Attochemistry: Is Controlling Electrons the Future of Photochemistry?
Attochemistry: Is Controlling Electrons the Future of Photochemistry?
复制标题
原子化学：控制电子是光化学的未来吗？
DOI：
10.1021/acs.jpclett.1c02016
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
M. Vacher
中科院分区：
文献类型：
--
作者：
Isabella C D Merritt;D. Jacquemin;M. Vacher
用光控制物质一直是一个巨大的挑战，导致光化学领域不断扩大。此外，自从第一代持续时间为阿秒（1 as = 10-18 s）的光脉冲出现以来，人们一直致力于在其固有时间尺度上观察和控制电子。由于持续时间短，阿秒脉冲具有较大的频谱带宽，以相干的方式填充几个电子激发态，即电子波包。由于干扰，这种波包具有新的电子分布，这意味着与传统光化学相比可能具有不同的全新反应性，从而导致了“原子化学”的新概念。这个新兴领域从一开始就需要理论的支持。在这一展望中，我们讨论了原子化学提供的机会、相关的挑战，以及精确建模所需的理论化学当前和未来的最新发展。
Controlling matter with light has always been a great challenge, leading to the ever-expanding field of photochemistry. In addition, since the first generation of light pulses of attosecond (1 as = 10-18 s) duration, a great deal of effort has been devoted to observing and controlling electrons on their intrinsic time scale. Because of their short duration, attosecond pulses have a large spectral bandwidth populating several electronically excited states in a coherent manner, i.e., an electronic wavepacket. Because of interference, such a wavepacket has a new electronic distribution implying a potentially different and totally new reactivity as compared to traditional photochemistry, leading to the novel concept of "attochemistry". This nascent field requires the support of theory right from the start. In this Perspective, we discuss the opportunities offered by attochemistry, the related challenges, and the current and future state-of-the-art developments in theoretical chemistry needed to model it accurately.
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