Unraveling time- and frequency-resolved nuclear resonant scattering spectra

Owing to their extremely narrow line-widths and exceptional coherence properties, Mössbauer nuclei form a promising platform for quantum optics, spectroscopy, and dynamics at energies of hard x-rays. A key requirement for further progress is the development of more powerful measurement and data analysis techniques. As one approach, recent experiments have employed time- and frequency-resolved measurements, as compared to the established approaches of measuring time-resolved or frequency-resolved spectra separately. In these experiments, the frequency-dependence is implemented using a tunable single-line nuclear reference absorber. Here, we develop spectroscopy and analysis techniques for such time- and frequency-resolved nuclear resonant scattering spectra in the frequency-frequency domain. Our approach is based on a Fourier-transform of the experimentally accessible intensities along the time axis, which results in complex-valued frequency-frequency correlation (FFC) spectra. We show that these FFC spectra not only exhibit a particularly simple structure, disentangling the different scattering contributions, but also allow one to directly access nuclear target properties and the complex-valued nuclear resonant part of the target response. In a second part, we explore the potential of an additional phase control of the x-rays resonantly scattered off of the reference absorber for our scheme. Such control provides selective access to specific scattering pathways, allowing for their separate analysis without the need to constrain the parameter space to certain frequency or time limits. All results are illustrated with pertinent examples in nuclear forward scattering and in reflection off of thin-film x-ray cavities containing thin layers of Mössbauer nuclei.