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Element-specific magnetism accessible by synchrotron-based X-ray spectroscopy has proven to be valuable to study spin and orbital moments of transition metals and lanthanides in technologically relevant thin-film and monolayer samples. The access to coherent spin superposition states relevant for emergent quantum technologies remains, however, elusive with ordinary X-ray spectroscopy. Here, we approach the study of such quantum-coherent states via the X-ray detection of microwave-driven electron paramagnetic resonance, which involves much smaller signal levels than X-ray detected ferromagnetic resonance on classical magnets. We demonstrate the feasibility of this approach with thin films of phthalocyanine-based metal complexes containing copper or vanadium centers. We also identify X-ray specific phenomena that we relate to charge trapping of secondary electrons resulting from the decay of the X-ray excited core-hole state. Our findings pave the way toward the element-specific X-ray detection of coherent superposition states in monolayers of atomic and molecular spins on virtually arbitrary surfaces.
Tobias Kippenberg, Rui Ning Wang, Arslan Sajid Raja, Guanhao Huang, Zheru Qiu, Alexey Tikan, Aleksandr Tusnin, Yujia Yang