Probing the Electronic Structure of Bulk Water at the Molecular Length Scale with Angle-Resolved Photoelectron Spectroscopy.,The Journal of Physical Chemistry Letters

当前位置： X-MOL 学术 › J. Phys. Chem. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Probing the Electronic Structure of Bulk Water at the Molecular Length Scale with Angle-Resolved Photoelectron Spectroscopy.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-06-01 , DOI: 10.1021/acs.jpclett.0c00968
Samer Gozem ₁ , Robert Seidel _{2,

3} , Uwe Hergenhahn _{4,

5} , Evgeny Lugovoy _{4,

6} , Bernd Abel _{4,

6} , Bernd Winter ₅ , Anna I Krylov _{7,

8} , Stephen E Bradforth ₇

Affiliation

We report a combined experimental and theoretical study of bulk water photoionization. Angular distributions of photoelectrons produced by ionizing the valence bands of neat water using X-ray radiation (250–750 eV) show a limited (∼20%) decrease in the β anisotropy parameter compared to the gas phase, indicating that the electronic structure of the individual water molecules can be probed. We show that, in the high-energy regime, photoionization of bulk can be described using an incoherent superposition of individual molecules, in contrast to a low-energy regime where photoionization probes delocalized entangled states of molecular aggregates. The two regimes—low versus high energy—are limiting cases where the de Broglie wavelength of the photoelectron is larger or smaller than the intermolecular distance between water molecules, respectively. The comparison of measured and computed anisotropies reveals that the reduction in β at high kinetic energies is mostly due to scattering rather than rehybridization due to solvation.

中文翻译：

用角分辨光电子能谱在分子长度尺度上探测散装水的电子结构。

我们报告了结合的实验和理论研究大量水的光电离。通过使用X射线辐射（250–750 eV）电离纯净水的价带所产生的光电子的角分布显示，与气相相比，β各向异性参数的减小幅度很小（约20％），表明该相的电子结构可以探测各个水分子。我们表明，在高能方案中，可以使用单个分子的非相干叠加来描述本体的光电离，而在低能方案中，光电离探针会散布分子聚集体的纠缠态。低能量与高能量这两种机制是限制性的情况，其中光电子的德布罗意波长分别大于或小于水分子之间的分子间距离。

更新日期：2020-07-02

点击分享查看原文

点击收藏

公开下载

阅读更多本刊最新论文本刊介绍/投稿指南11