Ultrafast Dynamics at the Na/D2O/Cu(111) Interface: Electron Solvation in Ice Layers and Na+-Mediated Surface Solvation
Ultrafast Dynamics at the Na/D2O/Cu(111) Interface: Electron Solvation in Ice Layers and Na+-Mediated Surface Solvation
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Na/D2O/Cu(111) 界面的超快动力学：冰层中的电子溶剂化和 Na 介导的表面溶剂化
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发表时间：
2011
期刊：
影响因子：
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通讯作者：
M. Wolf
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作者：
M. Meyer;M. Bertin;U. Bovensiepen;D. Wegkamp;M. Krenz;M. Wolf
利用飞秒时间分辨双光子光电子能谱研究了在冰/真空界面附近结合的钠离子对非晶D2O冰层中电子溶剂化动力学的影响。钠在多层非晶冰上的亚单层吸附导致Na+离子的形成，与纯非晶冰相比，观察到的超快动力学发生了显著变化。我们发现了一种Na+诱导的多余电子，与纯D2O冰中的多余电子相比，它具有更长的寿命，并且通过两个衰变时间τ2 = 880 fs和τ3 = 9.6 ps近似地描述了Na诱导的衰变贡献。此外，观察到激发电子的能量稳定速度更快，速率为Σ = 0.73 eV/ps。这些电子的占比非线性地依赖于钠的覆盖率。我们将na诱导的贡献归因于位于冰/真空界面的瞬态电子/离子/水配合物。这种解释是……
We have studied the influence of sodium ions bound near the ice/vacuum interface on the electron solvation dynamics in amorphous D2O ice layers by means of femtosecond time-resolved two-photon photoelectron spectroscopy. Adsorption of submonolayer coverages of sodium on top of multilayers of amorphous ice leads to the formation of Na+ ions and to pronounced changes in the observed ultrafast dynamics compared to pure amorphous ice. We identify a Na+-induced species of excess electrons which exhibits a much longer lifetime compared to excess electrons in pure D2O ice and approximate the decay of the Na-induced contribution by two decay times τ2 = 880 fs and τ3 = 9.6 ps. In addition, a faster energetic stabilization of the excited electrons with a rate of Σ = 0.73 eV/ps is observed. The population of these electrons depends nonlinearly on the sodium coverage. We attribute the Na-induced contribution to a transient electron/ion/water complex which is located at the ice/vacuum interface. This interpretation is...