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We demonstrate indirect electric-field control of ferromagnetic resonance (FMR) in devices that integrate the low-loss, molecule-based, room-temperature ferrimagnet vanadium tetracyanoethylene (V[TCNE]x∼2) mechanically coupled to PMN-PT piezoelectric transducers. Upon straining the V[TCNE]x films, the FMR frequency is tuned by more than 6 times the resonant linewidth with no change in Gilbert damping for samples with α = 6.5 × 10−5. We show this tuning effect is due to a strain-dependent magnetic anisotropy in the films and find the magnetoelastic coefficient |λs| ∼ (1–4.4) ppm, backed by theoretical predictions from density-functional theory calculations and magnetoelastic theory. Noting the rapidly expanding application space for strain-tuned FMR, we define a new metric for magnetostrictive materials, magnetostrictive agility, given by the ratio of the magnetoelastic coefficient to the FMR linewidth. This agility allows for a direct comparison between magnetostrictive materials in terms of their comparative efficacy for magnetoelectric applications requiring ultra-low loss magnetic resonance modulated by strain. With this metric, we show V[TCNE]x is competitive with other magnetostrictive materials, including YIG and Terfenol-D. This combination of ultra-narrow linewidth and magnetostriction, in a system that can be directly integrated into functional devices without requiring heterogeneous integration in a thin film geometry, promises unprecedented functionality for electric-field tuned microwave devices ranging from low-power, compact filters and circulators to emerging applications in quantum information science and technology. 

Integrating patterned, low-loss magnetic materials into microwave devices and circuits presents many challenges due to the specific conditions that are required to grow ferrite materials, driving the need for flip-chip and other indirect fabrication techniques. The low-loss (α = (3.98 ± 0.22) × 10−5), room-temperature ferrimagnetic coordination compound vanadium tetracyanoethylene (V[TCNE]x) is a promising new material for these applications that is potentially compatible with semiconductor processing. Here, we present the deposition, patterning, and characterization of V[TCNE]x thin films with lateral dimensions ranging from 1 μm to several millimeters. We employ electron-beam lithography and liftoff using an aluminum encapsulated poly(methyl methacrylate), poly(methyl methacrylate-methacrylic acid) copolymer bilayer [PMMA/P(MMA-MAA)] on sapphire and silicon. This process can be trivially extended to other common semiconductor substrates. Films patterned via this method maintain low-loss characteristics down to 25 μm with only a factor of 2 increase down to 5 μm. A rich structure of thickness and radially confined spin-wave modes reveals the quality of the patterned films. Further fitting, simulation, and analytic analysis provide an exchange stiffness, Aex = (2.2 ± 0.5) × 10−10erg/cm, as well as insights into the mode character and surface-spin pinning. Below a micron, the deposition is nonconformal, which leads to interesting and potentially useful changes in morphology. This work establishes the versatility of V[TCNE]x for applications requiring highly coherent magnetic excitations ranging from microwave communication to quantum information.