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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.
Merritt et al. (Thu,) studied this question.