Spin resonance spectroscopy with an electron microscope

Abstract Coherent spin resonance methods, such as nuclear magnetic resonance and electron spin resonance spectroscopy, have led to spectrally highly sensitive, non-invasive quantum imaging techniques. Here, we propose a pump-probe spin resonance spectroscopy approach, designed for electron microscopy, based on microwave pump fields and electron probes. We investigate how quantum spin systems couple to electron matter waves through their magnetic moments and how the resulting phase shifts can be utilized to gain information about the states and dynamics of these systems. Notably, state-of-the-art transmission electron microscopy provides the means to detect phase shifts almost as small as that due to a single electron spin. This could enable state-selective observation of spin dynamics on the nanoscale and indirect measurement of the environment of the examined spin systems, providing information, for example, on the atomic structure, local chemical composition and neighboring spins.