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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 (Alq 3 )-based organic spin valves (OSVs) using La 0.67 Sr 0.33 MnO 3  as a magnetic electrode. Here we demonstrate that one type of perovskite manganites, i.e., a (La 2/3 Pr 1/3 ) 5/8 Ca 3/8 MnO 3  thin film with pronounced electronic phase separation (EPS), can be used in Alq 3 -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.

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