The In Situ Optimization of Spinterface in Polymer Spin Valve by Electronic Phase Separated Oxides

Tailoring the interface between organic semiconductor (OSC) and ferromagnetic (FM) electrodes, that is, the spinterface, offers a promising way to manipulate and optimize the magnetoresistance (MR) ratio of the organic spin valve (OSV) devices. However, the non-destructive in situ regulation method of spinterface is seldom reported, limiting its theoretical research and further application in organic spintronics. (La_2/3 Pr_1/3 )_5/8 Ca_3/8 MnO₃ (LPCMO), a recently developed FM material, exhibits a strong electronic phase separation (EPS) property, and can be employed as an effective in situ spinterface adjuster. Herein, we fabricated a LPCMO-based polymer spin valve with a vertical configuration of LPCMO/poly(3-hexylthiophene-2,5-diyl) (P3HT)/Co, and emphasized the important role of LPCMO/P3HT spinterface in MR regulation. A unique competitive spin-scattering mechanism generated by the EPS characteristics of LPCMO inside the polymer spin valve was discovered by abstracting the anomalous non-monotonic MR value as a function of pre-set magnetic field (B_pre ) and temperature (T). Particularly, a record-high MR ratio of 93% was achieved in polymer spin valves under optimal conditions. These findings highlight the importance of interdisciplinary research between organic spintronics and EPS oxides and offer a novel scenario for multi-level storage via spinterface manipulation.