Observation of intermolecular Coulombic decay in liquid water

Outer Valence Intermolecular Coulombic Decay in Hydrogen-Bonded Complexes Induced by Resonant Two-Photon Excitation by 4.4 eV Photons

Photoexcitation of van der Waals complexes can lead to several decay pathways depending on the nature of the potential energy surfaces. Upon excitation of a chromophore in a complex, ionization of its weakly bound neighbour via energy transfer happens via a unique relaxation process known as intermolecular Coulombic decay (ICD); a phenomenon of renewed focus owing to its relevance in biological systems. Herein, we report an experimental evidence of outer-valence ICD induced by multiphoton excitation by near UV radiation of 4.4 eV photons, hitherto unknown in molecular systems. In the binary co…

Highly efficient double ionization of mixed alkali dimers by intermolecular Coulombic decay

As opposed to purely molecular systems where electron dynamics proceed only through intramolecular processes, weakly bound complexes such as He droplets offer an environment where local excitations can interact with neighbouring embedded molecules leading to new intermolecular relaxation mechanisms. Here, we report on a new decay mechanism leading to the double ionization of alkali dimers attached to He droplets by intermolecular energy transfer. From the electron spectra, the process is similar to the well-known shake-off mechanism observed in double Auger decay and single-photon double ioniz…

一种选择性驱动光致损伤的分子间机制

A new intermolecular mechanism to selectively drive photoinduced damages

低能量电子（LEE）被认为是有效的，在DNA链断裂。最近的实验表明，LEE的一个重要的直接来源是分子间库仑衰变（ICD）过程。在这里，我们提出了一个新的级联机制启动的核心激发和ICD终止，并证明其性质。显式计算表明，可以通过选择初始原子激发来控制发射的ICD电子的能量。级联的性质可能在电子光谱学和辐射损伤领域有有趣的应用。通过从嵌入癌细胞核中的高Z元素共振X射线吸收来启动这种级联，ICD将在吸收部位递送遗传毒性颗粒\textit{locally}，以这种方式增加诱导损伤的可控性。

The water-carbon monoxide dimer: new infrared spectra, ab initio rovibrational energy level calculations, and an interesting intermolecular mode

Rovibrational energy level calculations using a high-level intermolecular potential surface are reported for H2O-CO and D2O-CO. They predict the ground K = 1 levels to lie about 20 (12) cm-1 above K = 0 for H2O-CO (D2O-CO) in good agreement with past experiment. But the first excited K = 1 levels are predicted to lie about 3 cm-1 below their K = 0 counterparts in both cases. Intensity calculations also indicate that mid-infrared transitions from the K = 0 ground state to this seemingly anomalous excited K = 1 state should be observable. These predictions are strikingly verified by new spectros…

微溶剂化有机分子电子芯态空穴衰变中分子间过程的保护与损伤相互作用

Interplay of protection and damage through intermolecular processes in the decay of electronic core holes in microsolvated organic molecules

本研究通过PEPIPICO技术和理论计算发现，当芯态空穴位于水分子时，微溶剂化嘧啶分子的环境保护效应部分逆转，揭示了X射线光化学中保护与损伤的复杂相互作用。

从单分子数据推导水中的极化力

Polarization forces in water deduced from single molecule data

利用分布极化率建立的最小原子多极模型，确定了水中分子间的极化相互作用。水-水相互作用的氢键和其他性质仅由三个多极$μ_H$、$μ_O$和$θ_O$以及两个极化率$α_O$和$α_H$精确再现，它们表征单个水分子并从单分子数据推导。