Real-space subfemtosecond imaging of quantum electronic coherences in molecules

Abstract Tracking electron motion in molecules is the key to understanding and controlling chemical transformations. Contemporary techniques attosecond science are able generate trace consequences of this real time, but not space. Scanning tunnelling microscopy, on other hand, can locally probe valence density molecules, cannot alone provide dynamical information at ultrafast timescale. Here we show that, by combining scanning microscopy technologies, quantum electronic coherences induced <6-fs-long carrier-envelope-phase-stable near-infrared laser pulses be directly visualized ångström-scale spatial subfemtosecond temporal resolutions. We demonstrate concurrent real-space -time imaging involving orbitals perylenetetracarboxylic dianhydride full control over population involved orbitals. This approach opens way unambiguous observation manipulation dynamics complex molecular systems.