrank, P.

Femtosecond-laser induced dynamics of CO on Ru(0001): Deep insights from a hot-electron friction model including surface motion

Ru(0001) 上 CO 的飞秒激光诱导动力学：包括表面运动在内的热电子摩擦模型的深刻见解

• DOI: 10.1103/physrevb.94.165447
• 发表时间: 2016
• 期刊: Physical Review B
• 影响因子: 3.7
• 作者: R. Scholz;G. Floß;P. Saalfrank;G. Füchsel;I. Loncaric;J.I. Juaristi
• 通讯作者: J.I. Juaristi

Vibrational response and motion of carbon monoxide on Cu(100) driven by femtosecond laser pulses: Molecular dynamics with electronic friction

• DOI: 10.1103/physrevb.100.245431
• 发表时间: 2019-12-26
• 期刊: PHYSICAL REVIEW B
• 影响因子: 3.7
• 作者: Scholz, Robert;Lindner, Steven;Saalfrank, Peter
• 通讯作者: Saalfrank, Peter

Quantum dynamical simulations of the femtosecond-laser-induced ultrafast desorption of H2 and D2 from Ru(0001).

飞秒激光诱导 Ru(0001) 中 H2 和 D2 超快解吸的量子动力学模拟

• DOI: 10.1002/cphc.201200940
• 发表时间: 2013
• 期刊: Chemphyschem : a European journal of chemical physics and physical chemistry
• 作者: G. Füchsel;J.C. Tremblay;T. Klamroth;P. Saalfrank
• 通讯作者: P. Saalfrank

Strong Anisotropic Interaction Controls Unusual Sticking and Scattering of CO at Ru(0001).

强各向异性相互作用控制 CO 在 Ru(0001) 上异常的粘附和散射

• DOI: 10.1103/physrevlett.119.146101
• 发表时间: 2017
• 期刊: Physical review letters
• 影响因子: 8.6
• 作者: I. Loncaric;J.I. Juaristi;G. Füchsel;P. Saalfrank
• 通讯作者: P. Saalfrank