Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review Letters

Proposal for Observing XUV-Induced Rabi Oscillation Using Superfluorescent Emission

Jun Jie Cui, Yongjun Cheng, Xin Wang, Zheng Li, Nina Rohringer, Victor Kimberg, Song Bin Zhang

Published Jul 25, 2023• 10 citations
Publisher

Abstract

Intense x-ray and extreme ultraviolet (XUV) light sources have been available for decades, however, due to weak nonlinear interaction in the XUV photon energy range, observation of Rabi oscillation induced by XUV pulse remains a very challenging experimental task. Here we suggest a scheme where photoionization of a He medium by an intense XUV pump pulse is followed by a strong population inversion and Rabi oscillation at the He^{+}(1s-3p) transition and is accompanied by superfluorescence (SF) of the 7.56 eV pulse at the He^{+}(3p-2s) transition. Our numerical simulations show that the Rabi oscillation at the He^{+}(1s-3p) transition induced by an XUV pulse with photon energy 48.36 eV results in significant signatures in the SF spectra, allowing us to identify and characterize the XUV induced Rabi-oscillatory regime. The proposed scheme provides a sensitive tool to monitor and control ultrafast nonlinear dynamics in atoms and molecules triggered by intense XUV.

DOI
10.1103/physrevlett.131.043201

Related papers

Rabi oscillations in extreme ultraviolet ionization of atomic argon

Martin Flögel, Judith Durá, Bernd Schütte +3 more

We demonstrate Rabi oscillations in nonlinear ionization of argon by an intense femtosecond extreme ultraviolet (XUV) laser field produced by high-harmonic generation. We monitor the formation of $\mathrm{A}{\mathrm{r}}^{2+}$ as a function of the time delay between the XUV pulse and an additional near-infrared (NIR) femtosecond laser pulse, and show that the population of an $\mathrm{A}{\mathrm{r}}^{+*}$ intermediate resonance exhibits strong modulations both due to an NIR laser-induced Stark shift and XUV-induced Rabi cycling between the ground state of $\mathrm{A}{\mathrm{r}}^{+}$ and the $\mathrm{A}{\mathrm{r}}^{+*}$ excited state. Our experiment represents a direct experimental observation of a Rabi-cycling process in the XUV regime.

Physical Review A•Feb 10, 2017•22 citations

Quantum control of Rabi dynamics using chirped extreme ultraviolet pulses

Dongyang He, Boren Shen, Yi-Jia Mao +4 more

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.

New Journal of Physics•Oct 28, 2025•2 citations

Observation of Free-Electron-Laser-Induced Collective Spontaneous Emission (Superfluorescence)

Mitsuru Nagasono, James Robert Harries, Hiroshi Iwayama +7 more

We have observed and characterized 501.6 nm collective spontaneous emission (superfluorescence) following 1s(2) → 1s3p excitation of helium atoms by 53.7 nm free-electron laser radiation. Emitted pulse energies of up to 100 nJ are observed, corresponding to a photon number conversion efficiency of up to 10%. We observe the peak intensity to scale as ρ(2) and the emitted pulse width and delay to scale as ρ(-1), where ρ is the atom number density. Emitted pulses as short as 1 ps are observed, which corresponds to a rate around 75,000 times faster than the spontaneous 1s3p → 1s2s decay rate. To our knowledge, this is the first observation of superfluorescence following pumping in the extreme ultraviolet wavelength region, and extension of the technique to the generation of extreme ultraviolet and x-ray superfluorescence pulses should be straightforward by using suitable atomic systems and pump wavelengths.

Physical Review Letters•Nov 1, 2011•46 citations

Extreme-ultraviolet coherent pulse amplification in argon

Carles Serrat, J. Seres, E. Seres +1 more

The amplification of ultrashort extreme-ultraviolet (XUV) pulses in argon in high-order harmonic generation processes is studied by using the time-dependent Schr\"odinger equation in the spin-free one-active-electron and single-atom approximation. We consider a neutral argon atom initially in the valence 3p state and a sufficiently intense two-cycle driving infrared (IR) pulse for the atom to be mainly ionized after the first laser cycle. The correlated dynamics and transitions from the valence 3p to a virtual subvalence 3s state and in the ionized regions are examined by synchronizing a 1.5-fs XUV pulse to the IR pulse. The calculated single-atom gain spectrum (26--45 eV) agrees with recent experimental measurements. We discuss different channels that can be present in the gain process as a function of pulse parameters and through an analysis of the dynamics of the populations in terms of field-free eigenstates. When the XUV pulse is considered at the end of the driving IR field the amplification is due to contributions of stimulated recombination from excited Rydberg and low energy continuum states to the 3s and 3p states of argon. In regions where the IR field is intense, high energy and angular momentum states are populated and the medium can interact with the pulses through bound and continuum states involving parametric transitions, which is further confirmed by studying classical electron trajectories. We discuss how these parametric interactions might be suitable for amplification of photon energies far from the ionization threshold as observed in the experiments.

Physical Review A•Jun 25, 2019•8 citations

Enhancing Autler-Townes splittings by ultrafast XUV pulses

Wei‐Chao Jiang, Hao Liang, Shun Wang +2 more

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.

Physical Review Research•Aug 25, 2021•31 citations

Ultrafast opto-optical control of extreme ultraviolet light pulses

Samuel Bengtsson

Extreme ultraviolet (XUV) light is a valuable frequency range for ultrafast optics experiments. The short wavelength is a requirement for ultrashort pulses, which are widely used to characterize fast dynamics. Additionally, the high photon energy enables quantum control of high frequency transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Presently, however, no good modulators exist for these frequencies, which significantly reduces the possible ultrafast optics experiments or applications in the XUV regime. This thesis addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light a method is described which modulates the phase of XUV light emitted from a gas of noble atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation. After the excitation pulse has passed through the gas, the atoms will emit light in the absence of an external field, known as free induction. The phase of the emitted light is changed by shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse. This phase-control of the emitting atoms also translates into a control of the phase of the emitted XUV field.With the method described in the previous paragraph, the direction of XUV light emitted from noble gases was controlled, and the temporal dynamics of the emission was studied. The redirection of the XUV emission, through the use of a spatially offset IR pulse, was found to change both with intensity of the control pulse and by changing the spatial offset between the pulses. By varying the delay between the excitation and the control pulse the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, with two control pulses the emission was redirected twice, resulting in an XUV pulse shape with controlled duration emitted with a certain angle. Hopefully the presented work will result in more research into the development of this technique, to fully realize the possibility to shape the amplitude and phase of XUV pulses. Such a development would open the door for ultrafast XUV quantum control.

•Jan 1, 2017•1 citation
Intense x-ray and extreme ultraviolet (XUV) light sources have been available for decades, however, due to weak nonlinear interaction in the XUV photon energy range, observation of Rabi oscillation induced by XUV pulse remains a very challenging experimental task. Here we suggest a scheme where photoionization of a He medium by an intense XUV pump pulse is followed by a strong population inversion and Rabi oscillation at the He^{+}(1s-3p) transition and is accompanied by superfluorescence (SF) of the 7.56 eV pulse at the He^{+}(3p-2s) transition. Our numerical simulations show that the Rabi oscillation at the He^{+}(1s-3p) transition induced by an XUV pulse with photon energy 48.36 eV results in significant signatures in the SF spectra, allowing us to identify and characterize the XUV induced Rabi-oscillatory regime. The proposed scheme provides a sensitive tool to monitor and control ultrafast nonlinear dynamics in atoms and molecules triggered by intense XUV.
We demonstrate Rabi oscillations in nonlinear ionization of argon by an intense femtosecond extreme ultraviolet (XUV) laser field produced by high-harmonic generation. We monitor the formation of Ar2+\mathrm{A}{\mathrm{r}}^{2+}Ar2+ as a function of the time delay between the XUV pulse and an additional near-infrared (NIR) femtosecond laser pulse, and show that the population of an Ar+∗\mathrm{A}{\mathrm{r}}^{+*}Ar+∗ intermediate resonance exhibits strong modulations both due to an NIR laser-induced Stark shift and XUV-induced Rabi cycling between the ground state of Ar+\mathrm{A}{\mathrm{r}}^{+}Ar+ and the Ar+∗\mathrm{A}{\mathrm{r}}^{+*}Ar+∗ excited state. Our experiment represents a direct experimental observation of a Rabi-cycling process in the XUV regime.
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 have observed and characterized 501.6 nm collective spontaneous emission (superfluorescence) following 1s(2) → 1s3p excitation of helium atoms by 53.7 nm free-electron laser radiation. Emitted pulse energies of up to 100 nJ are observed, corresponding to a photon number conversion efficiency of up to 10%. We observe the peak intensity to scale as ρ(2) and the emitted pulse width and delay to scale as ρ(-1), where ρ is the atom number density. Emitted pulses as short as 1 ps are observed, which corresponds to a rate around 75,000 times faster than the spontaneous 1s3p → 1s2s decay rate. To our knowledge, this is the first observation of superfluorescence following pumping in the extreme ultraviolet wavelength region, and extension of the technique to the generation of extreme ultraviolet and x-ray superfluorescence pulses should be straightforward by using suitable atomic systems and pump wavelengths.
The amplification of ultrashort extreme-ultraviolet (XUV) pulses in argon in high-order harmonic generation processes is studied by using the time-dependent Schr\"odinger equation in the spin-free one-active-electron and single-atom approximation. We consider a neutral argon atom initially in the valence 3p state and a sufficiently intense two-cycle driving infrared (IR) pulse for the atom to be mainly ionized after the first laser cycle. The correlated dynamics and transitions from the valence 3p to a virtual subvalence 3s state and in the ionized regions are examined by synchronizing a 1.5-fs XUV pulse to the IR pulse. The calculated single-atom gain spectrum (26--45 eV) agrees with recent experimental measurements. We discuss different channels that can be present in the gain process as a function of pulse parameters and through an analysis of the dynamics of the populations in terms of field-free eigenstates. When the XUV pulse is considered at the end of the driving IR field the amplification is due to contributions of stimulated recombination from excited Rydberg and low energy continuum states to the 3s and 3p states of argon. In regions where the IR field is intense, high energy and angular momentum states are populated and the medium can interact with the pulses through bound and continuum states involving parametric transitions, which is further confirmed by studying classical electron trajectories. We discuss how these parametric interactions might be suitable for amplification of photon energies far from the ionization threshold as observed in the experiments.
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.
Extreme ultraviolet (XUV) light is a valuable frequency range for ultrafast optics experiments. The short wavelength is a requirement for ultrashort pulses, which are widely used to characterize fast dynamics. Additionally, the high photon energy enables quantum control of high frequency transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Presently, however, no good modulators exist for these frequencies, which significantly reduces the possible ultrafast optics experiments or applications in the XUV regime. This thesis addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light a method is described which modulates the phase of XUV light emitted from a gas of noble atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation. After the excitation pulse has passed through the gas, the atoms will emit light in the absence of an external field, known as free induction. The phase of the emitted light is changed by shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse. This phase-control of the emitting atoms also translates into a control of the phase of the emitted XUV field.With the method described in the previous paragraph, the direction of XUV light emitted from noble gases was controlled, and the temporal dynamics of the emission was studied. The redirection of the XUV emission, through the use of a spatially offset IR pulse, was found to change both with intensity of the control pulse and by changing the spatial offset between the pulses. By varying the delay between the excitation and the control pulse the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, with two control pulses the emission was redirected twice, resulting in an XUV pulse shape with controlled duration emitted with a certain angle. Hopefully the presented work will result in more research into the development of this technique, to fully realize the possibility to shape the amplitude and phase of XUV pulses. Such a development would open the door for ultrafast XUV quantum control.