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Spintronic, spin caloritronic, and magnonic phenomena arise from complexinteractions between charge, spin, and structural degrees of freedom that arechallenging to model and even more difficult to predict. This situation iscompounded by the relative scarcity of magnetically-ordered materials withrelevant functionality, leaving the field strongly constrained to work with ahandful of well-studied systems that do not encompass the full phase space ofphenomenology predicted by fundamental theory. Here we present an importantadvance in this coupled theory-experiment challenge, wherein we extend existingtheories of the spin Seebeck effect (SSE) to explicitly include thetemperature-dependence of magnon non-conserving processes. This expanded theoryquantitatively describes the low-temperature behavior of SSE signals previouslymeasured in the mainstay material yttrium iron garnet (YIG) and predicts a newregime for magnonic and spintronic materials that have low saturationmagnetization, $M_S$, and ultra-low damping. Finally, we validate thisprediction by directly observing the spin Seebeck resistance (SSR) in themolecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene(V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yieldingSSR signals comparable in magnitude to YIG and extracted magnon diffusionlength ($\lambda_m>1$ $\mu$ 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 relativelylow spin wave stiffness (exchange). This identification of a new regime forhighly efficient SSE-active materials opens the door to a new class of magneticmaterials for spintronic and magnonic applications.

Magnon Diffusion Length and Longitudinal Spin Seebeck Effect in Vanadium Tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$)