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Quantum information science and engineering requires novel low-loss magneticmaterials for magnon-based quantum-coherent operations. The search for low-lossmagnetic materials, traditionally driven by applications in microwaveelectronics near room-temperature, has gained additional constraints from theneed to operate at cryogenic temperatures for many applications in quantuminformation science and technology. Whereas yttrium iron garnet (YIG) has beenthe material of choice for decades, the emergence of molecule-based materialswith robust magnetism and ultra-low damping has opened new avenues forexploration. Specifically, thin-films of vanadium tetracyanoethylene (V[TCNE]x)can be patterned into the multiple, connected structures needed for hybridquantum elements and have shown room-temperature Gilbert damping ({\alpha} = 4\times 10^-5) that rivals the intrinsic (bulk) damping otherwise seen only inhighly-polished YIG spheres (far more challenging to integrate into arrays).Here, we present a comprehensive and systematic study of the low-temperaturemagnetization dynamics for V[TCNE]x thin films, with implications for theirapplication in quantum systems. These studies reveal a temperature-driven,strain-dependent magnetic anisotropy that compensates the thin-film shapeanisotropy, and the recovery of a magnetic resonance linewidth at 5 K that iscomparable to room-temperature values (roughly 2 G at 9.4 GHz). We can accountfor these variations of the V[TCNE]x linewidth within the context of scatteringfrom very dilute paramagnetic impurities, and anticipate additional linewidthnarrowing as the temperature is further reduced.

Exploring a quantum-information-relevant magnonic material: Ultralow damping at low temperature in the organic ferrimagnet V[TCNE]x