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The molecular-based ferrimagnetic insulator V(TCNE)x has gained recent interest for efficient spin-wave excitation due to its low Gilbert damping ratio a=4E-5, and narrow ferromagnetic resonance linewidth f=1Oe. Here we report a clean spin pumping signal detected on V(TCNE)x/metal bilayer structures, free from spin rectification or thermal artifacts. On-chip coupling of microwave power is achieved via a coplanar waveguide to measure the in-plane angle-dependence of the inverse spin-Hall effect under ferromagnetic resonance conditions with respect to a constant external magnetic field. A signature of pure spin current from V(TCNE)x is observed in both platinum and permalloy metal layers, demonstrating the utility of V(TCNE)x for magnon spintronics studies in molecule/solid-state heterostructures., Comment: Need to add more simulation results on EM coupling

Spintronic, spin caloritronic, and magnonic phenomena arise from complex interactions between charge, spin, and structural degrees of freedom that are challenging to model and even more difficult to predict. This situation is compounded by the relative scarcity of magnetically-ordered materials with relevant functionality, leaving the field strongly constrained to work with a handful of well-studied systems that do not encompass the full phase space of phenomenology predicted by fundamental theory. Here we present an important advance in this coupled theory-experiment challenge, wherein we extend existing theories of the spin Seebeck effect (SSE) to explicitly include the temperature-dependence of magnon non-conserving processes. This expanded theory quantitatively describes the low-temperature behavior of SSE signals previously measured in the mainstay material yttrium iron garnet (YIG) and predicts a new regime for magnonic and spintronic materials that have low saturation magnetization, $M_S$, and ultra-low damping. Finally, we validate this prediction by directly observing the spin Seebeck resistance (SSR) in the molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yielding SSR signals comparable in magnitude to YIG and extracted magnon diffusion length ($\lambda_m>1$ $\mu$ m) and magnon lifetime for V[TCNE]$_x$ ($\tau_{th}\approx 1-10$ $\mu$ s) exceeding YIG ($\tau_{th}\sim 10$ ns). Surprisingly, these properties persist to room temperature despite relatively low spin wave stiffness (exchange). This identification of a new regime for highly efficient SSE-active materials opens the door to a new class of magnetic materials for spintronic and magnonic applications.

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]$_{x \sim 2}$) 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 $\alpha = 6.5 \times 10^{-5}$. We show this tuning effect is due to a strain-dependent magnetic anisotropy in the films and find the magnetoelastic coefficient $|\lambda_S| \sim (1 - 4.4)$ ppm, backed by theoretical predictions from DFT calculations and magnetoelastic theory. Noting the rapidly expanding application space for strain-tuned FMR, we define a new metric for magnetostrictive materials, $\textit{magnetostrictive agility}$, 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.

Quantum information science and engineering requires novel low-loss magnetic materials for magnon-based quantum-coherent operations. The search for low-loss magnetic materials, traditionally driven by applications in microwave electronics near room-temperature, has gained additional constraints from the need to operate at cryogenic temperatures for many applications in quantum information science and technology. Whereas yttrium iron garnet (YIG) has been the material of choice for decades, the emergence of molecule-based materials with robust magnetism and ultra-low damping has opened new avenues for exploration. Specifically, thin-films of vanadium tetracyanoethylene (V[TCNE]x) can be patterned into the multiple, connected structures needed for hybrid quantum elements and have shown room-temperature Gilbert damping ({\alpha} = 4 \times 10^-5) that rivals the intrinsic (bulk) damping otherwise seen only in highly-polished YIG spheres (far more challenging to integrate into arrays). Here, we present a comprehensive and systematic study of the low-temperature magnetization dynamics for V[TCNE]x thin films, with implications for their application in quantum systems. These studies reveal a temperature-driven, strain-dependent magnetic anisotropy that compensates the thin-film shape anisotropy, and the recovery of a magnetic resonance linewidth at 5 K that is comparable to room-temperature values (roughly 2 G at 9.4 GHz). We can account for these variations of the V[TCNE]x linewidth within the context of scattering from very dilute paramagnetic impurities, and anticipate additional linewidth narrowing as the temperature is further reduced., Comment: The first two authors contributed equally

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 ($\alpha = 3.98 \pm 0.22 \times 10^{-5}$), room-temperature ferrimagnetic coordination compound vanadium tetracyanoethylene ($\mathrm{V[TCNE]}_x$) is a promising new material for these applications that is potentially compatible with semiconductor processing. Here we present the deposition, patterning, and characterization of $\mathrm{V[TCNE]}_x$ thin films with lateral dimensions ranging from 1 micron 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 microns with only a factor of 2 increase down to 5 microns. A rich structure of thickness and radially confined spin-wave modes reveals the quality of the patterned films. Further fitting, simulation, and analytic analysis provides an exchange stiffness, $A_{ex} = 2.2 \pm 0.5 \times 10^{-10}$ erg/cm, as well as insights into the mode character and surface spin pinning. Below a micron, the deposition is non-conformal, which leads to interesting and potentially useful changes in morphology. This work establishes the versatility of $\mathrm{V[TCNE]}_x$ for applications requiring highly coherent magnetic excitations ranging from microwave communication to quantum information., Comment: 18 pages, 7 figures, submitted to APL Materials