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arXiv:2201.10950

Studying ultrafast Rabi dynamics with a short-wavelength seeded free-electron laser

Saikat Nandi, Edvin Olofsson, Mattias Bertolino, Stefanos Carlström, Felipe Zapata, David Busto, Carlo Callegari, Michele Di Fraia, P. Johnsson, R. Feifel, Guillaume Gallician, Mathieu Gisselbrecht, Sylvain Maclot, Lana Neoričić, Jasper Peschel, Oksana Plekan, Kevin Charles Prince, Richard James Squibb, Shiyang Zhong, Philipp V. Demekhin, Michael Meyer, Catalin Miron, L. Badano, Miltcho Bojanov Danailov, Luca Giannessi, Michele Manfredda, Filippo Sottocorona, Marco Zangrando, Jan Marcus Dahlström

Published Jan 26, 2022• 0 citations
arXivHTMLPDF

Abstract

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. 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 interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

DOI
10.48550/arxiv.2201.10950

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Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. 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 interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.
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.
In coherent light-matter interactions the coherent state produced by the light pulse remains coherent during the entire period of observation. One of the well-known examples of such interactions is the Rabi oscillation—a periodic transfer of population in a two-level system induced by an external electromagnetic field. While these oscillations have been studied in light-matter interactions since the discovery of laser itself, most of the studies are limited to long wavelengths, typically ranging from microwave to visible radiation. Here, we discuss how such oscillations can be generated at shorter wavelengths, for example in the extreme ultraviolet domain, using intense femtosecond pulses from seeded free-electron lasers. When a two-level system is undergoing Rabi oscillations, it can be described via an ‘atom + photon’ dressed-state, the properties of which can be further manipulated to study quantum entanglement between massive particles. Our results offer opportunities to employ these intense laser pulses for generating and controlling coherent light-matter interactions across ultrashort timescales.
Abstract We present a theoretical study on the quantum control of ultrafast Rabi dynamics in atoms driven by chirped extreme ultraviolet (XUV) pulses. Motivated by recent experimental advances using free-electron lasers, we derive an analytical solution of the Rabi oscillation under the rotating wave approximation, incorporating the spectral chirp of the XUV field. Within the essential-states model, we demonstrate how the chirp modulates the phase of the excited-state amplitude, inducing an observable asymmetry in the Autler–Townes (AT) doublets of the photoelectrons. Our theoretical predictions, benchmarked against time-dependent Schrödinger equation simulations, reveal that chirp-dependent phase modulation governs the spectral asymmetry, offering a time-domain perspective for interpreting strong-field photoionization at short wavelengths. This work provides a compact analytical framework for chirp-mediated coherent control in the XUV regime and sheds light on recent experimental observations of asymmetric AT structures in helium.
We present an interferometric method for studying the Rabi dynamics in atoms by employing an $\ensuremath{\omega}\text{\ensuremath{-}}2\ensuremath{\omega}$ extreme ultraviolet pulse pair generated from the seeded free-electron laser. By solving the time-dependent Schr\"odinger equation (TDSE) for hydrogen atoms, we study the photoelectron spectrum that emerges when the $\ensuremath{\omega}$ pulse triggers Rabi oscillations between the ground state and the first excited state. The interference between the one-photon and two-photon ionization pathways in the photoelectron signal gives access to the phase difference between the one- and two-photon transition amplitudes. Compared to the cases without Rabi oscillations, an additional $\ensuremath{\pi}$ phase jump is observed in the energy domain. Based on perturbation theory, we demonstrate that this phase jump directly reflects the ultrafast buildup of Rabi oscillations in the time domain. The present $\ensuremath{\omega}\text{\ensuremath{-}}2\ensuremath{\omega}$ scheme can be generalized and applied to other more complex atoms or molecules provided that the populations of bound states can be efficiently and coherently modulated using the free-electron laser.
We study the photoelectron spectra of hydrogen and helium ionized by intense ultrafast two-color XUV laser pulses by numerically solving the time-dependent Schrödinger equation.The photon energy of the pump pulse is tuned to the 1s-2p excitation energy, inducing Rabi oscillations between these bound states and forming an Autler-Townes (AT) doublet of dressed states.When ionized by a time-delayed ultrafast XUV pulse with duration shorter than the Rabi oscillation period, we find novel and drastically enhanced AT splittings in the photoionization spectrum.We identify their origin in terms of the temporal interference of two attosecond wave packets whose spectral distribution is controlled by the interplay between Rabi frequency and bandwidth of the probe pulse.These time-dependent features in the spectra can be much larger than the standard AT spacing induced by the pump pulse alone and can be controlled by the time delay and the duration of the probe pulse.
We analyze theoretically the high intensity photoionization dynamics of a system with two atomic states resonantly coupled by coherent extreme ultraviolet laser radiation that also gives rise to the ionization. The ground state occupation of such a system is shown to exhibit damped Rabi oscillations. The corresponding ionization, which is responsible for the damping, scales almost linearly with the field intensity when the pulse length exceeds the Rabi period. For shorter pulses a quadratic scaling is found. The Rabi frequency is shifted compared to its value for an isolated two-level system. The shift increases with excitation intensity and can acquire a high percentage of the unrenormalized frequency at high intensities. Analytical results obtained within a simplified solvable model demonstrate that the damping and the shift both result from the coupling of the discrete states to the ionization continuum and are therefore closely related. Numerical simulations for a two-electron system reveal at high intensities the importance of off-resonant ionization channels.