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arXiv:2510.00970

Cumulant expansion approach to the decay dynamics of interacting Mössbauer nuclei after strong impulsive excitation

Miriam Gerharz, Jörg Evers

Published Oct 1, 2025• 0 citations
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Abstract

Recent progress in accelerator-based x-ray sources brings higher excitation of ensembles of Mössbauer nuclei closer to experimental feasibility. Yet, a theoretical modeling of the decay dynamics of the interacting nuclear ensemble after the impulsive excitation is still an open challenge. Here, we derive a set of nonlinear equations which is capable of efficiently modeling large nuclear ensembles for arbitrary degrees of excitation. As key signature for higher excitation, we identify a non-linear time-evolution of the nuclear dipole phase, which can be tuned via the scattering geometry, and interferometrically be measured. Furthermore, we identify interesting finite-size effects in the nuclear dynamics of small ensembles. Our results provide important guidance for future experiments aiming at the non-linear excitation of nuclei. We further envision the exploration of finite size-effects in Mössbauer spectroscopy with highest spatial resolution, i.e., small sample volumes.

DOI
10.48550/arxiv.2510.00970

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Recent progress in accelerator-based x-ray sources brings higher excitation of ensembles of Mössbauer nuclei closer to experimental feasibility. Yet, a theoretical modeling of the decay dynamics of the interacting nuclear ensemble after the impulsive excitation is still an open challenge. Here, we derive a set of nonlinear equations which is capable of efficiently modeling large nuclear ensembles for arbitrary degrees of excitation. As key signature for higher excitation, we identify a non-linear time-evolution of the nuclear dipole phase, which can be tuned via the scattering geometry, and interferometrically be measured. Furthermore, we identify interesting finite-size effects in the nuclear dynamics of small ensembles. Our results provide important guidance for future experiments aiming at the non-linear excitation of nuclei. We further envision the exploration of finite size-effects in Mössbauer spectroscopy with highest spatial resolution, i.e., small sample volumes.
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Up to now, experiments involving Mössbauer nuclei driven by x-rays have been restricted to the low-excitation regime. Here, a setup is proposed which promises significant excitation, ideally exceeding full inversion of the nuclear ensemble, at x-ray light sources under construction. We further introduce a method to experimentally verify such inversions, in which population inversions manifest themselves in symmetry flips of suitably recorded spectra. It neither requires per-shot spectra of the incoming x-ray pulses, nor absolute measurements of the scattered light intensity.
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In the study of optical properties of large atomic systems, a weak laser driving is often assumed to simplify the system dynamics by linearly coupled equations. Here we investigate the light-scattering properties of atomic ensembles beyond weak-field excitation through the cumulant expansion method. By progressively incorporating higher-order correlations into the steady-state equations, an enhanced accuracy can be achieved in comparison to the exact solutions obtained by solving a full density matrix. Our analysis reveals that, in the regime of weak dipole-dipole interaction, the first-order expansion yields satisfactory predictions for optical depth, while denser atomic configurations necessitate consideration of higher-order correlations. As the intensity of incident light increases, atom saturation effects become noticeable, giving rise to significant changes in light transparency, energy shift, and decay rate. This saturation phenomenon extends to subradiant atom arrays even under weak driving conditions, leading to substantial deviations from the linear model. Our findings demonstrate that the mean-field model is a good extension to linear models as it balances both accuracy and computational complexity. However, the crucial role of higher-order cumulants in large and dense atom systems remains unclear, since it is challenging theoretically owing to the exponentially increasing Hilbert space in such light-matter interacting systems.
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.
Abstract Mössbauer nuclei with quadrupole-split levels provide a versatile platform for exploring coherent x-ray light-matter interactions. We theoretically study ensembles of 57 Fe nuclei embedded in thin-film x-ray cavities, explicitly accounting for different orientations of the electric field gradient. By mapping isotropic electric field gradient distributions to an effective equal-weight two-transition model, we derive analytical expressions for the time-dependent reflectivity and reveal the emergence of cavity-mediated quantum beats. The oscillation frequency and temporal profile of these beats can be tuned via the cavity-induced coherent coupling, offering a flexible approach to control collective nuclear dynamics and manipulate nuclear coherence in the x-ray regime.