Ultrafast dynamics of low-energy electron attachment via a non-valence correlation-bound state

Joshua P Rogers; Cate S Anstöter; Jan R R Verlet

doi:10.1038/nchem.2912

Ultrafast dynamics of low-energy electron attachment via a non-valence correlation-bound state

Joshua P Rogers, Cate S Anstöter, Jan R R Verlet

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

The primary electron-attachment process in electron-driven chemistry represents one of the most fundamental chemical transformations with wide-ranging importance in science and technology. However, the mechanistic detail of the seemingly simple reaction of an electron and a neutral molecule to form an anion remains poorly understood, particularly at very low electron energies. Here, time-resolved photoelectron imaging was used to probe the electron-attachment process to a non-polar molecule using time-resolved methods. An initially populated diffuse non-valence state of the anion that is bound by correlation forces evolves coherently in ∼30 fs into a valence state of the anion. The extreme efficiency with which the correlation-bound state serves as a doorway state for low-energy electron attachment explains a number of electron-driven processes, such as anion formation in the interstellar medium and electron attachment to fullerenes.

Original language	English
Pages (from-to)	341-346
Number of pages	6
Journal	Nature Chemistry
Volume	10
Issue number	3
Early online date	8 Jan 2018
DOIs	https://doi.org/10.1038/nchem.2912
Publication status	Published - 1 Mar 2018

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10.1038/nchem.2912

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title = "Ultrafast dynamics of low-energy electron attachment via a non-valence correlation-bound state",

abstract = "The primary electron-attachment process in electron-driven chemistry represents one of the most fundamental chemical transformations with wide-ranging importance in science and technology. However, the mechanistic detail of the seemingly simple reaction of an electron and a neutral molecule to form an anion remains poorly understood, particularly at very low electron energies. Here, time-resolved photoelectron imaging was used to probe the electron-attachment process to a non-polar molecule using time-resolved methods. An initially populated diffuse non-valence state of the anion that is bound by correlation forces evolves coherently in ∼30 fs into a valence state of the anion. The extreme efficiency with which the correlation-bound state serves as a doorway state for low-energy electron attachment explains a number of electron-driven processes, such as anion formation in the interstellar medium and electron attachment to fullerenes.",

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