Coherent nonlinear X-ray four-photon interaction with core-shell electrons
TL;DR
Researchers demonstrated coherent four-photon interactions with core-shell electrons using X-ray free-electron lasers, enabling background-free four-wave mixing in gaseous neon. This method advances multidimensional correlation spectroscopy at atomic scales and shows potential for ultrafast time-resolved studies of electron dynamics in various systems.
Key Takeaways
- •Coherent nonlinear X-ray four-wave mixing with core-shell electrons was achieved using single broadband pulses from a free-electron laser, producing background-free signals.
- •The technique involves doubly resonant processes like X-ray coherent anti-Stokes electronic Raman scattering, enabling 2D spectral mapping for atomic-scale correlation spectroscopy.
- •Time-delayed multicolour X-ray pulses extend the methodology to the ultrafast time domain, facilitating studies of localized electron dynamics in biomolecules and quantum materials.
- •Potential applications include energy conversion, biomedical imaging, and quantum information technologies, leveraging state and site selectivity in electronic interactions.
Tags
Abstract
Coherent nonlinear light–matter interaction with X-rays gives access to a regime in ultrafast spectroscopy in which atomic resolution meets femtosecond and attosecond timescales1,2. Particularly, X-ray four-wave mixing, involving several resonant transitions in a single coherent nonlinear process, has the potential to provide information on the electronic states coupling, coherent electron motion, correlation and dynamics, with state and site selectivity3,4,5. Here we demonstrate coherent, background-free four-photon interactions with core-shell electrons using single broadband X-ray pulses from a free-electron laser. The all-X-ray four-wave mixing signals, measured in gaseous neon, arise from doubly resonant nonlinear processes involving Raman transitions6, including X-ray coherent anti-Stokes electronic Raman scattering. The 2D spectral maps (photon-in/photon-out) represent a step towards multidimensional correlation spectroscopy at the atomic scale. Using a multicolour time-delayed X-ray pulse scheme, we further demonstrate the feasibility of extending the proposed methodology to the ultrafast time domain. These results reveal potential for studying localized electron dynamics in multiple systems, from biomolecules to correlated quantum materials, with applications in areas such as energy conversion, biomedical imaging and quantum information technologies.
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Data availability
The raw data used in this study are available in a collaborative manner at the PSI Public Data Repository: https://doi.org/10.16907%2F7a7bd9c2-3258-454f-96cd-4c8f9d46464c.
Code availability
Data analysis codes are available on request. The codes for the model are available in a collaborative manner on request.
References
Mukamel, S., Healion, D., Zhang, Y. & Biggs, J. D. Multidimensional attosecond resonant X-ray spectroscopy of molecules: lessons from the optical regime. Annu. Rev. Phys. Chem. 64, 101–127 (2013).
Leone, S. R. & Neumark, D. M. Probing matter with nonlinear spectroscopy. Science 379, 536–537 (2023).
Tanaka, S. & Mukamel, S. Coherent X-ray Raman spectroscopy: a nonlinear local probe for electronic excitations. Phys. Rev. Lett. 89, 043001 (2002).
Kraus, P. M., Zürch, M., Cushing, S. K., Neumark, D. M. & Leone, S. R. The ultrafast X-ray spectroscopic revolution in chemical dynamics. Nat. Rev. Chem. 2, 82–94 (2018).
Chergui, M., Beye, M., Mukamel, S., Svetina, C. & Masciovecchio, C. Progress and prospects in nonlinear extreme-ultraviolet and X-ray optics and spectroscopy. Nat. Rev. Phys. 5, 578–596 (2023).
Weninger, C. et al. Stimulated electronic X-ray Raman scattering. Phys. Rev. Lett. 111, 233902 (2013).
Mukamel, S. Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations. Annu. Rev. Phys. Chem. 51, 691–729 (2000).