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Hard X-ray quantum optics in thin-film nanostructures

Johann Haber

Published May 12, 2017• 1 citation
Publisher

Abstract

This thesis describes quantum optical experiments with x-rays with the aim of reaching the strong-coupling regime of light and matter. We make use of the interaction which arisesbetween resonant matter and x-rays in specially designed thin-film nanostructures which form x-ray cavities. Here, the resonant matter are Tantalum atoms and the Iron isotope $^{57}$Fe. Both limit the number of modes available to the resonant atoms for interaction, and enhances the interaction strength. Thus we have managed to observe a number of phenomena well-known in quantum optics, which are the building blocks for sophisticated applications in e.g. metrology. Among these are the strong coupling of light and matter and the concurrent exchange of virtual photons, often called Rabi oscillations. Furthermore we have designed and tested a type of cavity hitherto unused in x-ray optics. Finally, we develop a new method for synchrotron Mössbauer spectroscopy, which not only promises to yield high-resolution spectra, but also enables the retrieval of the phase of the scattered light. The results open new avenues for quantum optical experiments with x-rays, particularly with regards to the ongoing development of high-brilliance x-ray free-electron lasers.

DOI
10.3204/pubdb-2017-02595

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This thesis describes quantum optical experiments with x-rays with the aim of reaching the strong-coupling regime of light and matter. We make use of the interaction which arisesbetween resonant matter and x-rays in specially designed thin-film nanostructures which form x-ray cavities. Here, the resonant matter are Tantalum atoms and the Iron isotope 57^{57}57Fe. Both limit the number of modes available to the resonant atoms for interaction, and enhances the interaction strength. Thus we have managed to observe a number of phenomena well-known in quantum optics, which are the building blocks for sophisticated applications in e.g. metrology. Among these are the strong coupling of light and matter and the concurrent exchange of virtual photons, often called Rabi oscillations. Furthermore we have designed and tested a type of cavity hitherto unused in x-ray optics. Finally, we develop a new method for synchrotron Mössbauer spectroscopy, which not only promises to yield high-resolution spectra, but also enables the retrieval of the phase of the scattered light. The results open new avenues for quantum optical experiments with x-rays, particularly with regards to the ongoing development of high-brilliance x-ray free-electron lasers.
A promising platform for the emerging field of x-ray quantum optics consists of M\"ossbauer nuclei embedded in thin-film cavities probed by near-resonant x-ray light, as used in a number of recent experiments. Here we develop a quantum optical framework for the description of experimentally relevant settings involving nuclei embedded in x-ray waveguides. We apply our formalism to two settings of current experimental interest based on the archetype M\"ossbauer isotope 57{}^{57}57Fe. For the present experimental conditions, we derive compact analytical expressions and show that the alignment of medium magnetization, as well as incident and detection polarization, enable the engineering of advanced quantum optical level schemes. The model encompasses nonlinear and quantum effects which could become accessible in future experiments.
In this thesis thin-film cavities with embedded Mössbauer nuclei probed by near-resonant x-ray light are studied from a quantum optical perspective. A theoretical framework is developed and compact expressions for the observables are derived for the linear excitation regime, which is encountered in current experiments. Even advanced cavity layouts can be modeled in excellent agreement with the results of previous experiments and semi-classical approaches. In the absence of magnetic hyperfine splitting, the spectral response of the system is found to be formed by tunable Fano profiles. An experimental implementation of this line shape control allows to extract spectroscopic signatures with high precision and to reconstruct the phase of the nuclear transition in good agreement with the theoretical predictions. The alignment of medium magnetization and polarization control of the x-rays enable to engineer advanced quantum optical level schemes, in which vacuum induced coherence effects are predicted and successfully demonstrated in an experiment. Furthermore, it is shown that group velocity control for x-ray pulses can be achieved in the cavity. A scheme for its observation is proposed and then employed to experimentally confirm sub-luminal x-ray propagation. Finally, non-linear effects, which could become accessible with future light sources, are explored and a non-linear line shape control mechanism is discussed.
Thin-film cavities containing layers of M\"ossbauer nuclei have been demonstrated to be a rich platform for x-ray quantum optics. At low excitation, these systems can be described by effective few-level schemes, thereby providing tunable artificial quantum systems at hard x-ray energies. With the recent advent of an ab initio theory, a numerically efficient description of these systems is now possible. On this basis, we introduce the inverse design and develop a comprehensive optimization for an archetypal system with a single resonant layer, corresponding to an artificial two-level scheme. We discover a number of qualitative insights into x-ray photonic environments for nuclei that will likely impact the design of future x-ray cavities and thereby improve their performance. The methods presented readily generalize beyond the two-level case and thus provide a clear perspective towards the inverse design of more advanced tunable x-ray quantum optical level schemes.
The resonant interaction between x-ray photons and nuclei is one of the most exciting subjects in the burgeoning field of x-ray quantum optics. A resourceful platform used to date is thin-film x-ray cavities with embedded layers or M\"ossbauer nuclei such as 57Fe^{57}\mathrm{Fe}57Fe. A quantum optical model based on the classical electromagnetic Green's function is developed to investigate theoretically the nuclear response inside the x-ray cavity. The model is versatile and provides an intuitive picture about the influence of the cavity structure on the resulting spectra. We test its predictive powers with the help of the semiclassical coherent scattering formalism simulations and discuss our results on increasing complexity of layer structures.
Abstract The increase in the brightness of modern synchrotron radiation sources and X-ray free-electron lasers have made it possible to observe nonlinear and quantum-optical phenomena for X rays. The peak intensity after focusing with application of bent crystals is as high as 1020 W/cm2 for modern sources and exceeds that characteristic of intraatomic fields. X-ray detectors with close-to-unity quantum efficiency and resolution in number of photons have become available. This provided prerequisites for studying fundamental concepts of quantum optics in the X-ray region of the electromagnetic spectrum.
This thesis is dedicated to the study of collective effects of nuclei in single xray photon superradiance. To this end we investigate aspects of superradiance in both nuclear forward scattering and in thin-film cavities with an embedded 57Fe nuclear layer. A general theoretical framework is developed to investigate a single-photon cooperative emission from a cloud of resonant systems, atoms or nuclei, in the presence of magnetic hyperfine splitting. In the limit of a thick sample, we present our results for two means to coherently control the collective single x-ray photon emission in nuclear forward scattering. In the limit of a thin sample in a thin-film cavity with embedded resonant nuclei, we find out that unlike the magnetic hyperfine splitting of a single atom or nucleus, interesting collective effects may occur which modify the hyperfine level structure. In addition, for a certain parameter regime a spectrum reminiscent of electromagnetically induced transparency (EIT) can be achieved. Based on this EIT-like effect, a theoretical control mechanism for stopping x-ray pulses in the thin-film x-ray cavity is put forward. Finally, we show theoretically that for the case of two nuclear ensembles in the thin-film cavity, pseudo-Rabi splitting due to the strong coupling between the two layers should occur. The latter findings are confirmed by preliminary experimental data.