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arXiv:1205.4918 · Physical Review A

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

Stefano M. Cavaletto, Christian Buth, Z. Harman, Elliot P. Kanter, Stephen H. Southworth, Linda Young, Christoph H. Keitel

Published Sep 4, 2012• 48 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreva.86.033402

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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 1s2p\ensuremath−1\ensuremath→1s\ensuremath−12p1s2{p}^{\ensuremath{-}1}\ensuremath{\rightarrow}1{s}^{\ensuremath{-}1}2p1s2p\ensuremath−1\ensuremath→1s\ensuremath−12p 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.
The direct and optical control of x-ray transitions is studied theoretically by investigating the spectra of resonance fluorescence and absorption. The work is motivated by the rapid advances in x-ray science, enabling the application of quantum-control schemes at short wavelengths. In a two-level system we study Rabi oscillations of atomic inner-shell electrons, induced by intense x-ray pulses and competing with Auger decay, and their signature in the spectrum of resonance fluorescence. Subsequently, optical manipulation of x-ray transitions is examined, by employing an optical frequency comb coupling nearby excited levels to control their spontaneous decay. First, narrow-bandwidth x rays are adopted, giving rise to the periodic shaping of the atomic dynamic variables and the imprinting of a comb onto the x-ray resonance fluorescence spectrum. A more realistic model for an immediate experimental implementation is then provided, by developing a scheme to imprint a comb onto the absorption spectrum of an ultrashort x-ray pulse. An experimental realization of the predicted comb structures is anticipated to transfer the accuracy of optical frequency combs into the x-ray regime
We present a time-dependent Schr\"odinger equation approach within a nonrelativistic quantum electrodynamics framework to investigate resonant x-ray scattering driven by intense x-ray pulses. This method enables us to explore how coherent x-ray electron dynamics influence scattering signals from Ne+{\mathrm{Ne}}^{+}Ne+. We account for both resonance fluorescence and elastic scattering channels, while also considering competing photoionization and inner-shell decay processes. By computing the angular distribution and energy spectrum of scattered photons, we uncover interference effects between elastic scattering and resonance fluorescence pathways. Notably, this interference results in a small asymmetry in the energy spectrum. We discuss the experimental potential for detecting signatures of interference. Our findings demonstrate that the x-ray Rabi dynamics can be used to control scattering responses and provide insights into interference mechanisms and scattering efficiency in high-intensity x-ray regimes.
The direct interaction between nuclei and strong electromagnetic fields generated by novel coherent x-ray light sources such as the x-ray free electron laser is studied. We investigate the case of various stable or long-lived isotopes with energetically low-lying excited states, where the laser drives the nuclear transition from the ground to the first excited state. We therefore consider the nucleus as a two-level system including the corresponding hyperfine levels in our theoretical description. The performance of present and upcoming x-ray free electron laser facilities in coherently controlling the nuclear excited state population is analyzed for setups involving both solid state as well as accelerated nuclear targets to bridge the gap between photon and transition frequency. Current and predicted laser parameters are applied to calculate excited state populations and signal photon rates of nuclei after a radiation pulse, finding significant improvements compared to former calculations. Furthermore, we determine the parameters necessary to transfer substantial amounts of the nuclear ground state population to the excited state, and therefore to bring nuclear Rabi-oscillation within reach. Additionally, we take into account for the first time collective effects that take place in solid state targets and show that they may provide a significant effect in broadening natural linewidths of nuclear levels depending on the experimental setup. Our findings support the case of nuclear quantum optics for XFEL applications. Therefore, one hopes that eventually coherent control of nuclear transitions can be successfully applied in a number of areas in nuclear physics including preparation, control and detection methods.
Irradiation of a medium by short intense pulses from x-ray (XUV) free-electron lasers can result in saturated photoionization of inner electronic shells. As a result an inversion of populations between core levels appears. The resulting fluorescent radiation can be amplified during its propagation through the inverted medium and results in intense, quasi-transform-limited radiation bursts. While the optical counterpart of this phenomena, known as superfluorescence, was intensively investigated, a generalized treatment is needed in the x-ray (XUV) domain, where the dynamics of pumping and evolution due to fast decay processes play a crucial role. To provide a general theoretical approach, we start from the fundamental, quantized minimal coupling Hamiltonian of light-matter interaction and after a series of approximations arrive at a closed system of equations for the two-point correlation function of atomic coherences and the two-time correlation function of the emitted field. The obtained formalism enables us to investigate collective spontaneous emission in various regimes. It is extended consistently to include incoherent processes that are relevant in the x-ray (XUV) domain. These processes are introduced into the formalism by corresponding Lindblad superoperators. The connection to other approaches is discussed and numerical examples related to recent experiments are presented.
We develop a large scale quantum master equation approach to describe dynamical processes of practical open quantum systems driven by both coherent and stochastic interactions by including more than one thousand true states of the systems, motivated by the development of highly bright and fully coherent lasers in the X-ray wavelength regime. The method combines the processes of coherent dynamics induced by the X-ray laser and incoherent relaxations due to spontaneous emissions, Auger decays, and electronic collisions. As examples, theoretical investigation of {\it real} coherent dynamics of inner-shell electrons of a neon gas, irradiated by a high-intensity X-ray laser with a full temporal coherence, is carried out with the approach. In contrast to the rate equation treatment, we find that coherence can suppress the multiphoton absorptions of a neon gas in the ultra-intense X-ray pulse, due to coherence-induced Rabi oscillations and power broadening effects. We study the influence of coherence on ionization processes of neon, and directly prove that sequential single-photon processes for both outer- and inner-shell electrons dominate the ionizations for the recently typical experiments with a laser intensity of ≈1018\approx10^{18}≈1018 W/cm2{\rm W/cm^2}W/cm2. We discuss possible experimental implementations such as signatures for coherent evolution of inner-shell electrons via resonance fluorescence processes. The approach can also be applied to many different practical open quantum systems in atomic, quantum optical, and cold matter systems, which are treated qualitatively by a few-level master equation model before.
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.