Solvated dielectrons from optical excitation: An effective source of low-energy electrons

• 成果类型: Article
• 署名作者: Hartweg, Sebastian; Barnes, Jonathan; Yoder, Bruce L.; Garcia, Gustavo A.; Nahon, Laurent; Miliordos, Evangelos; Signorell, Ruth
• 署名单位: SOLEIL Synchrotron; University of Freiburg; Swiss Federal Institutes of Technology Domain; ETH Zurich; Auburn University System; Auburn University
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11692
• DOI: 10.1126/science.adh0184
• 发表日期: 2023-06-16
• 页码: 1161-1165
• 关键词: transfer-mediated decay; DYNAMICS; water; simulation; reduction; metals

摘要

Low-energy electrons dissolved in liquid ammonia or aqueous media are powerful reducing agents that promote challenging reduction reactions but can also cause radiation damage to biological tissue. Knowledge of the underlying mechanistic processes remains incomplete, particularly with respect to the details and energetics of the electron transfer steps. In this work, we show how ultraviolet (UV) photoexcitation of metal-ammonia clusters could be used to generate tunable low-energy electrons in situ. Specifically, we identified UV light-induced generation of spin-paired solvated dielectrons and their subsequent relaxation by an unconventional electron transfer-mediated decay as an efficient, low-energy electron source. The process is robust and straightforward to induce with the prospect of improving our understanding of radiation damage and fostering mechanistic studies of solvated electron reduction reactions.