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Physical Review A

Pulse propagation of synchrotron radiation through a nuclear two-resonance system

Uwe van Bürck, W. Potzel, P. Schindelmann, Yuri V. Shvyd'ko, Erich Gerdau, O. Leupold, H. D. Rüter

Published Dec 8, 1999• 11 citations
Publisher

Abstract

Pulse propagation through a two-resonance medium was investigated in nuclear forward scattering (NFS) of synchrotron radiation (SR). The SR pulse was coherently transmitted through a target system exhibiting two equivalent resonances, the energy separation of which was varied via the Doppler effect. This allowed a continuous change from a single-resonance medium to a two-resonance system with adjustable splitting. For increasing splitting, the observed time evolutions of NFS changed from a dynamical beat (DB) via hybrid forms of beating into a DB-modulated quantum beat. The experimental results were consistently fitted using a dynamical theory for NFS of SR.

DOI
10.1103/physreva.61.013803

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•Jan 1, 2006•1 citation
Pulse propagation through a two-resonance medium was investigated in nuclear forward scattering (NFS) of synchrotron radiation (SR). The SR pulse was coherently transmitted through a target system exhibiting two equivalent resonances, the energy separation of which was varied via the Doppler effect. This allowed a continuous change from a single-resonance medium to a two-resonance system with adjustable splitting. For increasing splitting, the observed time evolutions of NFS changed from a dynamical beat (DB) via hybrid forms of beating into a DB-modulated quantum beat. The experimental results were consistently fitted using a dynamical theory for NFS of SR.
The nuclear forward scattering of synchrotron radiation (SR) of two spatially separated stainless-steel foils has been investigated. Immediately after the SR pulse a nuclear exciton extending over both targets is formed, which then decays under the influence of radiative coupling of the nuclear oscillators both within and between the targets. Cooling one target to low temperatures causes the M\"ossbauer linewidth to increase by inhomogeneous broadening, which leads to a rapid dephasing of the nuclear oscillators of this system. In general, the influence of the radiation field of the upstream oscillators on the oscillators of the downstream target causes the latter to radiate at a high decay rate (steep slope) at early times. Surprisingly, for the combined targets, the initial decay can be less steep than that of the inhomogeneously broadened sample alone if this broadening is sufficiently large. In addition, when the upstream oscillators are broadened in energy they may cause the downstream oscillators to emit only very little intensity at late times. In the experiments, this influence on the downstream sample was changed by varying the inhomogeneous resonance broadening and the resonance frequencies of the targets. Drastic changes of the time evolution of the nuclear forward scattering were observed, which are discussed within the dynamical theory.
Means to coherently control single x-ray photons in resonant scattering of light off nuclei by electric or magnetic fields are investigated theoretically. In order to derive the time response in nuclear forward scattering, we adapt the Maxwell–Bloch equations known from quantum optics to describe the resonant light pulse propagation through a nuclear medium. Two types of time-dependent perturbations of nuclear forward scattering are considered for coherent control of the resonantly scattered x-ray quanta. Firstly, the simultaneous coherent propagation of two pulses through the nuclear sample is addressed. We find that the signal of a weak pulse can be enhanced or suppressed by a stronger pulse simultaneously propagating through the sample in counter-propagating geometry. Secondly, the effect of a time-dependent hyperfine splitting is investigated and we put forward a scheme that allows parts of the spectrum to be shifted forward in time. This is the inverse effect of coherent photon storage and may become a valuable technique if single x-ray photon wavepackets are to become the information carriers in future photonic circuits.
Synchrotron pulses will excite low lying nuclear levels, and in crystals, will create nuclear exciton states which are spatially coherent superpositions of the various excited state hyperfine levels of all the nuclei in the crystal. The subsequent radiative decay is radically affected by coherence, exhibiting both a speed-up due to "coherent enhancement", and a quantum beat modulation of the decay rate which gives a periodic speed-up/slow-down of the rate for photon decay into the coherent channels. For a nuclear exciton in an antiferromagnet, the quantum beat modulation will result in an interesting "temporal pendulösung" effect.
The time evolution of the coherent decay of the nuclear exciton induced by 14.4 keV synchrotron radiation was observed with a system of two stainless-steel resonance absorbers. In between these foils, the radiation was Bragg-scattered from a vibrating quartz crystal. The ultrasound-modulated radiation disrupts the coherent superposition of the radiation from both targets. However, at times corresponding to multiples of the ultrasound period, spikes or dips in the decay were observed which are interpreted as ultrasound-induced echoes.
The present thesis is devoted to theoretical studies of pulse propagation of light through linear and nonlinear media, and of light-induced nuclear dynamics. The first part of the thesis addresses propagation of light pulses in linear periodical media - photonic crystals. The main accent was put on studies of the angular properties of two qualitatively different types of photonic crystals: holographic photonic crystals, and impurity band based photonic crystals. The anisotropy of band structure, group velocity and pulse delay with respect to the light polarization are analyzed. In the second part of the thesis a strict theory of nonlinear propagation of a few strong interacting light beams is presented. The key idea of this approach is a self-consistent solution of the nonlinear wave equation and the density matrix equations of the material. This technique is applied to studies of dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. It is shown that interaction of co- and counter-propagating pulses of amplified spontaneous emission (ASE) affects the dynamics and efficiency of nonlinear conversion. Our dynamical theory allows to explain the asymmetric spectral properties of the forward and backward ASE pulses, which were observed in recent experiment with different dye molecules. It is shown that the ASE spectral profile changes drastically when the pump intensity approaches the threshold level. The effect of the temporal self-pulsation of ASE is studied in detail. The third part of the thesis is devoted to light-induced nuclear dynamics. Time- and frequency-resolved X-ray spectroscopy of molecules driven by strong and coherent infrared (IR) pulses shows that the phase of the IR field strongly influences the trajectory of the nuclear wave packet, and hence, the X-ray spectrum. Such a dependence arises due to the interference of one (X-ray) and two-photon (X-ray + IR) excitation channels. The phase of the light influences the dynamics also when the Rabi frequency approaches the vibrational frequency, breaking down the rotating-wave approximation. The probe X-ray spectra are also sensitive to the delay time, the duration, and the shape of the pulses. The evolution of the nuclear wave packets in the dissociative core-excited state affects the dynamics of resonant Auger scattering from fixed-in-space molecules. One of the important dynamical effects is the atomic-like resonance which experiences electronic Doppler shift. We predict that the scattering of the Auger electrons by nearby atoms leads to new Doppler shifted resonances. These extra resonances show sharp maxima in the bond directions, which makes them very promising as probes for local molecular structure using energy and angular resolved electron-ion coincidence techniques. Our theory provides prediction of several new effects, but also results that are in good agreement with the available experimental data.