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arXiv:2403.06508 · Physical Review Letters

Collective Nuclear Excitation and Pulse Propagation in Single-Mode X-Ray Waveguides

Leon Merten Lohse, Petar Andrejić, Sven Velten, Malte Vassholz, Charlotte Neuhaus, Ankita Negi, Anjali Panchwanee, I. Sergueev, Adriana Pálffy, Tim Salditt, Ralf Röhlsberger

Published Jun 27, 2025• 2 citations
arXivHTMLPDF

Abstract

Waveguides offer a means to controllably couple atomic ensembles to the electromagnetic field therein. Here, we demonstrate x-ray propagation in planar thin-film waveguides coupled to Mössbauer nuclei under collective resonant excitation by short pulses of synchrotron radiation. We record x-ray photons that have been emitted into resonant modes of the waveguide. Depending on the geometry and mode of excitation, two fundamentally different signatures of the collective emission are observed, for which we present a unifying theoretical model. Our results form a new platform for waveguide quantum electrodynamics in the hard x-ray regime with the potential to provide a coherent narrow band source of x-rays on the nanometer scale.

DOI
10.1103/r2hf-9qn9

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Waveguides offer a means to controllably couple atomic ensembles to the electromagnetic field therein. Here, we demonstrate x-ray propagation in planar thin-film waveguides coupled to Mössbauer nuclei under collective resonant excitation by short pulses of synchrotron radiation. We record x-ray photons that have been emitted into resonant modes of the waveguide. Depending on the geometry and mode of excitation, two fundamentally different signatures of the collective emission are observed, for which we present a unifying theoretical model. Our results form a new platform for waveguide quantum electrodynamics in the hard x-ray regime with the potential to provide a coherent narrow band source of x-rays on the nanometer scale.
Abstract The narrow nuclear resonances of Mössbauer isotopes constitute almost ideal two‐level systems to study cooperative effects in the interaction of x‐rays with matter. Embedding an ensemble of resonant Mössbauer nuclei into a planar cavity facilitates the excitation of superradiant oscillatory eigenmodes via pulses of synchrotron radiation. These modes exhibit a large collective Lamb shift that can be controlled via the excitation conditions and the cavity geometry. Cooperative emission in connection with the radiative coupling of two resonant ensembles in a cavity leads to electromagnetically induced transparency (EIT). This contribution gives a review on cooperative effects in nuclear resonant scattering of synchrotron radiation. Special emphasis is given to the basic principles of recent experiments that led to the observation of the collective Lamb shift and EIT with nuclear resonances in the regime of hard x‐rays.
We have investigated the spontaneous radiative decay of resonant nuclei in a planar x-ray waveguide after excitation by synchrotron radiation pulses. The waveguide acts as a cavity and modifies the mode structure of the electromagnetic field. As a result, the rate of spontaneous emission is enhanced by a factor proportional to the density of photon states in the cavity. In this experiment, we have observed a sixfold acceleration of the coherent radiative decay of 57Fe nuclei located in the center of the first-order guided mode. This is in very good agreement with theoretical predictions.
Thin-film nanostructures with embedded M\"ossbauer nuclei have been successfully used for x-ray quantum optical applications with hard x-rays coupling in grazing incidence. Here we address theoretically an alternative geometry, in which hard x rays are coupled in forward incidence (front coupling), setting the stage for waveguide QED with nuclear x-ray resonances. We present in a self-contained manner a general model based on the Green's function formalism of the field-nucleus interaction in one-dimensional waveguides and show that it combines aspects of both nuclear forward scattering, visible as dynamical beating in the spatiotemporal response, and the resonance structure from grazing incidence, visible in the spectrum of guided modes. The interference of multiple modes is shown to play an important role, resulting in beats with wavelengths on the order of tens of micrometers, on the scale of practical photolithography. This allows for the design of special sample geometries to explore the resonant response or microstriped waveguides, opening a toolbox of geometrical design for hard x-ray quantum optics.
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.
Current implementations of quantum batteries are constrained by limited energy density and short retention times associated with the electronic or molecular excitations. Here we propose a nuclear quantum battery based on collective excitation of the 57^{57}57Fe nuclei of density nnn embedded in a planar hard X-ray waveguide. Using a Green function waveguide-QED description, we study charging via excitation beyond linear response, where saturation and drive back-action reshape the incident pulse. We introduce a self-consistent waveform-engineering protocol that inhibits local radiative decay in the waveguide thus promoting absorption into high-lying collective nuclear excitation manifolds. We show an enhanced excitation cross section of the nuclear ensemble which yields superlinear charging, with maximum studied energy density scaling approximately like nnn \sqrt{n}nn​. Our results provide a route to high-energy-density quantum charging at hard X-ray energies using contemporary X-ray sources and waveguide architectures by identifying nonlinear, collectively enhanced absorption as a key mechanism for nuclear quantum battery operation.
Up to now, experiments involving M\"ossbauer nuclei have been restricted to the low-excitation regime (LER). The reason for this is the narrow spectral linewidth of the nuclei. This defining feature enables M\"ossbauer spectroscopy with remarkable resolution and convenient control and measurements in the time domain, but at the same time implies that only a tiny part of the photons delivered by accelerator-based x-ray sources with orders-of-magnitude larger pulse bandwidth are resonant with the nuclei. X-ray free-electron lasers promise a substantial enhancement of the number of nuclear-resonant photons per pulse, such that excitations beyond the LER come within reach. This raises the question of how the onset of nonlinear excitations could be experimentally verified. Here, we develop and explore a method to detect an excitation of nuclear ensembles beyond the LER for ensembles of nuclei embedded in x-ray waveguides. It relies on the comparison of the x rays coherently and incoherently scattered off of the nuclei. As a key result, we show that the ratio of the two observables is constant within the LER, essentially independent of the details of the nuclear system and the characteristics of the exciting x rays. Conversely, deviations from this equivalence serve as a direct indication of excitations beyond the LER. Building upon this observation, we develop a variety of experimental signatures both, for near-instantaneous impulsive and for temporally extended nonimpulsive x-ray excitation. Correlating coherently and incoherently scattered intensities further allows one to compare theoretical models of nonlinear excitations more rigorously to corresponding experiments.