Attosecond Control and Measurement of Chiral Photoionisation Dynamics

Abstract: Many chirality-sensitive light-matter interactions are governed by chiral electron dynamics. Therefore, the development of advanced technologies harnessing chiral phenomena would critically benefit from measuring and controlling chiral electron dynamics on their natural attosecond time scales. Such endeavors have so far been hampered by the lack of characterized circularly polarized attosecond pulses, an obstacle that has recently been overcome (Han et al. Optica 10 (2023) 1044-1052, Han et al. Nature Physics 19 (2023) 230-236). In this article, we introduce chiroptical spectroscopy with attosecond pulses and demonstrate attosecond coherent control over photoelectron circular dichroism (PECD) (Goetz et al. Physical Review Letters 122 (2019) 013204, Goetz et al. arXiv:2104.07522), as well as the measurement of chiral asymmetries in the forward-backward and angle-resolved photoionisation delays of chiral molecules. We show that co-rotating attosecond and near-infrared pulses can nearly double the PECD and even change its sign compared to single-photon ionisation. We demonstrate that chiral photoionisation delays depend on both polar and azimuthal angles of photoemission in the light-propagation frame, requiring three-dimensional momentum resolution. We measure forward-backward chiral-sensitive delays of up to 120 as and polar-angle-resolved photoionisation delays up to 240 as, which include an asymmmetry of $\sim$60 as originating from chirality in the continuum-continuum transitions. Attosecond chiroptical spectroscopy opens the door to quantitatively understanding and controlling the dynamics of chiral molecules on the electronic time scale.