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 A

Propagation of a strong x-ray pulse: Pulse compression, stimulated Raman scattering, amplified spontaneous emission, lasing without inversion, and four-wave mixing

Yuping Sun, Ji‐Cai Liu, Chuan‐Kui Wang, Faris Gel’mukhanov

Published Jan 20, 2010• 71 citations
Publisher

Abstract

We study the compression of strong x-ray pulses from x-ray free-electron lasers (XFELs) propagating through the resonant medium of atomic argon. The simulations are based on the three-level model with the frequency of the incident x-ray pulse tuned in the $2{p}_{3/2}\text{\ensuremath{-}}4s$ resonance. The pulse propagation is accompanied by the self-seeded stimulated resonant Raman scattering (SRRS). The SRRS starts from two channels of amplified spontaneous emission (ASE), $4s\text{\ensuremath{-}}2{p}_{3/2}$ and $3s\text{\ensuremath{-}}2{p}_{3/2}$, which form the extensive ringing pattern and widen the power spectrum. The produced seed field triggers the Stokes ASE channel $3s\text{\ensuremath{-}}2{p}_{3/2}$. The population inversion is quenched for longer propagation distances where the ASE is followed by the lasing without inversion (LWI), which amplifies the Stokes component. Both ASE and LWI reshape the input pulse: The compressed front part of the pulse (up to 100 as) is followed by the long tail of the ringing and beating between the pump and Stokes frequencies. The pump pulse also generates weaker Stokes and anti-Stokes fields caused by four-wave mixing. These four spectral bands have fine structures caused by the dynamical Stark effect. A slowdown of the XFEL pulse up to 78% of the speed of light in vacuum is found because of a large nonlinear refractive index.

DOI
10.1103/physreva.81.013812

Related papers

The propagation of a strong x-ray pulse followed by pulse slowdown and compression, amplified spontaneous emission and lasing without inversion

Yuping Sun, Ji‐Cai Liu, Faris Gel’mukhanov

We study self-seeded stimulated resonant x-ray Raman scattering and show a 20-fold compression of the strong XFEL pulse propagating through the resonant medium of atomic argon with the frequency (244.3 eV) tuned to the 2p 3/2 –4s resonance. The strong x-ray pulse inverts the medium and produces an extensive ringing tail which widens the power spectrum. Newly created seed field triggers the Stokes channel 3s–2p 3/2 of amplified spontaneous emission. The population inversions are quenched for longer propagation distances where lasing without inversion enhances the Stokes component. The pump pulse also generates weaker Stokes and anti-Stokes fields caused by four-wave mixing. The group velocity is decreased up to 78% of the speed of light in vacuum.

Journal of Physics B Atomic Molecular and Optical Physics•Oct 7, 2009•8 citations

Suppression of resonant auger effect with chirped x-ray free-electron laser pulse

Yuping Sun, Quan Miao, Aiping Zhou +3 more

Abstract We study the Auger effect in the presence of strong x-ray free-electron lasers (XFELs) propagating through resonant argon vapors by solving the Maxwell–Bloch equations numerically. The simulations are based on the three-level system with the carrier frequency tuned in the 2 p 3/2 –4 s resonance. It is shown that the Auger branching is sensitive to the pulse area and duration. The relative Auger yield can be suppressed in the course of pulse propagation due to the interplay between the Auger decay and stimulated emission. Further suppression can be achieved by chirping the initial pulse, which is more effective for the long-pulse case. In addition, the sign and magnitude of the chirp rate play important roles in pulse reshaping and Auger emission.

Journal of Physics B Atomic Molecular and Optical Physics•Nov 1, 2017•2 citations

Influence on parametric four-wave mixing of a two-photon interference effect

W. R. Garrett, Richard Wunderlich, Roger C. Hart +2 more

If an extended Na vapor column (heat pipe configuration) is subjected to strong laser pumping near two-photon resonance with 3D3/2,5/2 or 4D3/2,5/2 states at pressures above tens of millitorr, strong stimulated emissions are produced by amplified spontaneous emission (ASE) or stimulated electron in hyper-Raman scattering (SEHRS) and by phase matched parametric four-wave mixing (PFWM). These new electromagnetic fields that are generated within the near-resonant nonlinear medium can strongly influence the total atomic response and produce several saturation and total cancellation types of effect.

Quantum Electronics and Laser Science Conference•Apr 24, 1989•0 citations

Transition between amplified spontaneous emission and superfluorescence in a longitudinally pumped medium by an x-ray free-electron-laser pulse

Yu-Hung Kuan, Wen-Te Liao

The transition from the amplification of spontaneous emission to superfluorescence in a three-level and swept-gain medium excited by an x-ray free-electron-laser pulse is theoretically investigated. Given the specific timescale of an x-ray free-electron-laser pulse, we investigate the swept pumping process in detail, and our results show that the temporal structure of an x-ray free-electron-laser pulse plays a more critical role than its peak intensity does for producing population inversion. The typical watershed of two radiant regions depends on the optical depth of the gain medium for a given coherence time, namely, the particle number density and medium length are equally important. However, we find that medium length plays a more important role than particle density for making the forward-backward asymmetry. The transient gain length and the total medium length are identified as two important factors to observe length-induced backward transition. The present results suggest an application of parametric controls over a single-pass-amplified light source.

arXiv:1911.00450•Physical Review A•Feb 24, 2020•7 citations

Resonance fluorescence in ultrafast and intense x-ray free-electron-laser pulses

Stefano M. Cavaletto, Christian Buth, Z. Harman +4 more

The spectrum of resonance fluorescence is calculated for a two-level system excited by an intense, ultrashort x-ray pulse made available, for instance, by free-electron lasers such as the Linac Coherent Light Source. We allow for inner-shell hole decay widths and destruction of the system by further photoionization. This two-level description is employed to model neon cations strongly driven by x rays tuned to the $1s2{p}^{\ensuremath{-}1}\ensuremath{\rightarrow}1{s}^{\ensuremath{-}1}2p$ transition at $848\phantom{\rule{0.28em}{0ex}}\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$; the x rays induce Rabi oscillations which are so fast that they compete with Ne $1s$-hole decay. We predict resonance fluorescence spectra for two different scenarios: first, chaotic pulses based on the self-amplified spontaneous emission principle, like those presently generated at x-ray free-electron-laser facilities and, second, Gaussian pulses which will become available in the foreseeable future with self-seeding techniques. As an example of the exciting opportunities derived from the use of seeding methods, we predict, in spite of the above obstacles, the possibility to distinguish at x-ray frequencies a clear signature of Rabi flopping in the spectrum of resonance fluorescence.

arXiv:1205.4918•Physical Review A•Sep 4, 2012•48 citations

Dynamics of multiphoton processes in nonlinear optics and x-ray spectroscopy

Ji‐Cai Liu

New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of microsecond pulses is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties. The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation. We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation.

•Jan 1, 2009•0 citations
We study the compression of strong x-ray pulses from x-ray free-electron lasers (XFELs) propagating through the resonant medium of atomic argon. The simulations are based on the three-level model with the frequency of the incident x-ray pulse tuned in the 2p3/2\ensuremath-4s2{p}_{3/2}\text{\ensuremath{-}}4s2p3/2​\ensuremath-4s resonance. The pulse propagation is accompanied by the self-seeded stimulated resonant Raman scattering (SRRS). The SRRS starts from two channels of amplified spontaneous emission (ASE), 4s\ensuremath-2p3/24s\text{\ensuremath{-}}2{p}_{3/2}4s\ensuremath-2p3/2​ and 3s\ensuremath-2p3/23s\text{\ensuremath{-}}2{p}_{3/2}3s\ensuremath-2p3/2​, which form the extensive ringing pattern and widen the power spectrum. The produced seed field triggers the Stokes ASE channel 3s\ensuremath-2p3/23s\text{\ensuremath{-}}2{p}_{3/2}3s\ensuremath-2p3/2​. The population inversion is quenched for longer propagation distances where the ASE is followed by the lasing without inversion (LWI), which amplifies the Stokes component. Both ASE and LWI reshape the input pulse: The compressed front part of the pulse (up to 100 as) is followed by the long tail of the ringing and beating between the pump and Stokes frequencies. The pump pulse also generates weaker Stokes and anti-Stokes fields caused by four-wave mixing. These four spectral bands have fine structures caused by the dynamical Stark effect. A slowdown of the XFEL pulse up to 78% of the speed of light in vacuum is found because of a large nonlinear refractive index.
We study self-seeded stimulated resonant x-ray Raman scattering and show a 20-fold compression of the strong XFEL pulse propagating through the resonant medium of atomic argon with the frequency (244.3 eV) tuned to the 2p 3/2 –4s resonance. The strong x-ray pulse inverts the medium and produces an extensive ringing tail which widens the power spectrum. Newly created seed field triggers the Stokes channel 3s–2p 3/2 of amplified spontaneous emission. The population inversions are quenched for longer propagation distances where lasing without inversion enhances the Stokes component. The pump pulse also generates weaker Stokes and anti-Stokes fields caused by four-wave mixing. The group velocity is decreased up to 78% of the speed of light in vacuum.
Abstract We study the Auger effect in the presence of strong x-ray free-electron lasers (XFELs) propagating through resonant argon vapors by solving the Maxwell–Bloch equations numerically. The simulations are based on the three-level system with the carrier frequency tuned in the 2 p 3/2 –4 s resonance. It is shown that the Auger branching is sensitive to the pulse area and duration. The relative Auger yield can be suppressed in the course of pulse propagation due to the interplay between the Auger decay and stimulated emission. Further suppression can be achieved by chirping the initial pulse, which is more effective for the long-pulse case. In addition, the sign and magnitude of the chirp rate play important roles in pulse reshaping and Auger emission.
If an extended Na vapor column (heat pipe configuration) is subjected to strong laser pumping near two-photon resonance with 3D3/2,5/2 or 4D3/2,5/2 states at pressures above tens of millitorr, strong stimulated emissions are produced by amplified spontaneous emission (ASE) or stimulated electron in hyper-Raman scattering (SEHRS) and by phase matched parametric four-wave mixing (PFWM). These new electromagnetic fields that are generated within the near-resonant nonlinear medium can strongly influence the total atomic response and produce several saturation and total cancellation types of effect.
The transition from the amplification of spontaneous emission to superfluorescence in a three-level and swept-gain medium excited by an x-ray free-electron-laser pulse is theoretically investigated. Given the specific timescale of an x-ray free-electron-laser pulse, we investigate the swept pumping process in detail, and our results show that the temporal structure of an x-ray free-electron-laser pulse plays a more critical role than its peak intensity does for producing population inversion. The typical watershed of two radiant regions depends on the optical depth of the gain medium for a given coherence time, namely, the particle number density and medium length are equally important. However, we find that medium length plays a more important role than particle density for making the forward-backward asymmetry. The transient gain length and the total medium length are identified as two important factors to observe length-induced backward transition. The present results suggest an application of parametric controls over a single-pass-amplified light source.
The spectrum of resonance fluorescence is calculated for a two-level system excited by an intense, ultrashort x-ray pulse made available, for instance, by free-electron lasers such as the Linac Coherent Light Source. We allow for inner-shell hole decay widths and destruction of the system by further photoionization. This two-level description is employed to model neon cations strongly driven by x rays tuned to the $1s2{p}^{\ensuremath{-}1}\ensuremath{\rightarrow}1{s}^{\ensuremath{-}1}2p$ transition at 848eV848\phantom{\rule{0.28em}{0ex}}\phantom{\rule{0.16em}{0ex}}\mathrm{eV}848eV; the x rays induce Rabi oscillations which are so fast that they compete with Ne 1s1s1s-hole decay. We predict resonance fluorescence spectra for two different scenarios: first, chaotic pulses based on the self-amplified spontaneous emission principle, like those presently generated at x-ray free-electron-laser facilities and, second, Gaussian pulses which will become available in the foreseeable future with self-seeding techniques. As an example of the exciting opportunities derived from the use of seeding methods, we predict, in spite of the above obstacles, the possibility to distinguish at x-ray frequencies a clear signature of Rabi flopping in the spectrum of resonance fluorescence.
New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of microsecond pulses is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties. The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation. We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation.