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We demonstrate interface energy level engineering, exploiting themodification in energy band structure across Verwey phase transition of$Fe_{3}O_{4}$ electrode, in a $Fe_{3}O_{4}$(111)/$Alq_{3}$/Co verticalspin-valve (SV) device. Experimental results on device characteristics I-V)study exhibit a transition in conduction mode from carrier injection totunneling across Verwey transition temperature ($T_{V}$) of $Fe_{3}O_{4}$electrode. Both giant magneto-resistance (GMR) and tunneling MR (TMR) have beenobserved in a single SV device as a function of temperature, below and above$T_{V}$, respectively. Appearance of GMR, accompanied by injection limitednatural Schottky-like I-V characteristics, provide evidences of spin injectionat electrode/$Alq_{3}$ interface and transport through molecular orbitals inthis SV device. Features of TMR exhibit significant differences from that ofGMR. This is due to the dominant hyperfine-field interaction in the multi-steptunneling regime. We have achieved room-temperature SV operation in our device.A phenomenological model for device operation has been proposed to explain thetransition in the conduction mode and associated MR features across $T_{V}$. Wepropose that the tuning of charge gap at Fermi level across Verwey transitiondue to charge ordering on the octahedral iron sites of $Fe_{3}O_{4}$ results ina corresponding tuning of conduction mode causing this unique cross over fromGMR to TMR in this ferrite-based organic SV.

Crossover from injection to tunneling conduction mode and associated  magneto-resistance in a single $Fe_{3}O_{4}$(111)/$Alq_{3}$/Co spin-valve  device