X-ray/Extreme Ultraviolet Floquet State Multidimensional Spectroscopy, an Analogue of Multiple Quantum Nuclear...

There is great interest in developing fully coherent multidimensional X-ray/extreme ultraviolet (XUV) spectroscopic techniques because of their capability for achieving atomic spectral selectivity. Current proposals rest on using sequentially and coherently driven core excitations with multiple X-ray/XUV excitation pulses and measuring the output using time domain Fourier transform methods. In this paper, we propose an alternative method that creates an entanglement of core and optical transitions to form a Floquet state that creates directional and coherent output beams. Multidimensional spectra are obtained by measuring the intensity of output beams while tuning the optical frequencies across resonances. This approach expands on previous optical pump-XUV probe spectroscopy of MoTe₂ by theoretically demonstrating its multidimensional capabilities. Both parametric and non-parametric pathways are proposed to optimize the resolution of inhomogeneous broadening and k-selective features.