Observation of Rabi dynamics with a short-wavelength free-electron laser

Saikat Nandi (), Edvin Olofsson, Mattias Bertolino, Stefanos Carlström, Felipe Zapata, David Busto, Carlo Callegari, Michele Fraia, Per Eng-Johnsson, Raimund Feifel, Guillaume Gallician, Mathieu Gisselbrecht, Sylvain Maclot, Lana Neoričić, Jasper Peschel, Oksana Plekan, Kevin C. Prince, Richard J. Squibb, Shiyang Zhong, Philipp V. Demekhin, Michael Meyer, Catalin Miron, Laura Badano, Miltcho B. Danailov, Luca Giannessi, Michele Manfredda, Filippo Sottocorona, Marco Zangrando and Jan Marcus Dahlström ()
Additional contact information
Saikat Nandi: Université de Lyon, Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière
Edvin Olofsson: Lund University
Mattias Bertolino: Lund University
Stefanos Carlström: Lund University
Felipe Zapata: Lund University
David Busto: Lund University
Carlo Callegari: Elettra-Sincrotrone Trieste
Michele Fraia: Elettra-Sincrotrone Trieste
Per Eng-Johnsson: Lund University
Raimund Feifel: University of Gothenburg
Guillaume Gallician: Université Paris-Saclay, CEA, CNRS, LIDYL
Mathieu Gisselbrecht: Lund University
Sylvain Maclot: Lund University
Lana Neoričić: Lund University
Jasper Peschel: Lund University
Oksana Plekan: Elettra-Sincrotrone Trieste
Kevin C. Prince: Elettra-Sincrotrone Trieste
Richard J. Squibb: University of Gothenburg
Shiyang Zhong: Lund University
Philipp V. Demekhin: University of Kassel
Michael Meyer: European XFEL
Catalin Miron: Université Paris-Saclay, CEA, CNRS, LIDYL
Laura Badano: Elettra-Sincrotrone Trieste
Miltcho B. Danailov: Elettra-Sincrotrone Trieste
Luca Giannessi: Elettra-Sincrotrone Trieste
Michele Manfredda: Elettra-Sincrotrone Trieste
Filippo Sottocorona: Elettra-Sincrotrone Trieste
Marco Zangrando: Elettra-Sincrotrone Trieste
Jan Marcus Dahlström: Lund University

Nature, 2022, vol. 608, issue 7923, 488-493

Abstract: Abstract Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

Date: 2022
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DOI: 10.1038/s41586-022-04948-y

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