Aboslute clustering effects on electron attachment

电子附着在辐射化学中起着重要的作用，例如DNA损伤和臭氧消耗。因此，对孤立分子和凝聚态环境中电子附着过程的详细理解和量化对于模拟纳米尺度上的辐射效应至关重要。我的EPSRC CAF探测了选定生物分子簇中的电子附着动力学和反应途径，建立在最近的进展，如观察电子驱动的质子转移在沃森克里克对[Bowen等人]。化学物理学报11(2010):880]。然而，对于聚类如何改变电子附着诱导过程的绝对概率，人们知之甚少。而我的合作者Fabrikant和Gorfinkiel的理论计算[J]。化学。Phys. 136(2012) 184301]已经提供了在特定的簇构型中有很强的增强的证据，但电子附着在簇上的绝对实验数据是极其罕见的。本项目的核心是开发一种原创技术，以产生具有已知目标密度的中性质量选择光束，用于电子附着实验。该方法涉及通过电子光脱离特定弱束缚阴离子状态来中和大量选择的簇阴离子，其稳定性和解离变化最小。该项目将在量化局部化学环境对电子附着诱导过程的影响方面提供突破。

Electron attachment plays an important role in radiation chemistry, for example in DNA damage and ozone depletion. Detailed understanding and quantification of electron attachment processes in isolated molecules and condensed environments is therefore essential to model radiation effects on the nanoscale. My EPSRC CAF probes electron attachment dynamics and reactive pathways in selected biomolecular clusters, building on recent advances such as the observation of electron driven proton transfer in Watson Crick pairs [Bowen et al. ChemPhysChem 11 (2010) 880]. However, relatively little is known about how clustering modifies the absolute probabilities for electron attachment induced processes. While theoretical calculations by my collaborators Fabrikant and Gorfinkiel [J. Chem. Phys. 136 (2012) 184301] have provided evidence for strong enhancements in specific cluster configurations, absolute experimental data for electron attachment to clusters are extremely rare. This project is centered on developing an original technique to produce neutral mass-selected beams with known target density for electron attachment experiments. The method involves neutralization of mass-selected cluster anions by electron photo-detachment from specific weakly-bound anionic states, with minimal change in stability and hence dissociation. The project will provide a breakthrough in quantifying the effects of the local chemical environment on electron attachment induced processes.