Merritt Isabella C D, Jacquemin Denis, Vacher Morgane
Université de Nantes, CNRS, CEISAM, UMR 6230, F-44000 Nantes, France.
J Phys Chem Lett. 2021 Sep 2;12(34):8404-8415. doi: 10.1021/acs.jpclett.1c02016. Epub 2021 Aug 26.
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 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.
用光控制物质一直是一项巨大的挑战,这也推动了光化学领域的不断拓展。此外,自第一代阿秒(1阿秒 = 10⁻¹⁸秒)持续时间的光脉冲出现以来,人们投入了大量精力来在电子的固有时间尺度上观测和控制电子。由于阿秒脉冲持续时间短,具有很大的光谱带宽,能够以相干方式填充多个电子激发态,即形成一个电子波包。由于干涉作用,这样的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且全新的反应活性,从而引出了“阿秒化学”这一全新概念。这个新兴领域从一开始就需要理论的支持。在这篇展望文章中,我们将探讨阿秒化学所带来的机遇、相关挑战,以及为准确模拟它所需的理论化学领域当前和未来的前沿发展。