Attosecond control and measurement of chiral photoionization dynamics

Journal Article · Wed Aug 27 00:00:00 EDT 2025 · Nature (London)

DOI:https://doi.org/10.1038/s41586-025-09455-4· OSTI ID:3003065

Han, Meng ^[1]; Ji, Jia-Bao ^[2]; Blech, Alexander ^[3]; Goetz, R. Esteban ^[4]; Allison, Corbin ^[5]; Greenman, Loren ^[5]; Koch, Christiane P. ^[3]; Wörner, Hans Jakob ^[2]

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1. ETH Zürich (Switzerland); Kansas State University, Manhattan, KS (United States)
2. ETH Zürich (Switzerland)
3. Freie Universität Berlin (Germany)
4. University of Connecticut, Storrs, CT (United States)
5. Kansas State University, Manhattan, KS (United States)

Many chirality-sensitive light–matter interactions are governed by chiral electron dynamics. Therefore, the development of advanced technologies making use of chiral phenomena would critically benefit from measuring and controlling chiral electron dynamics on their natural attosecond timescales. Such endeavours have so far been hampered by the lack of characterized circularly polarized attosecond pulses, an obstacle that has recently been overcome. Here we introduce chiroptical spectroscopy with attosecond pulses and demonstrate attosecond coherent control over photoelectron circular dichroism (PECD), as well as the measurement of chiral asymmetries in the forward–backward and angle-resolved photoionization delays of chiral molecules. We show that co-rotating attosecond and near-infrared (IR) pulses can nearly double the PECD and even change its sign compared with single-photon ionization. We demonstrate that chiral photoionization delays depend on both polar and azimuthal angles of photoemission in the light-propagation frame, requiring 3D momentum resolution. We measure forward–backward chiral-sensitive delays of up to 60 as and polar-angle-resolved photoionization delays of up to 240 as, which include an asymmetry of about 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 timescale.

• Research Organization: Kansas State University, Manhattan, KS (United States)
• Sponsoring Organization: National Energy Research Scientific Computing Center (NERSC); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
• Grant/Contract Number: AC02-05CH11231; FG02-86ER13491; SC0022105
• Other Award/Contract Number: CNS-1006860; EPS-1006860; EPS-0919443; ACI-1440548; CHE-1726332; NIH P20GM113109; BES-ERCAP0024357; 2244539
• OSTI ID: 3003065
• Journal Information: Nature (London), Journal Name: Nature (London) Journal Issue: 8079 Vol. 645; ISSN 1476-4687; ISSN 0028-0836
• Publisher: Nature Publishing Group
• Country of Publication: United States
• Language: English

Related Subjects

Atomic and molecular interactions with photons
Chemical physics
Circular dichroism