Abstract

M\"ossbauer nuclei feature exceptionally narrow resonances at hard x-ray energies, which render them ideal probes for structure and dynamics in condensed-matter systems, and a promising platform for x-ray quantum optics and fundamental tests. However, a direct spectroscopy at modern x-ray sources such as synchrotrons or x-ray free electron lasers is challenging, because of the broad spectral bandwidth of the delivered x-ray pulses, and because of a limited spectral resolution offered by x-ray optics and detectors. To overcome these challenges, here, we propose a spectroscopy technique based on a spectrally narrow reference absorber that is rapidly oscillating along the propagation direction of the x-ray light. The motion induces sidebands to the response of the absorber, which we scan across the spectrum of the unknown target to gain spectral information. The oscillation further introduces a dependence of the detected light on the motional phase at the time of x-ray excitation as an additional controllable degree of freedom. We show how a Fourier analysis with respect to this phase enables one to selectively extract parts of the recorded intensity after the actual experiment, throughout the data analysis. This allows one to improve the spectral recovery by removing unwanted signal contributions. Our method is capable of gaining spectral information from the entire measured intensity, and not only from the intensity at late times after the excitation, such that a significantly higher part of the signal photons can be used. Furthermore, it not only enables one to measure the amplitude of the spectral response, but also its phase.

Highlights

  • Spectroscopy is an indispensable tool to study matter and its dynamics

  • Starting from initial work in the visible regime, its different variants are established across vast ranges of the electromagnetic spectrum, covering many orders of magnitude on the frequency scale, and there is a continuous progress in further advancing the different spectroscopy techniques

  • The PHANTASY method is able to reconstruct the number of peaks and dips correctly, while the Doppler-drive generates spurious spectral splittings and small residual oscillations across the entire spectrum

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Summary

INTRODUCTION

Spectroscopy is an indispensable tool to study matter and its dynamics. Starting from initial work in the visible regime, its different variants are established across vast ranges of the electromagnetic spectrum, covering many orders of magnitude on the frequency scale, and there is a continuous progress in further advancing the different spectroscopy techniques. The requirement to restrict the analysis to late detection times severely reduces the part of the signal photons contributing to the recovery of the spectrum due to the nearexponential decay of the signal This method as well as most other techniques for Mössbauer nuclei only allow one to measure the magnitude of the target response, but not its phase. We put forward a spectroscopy method to characterize the amplitude and phase of the response of an unknown sample containing Mössbauer nuclei, which we denote as phase-sensitive nuclear target spectroscopy (PHANTASY) It uses a spectrally narrow reference absorber but employs oscillatory motions of the reference absorber, instead of the conventional motion with constant velocity [see Fig. 1(a)].

General setting
Response of the stationary nuclear reference analyzer
Response of the moving nuclear reference analyzer
Harmonic oscillation
Phase-sensitive single-line absorber
Sensing head approximation
Disentangling the detector signal using the φ0 filter
Disentangling the detector signal using the t filter
Reconstruction of amplitude and phase of the target’s spectral response
Fit of the experimental data
Numerical simulation
Amplitude of the target’s spectral response
Phase of the target’s spectral response
Doppler-drive spectroscopy method as a reference
Comparison of suitable integration ranges in the two methods
DISCUSSION AND SUMMARY
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