Attosecond Optical Orientation
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- University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Max Born Institute, Berlin (Germany)
- King’s College, London (United Kingdom); Max Born Institute, Berlin (Germany)
- University of California, Berkeley, CA (United States)
- University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Circularly polarized light offers opportunities to probe symmetry-dependent properties of matter such as chirality and spin. Circular-dichroic measurements typically require further intrinsic or extrinsic breaking of symmetry by, e.g., enantiomeric excess, orientation, magnetic fields, or direction-sensitive detectors. Here we introduce circular-dichroic attosecond transient absorption spectroscopy by leveraging the angular momentum of two circularly polarized pulses, both pump and probe, in an isotropic medium, optically orienting the angular momentum of excited states on an attosecond timescale. We investigate a circular-dichroic measurement of the attosecond transient absorption of He Rydberg states. By limiting the allowed pathways via dipole selection rules for co- and counterrotating circularly polarized near-infrared and extreme ultraviolet (XUV) pulses, different spectral reshapings of the XUV transient absorption due to the AC Stark effect are observed. Furthermore, paired with time-dependent Schrödinger equation calculations, the results show the role of selection and propensity rules and open up new opportunities to study coupling pathways of excited states as well as spin-dependent dynamics in atoms and beyond via attosecond optical orientation.
- Research Organization:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Organization:
- European Union’s Horizon research and innovation programme; National Science Foundation (NSF; UK Research and Innovation (UKRI); US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
- Grant/Contract Number:
- AC02-05CH11231
- OSTI ID:
- 3014361
- Journal Information:
- Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 16 Vol. 135; ISSN 1079-7114; ISSN 0031-9007
- Publisher:
- American Physical Society (APS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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