Temperature‐Dependent Spinterface‐Induced Cross‐Zero‐Field Magnetoresistance Shift in Organic Spin Valve for Spin Logic

ABSTRACT Organic spintronics exploits the spin degree of freedom in molecular and π‐conjugated systems for information processing, with the spinterface now recognized as key to spin injection and detection. However, intrinsic and in situ control of electrode‐molecular spinterface remains challenging. Decoupling the two electrode‐molecular spinterfaces to enable independent interfacial operation provides a promising route toward enhanced functionality in spintronic devices. Here, we present an interface‐stabilized organic spin valve (OSV) with programmable logic function, in which the two spinterfaces are successfully decoupled; one is highly reproducible and stable while another remains tunable. The device combines the temperature‐dependent organic‐ Ni 80 Fe 20 (NiFe) spinterface and the pronounced anisotropic magnetoresistance (AMR) from the NiFe electrode. The overall magnetoresistance (MR) is governed by the interplay between interfacial spin‐dependent polarization and AMR. As the temperature increases from 10 to 50 K, the MR peak continuously shifts and finally misaligns. The calculation and simulation results attribute this to the temperature‐dependent reconfiguration of the spinterface. Using temperature and magnetic field as independent inputs, reconfigurable logic truth tables can be implemented within a single device. This platform establishes a robust, defect‐free architecture for probing spin transport mechanisms and realizing compact, multifunctional spin‐logic elements in molecular electronics.