An Ultrasensitive Molecular Detector for Direct Sensing of Spin Currents at Room Temperature

The experimental analysis of pure spin currents at interfaces is one major goal in the field of magnonics and spintronics. Complementary to the established Spin-Hall effect using the spin-to-charge conversion in heavy metals for information processing, we present a novel approach based on spin pumping detection by an interfacial, resonantly excited molecular paramagnet adsorbed to the surface of the spin current generating magnet. Here, we show that the sensitivity of this electron paramagnetic resonance (EPR) detector can be enhanced by orders of magnitude through intramolecular transfer of spin polarization at room temperature. Our proof-of-principle sample consists of octahedral-shaped ferrimagnetic Fe₃O₄ nanoparticles covered by oleic acid (OA) which has two paramagnetic centers, S1 and S2. S1 arises from the chemisorption of OA and is located directly at the interface to Fe₃O₄. S2 originates from radical formation at the center of the molecule close to the double bond of oleic acid and is not influenced by chemisorption. Using ferromagnetic resonance (FMR) excitation of the Fe₃O₄ nanoparticles to pump spins into S1, a population inversion of the spin-split levels of S2 is formed, vastly enhancing the detection sensitivity on the atomic scale.