Achieving large and nonvolatile tunable magnetoresistance in organic spin valves using electronic phase separated manganites

Tailoring molecular spinterface between novel magnetic materials and organic semiconductors offers promise to achieve high spin injection efficiency. Yet it has been challenging to achieve simultaneously a high and nonvolatile control of magnetoresistance effect in organic spintronic devices. To date, the largest magnetoresistance (~300% at T = 10 K) has been reached in tris-(8-hydroxyquinoline) aluminum (Alq3)-based organic spin valves (OSVs) using La0.67Sr0.33MnO3 as a magnetic electrode. Here we demonstrate that one type of perovskite manganites, i.e., a (La2/3Pr1/3)5/8Ca3/8MnO3 thin film with pronounced electronic phase separation (EPS), can be used in Alq3-based OSVs to achieve a large magnetoresistance (MR) up to 440% at T = 10 K and a typical electrical Hanle effect as the Hallmark of the spin injection. The contactless magnetic field-controlled EPS enables us to achieve a nonvolatile tunable MR response persisting up to 120 K. Our study suggests a new route to design high performance multifunctional OSV devices using electronic phase separated manganites.