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Single-molecule magnets (SMMs) are pivotal in molecular spintronics, showing unique quantum behaviors that can advance spin-based technologies. By incorporating SMMs into magnetic tunnel junctions (MTJs), new possibilities emerge for low-power, energy-efficient data storage, memory devices and quantum computing. This study explores how SMMs influence spin-dependent transport in antiferromagnet-based MTJ molecular spintronic devices (MTJMSDs). We fabricated cross-junction MTJ devices with an antiferromagnetic Ta/FeMn bottom electrode and ferromagnetic NiFe/Ta top electrode, with a ∼2 nm AlOx layer, designed so that the AlOx barrier thickness at the junction intersection matched the SMM length, allowing them to act as spin channels bridging the two electrodes. Following SMM treatment, the MTJMSDs exhibited significant current enhancement, reaching a peak of 40 μA at 400 mV at room temperature. In contrast, bare MTJ junctions experienced a sharp current reduction, falling to the pA range at 0°C and remaining stable at lower temperatures—a suppression notably greater than in SMM-treated samples (Ref: Sankhi et al., Journal of Magnetism and Magnetic Materials, p. 172608, 2024). Additional vibration sample magnetometry on pillar shaped devices of same material stacks indicated a slight decrease in magnetic moment after incorporating SMMs, suggesting an effect on magnetic coupling of molecule with electrodes. Overall, this work highlights the promise of antiferromagnetic materials in optimizing MTJMSD devices and advancing molecular spintronics. 

The single-molecule magnet (SMM) is demonstrated here to transform conventional magnetic tunnel junctions (MTJ), a memory device used in present-day computers, into solar cells. For the first time, we demonstrated an electronic spin-dependent solar cell effect on an SMM-transformed MTJ under illumination from unpolarized white light. We patterned cross-junction-shaped devices forming a CoFeB/MgO/CoFeB-based MTJ. The MgO barrier thickness at the intersection between the two exposed junction edges was less than the SMM extent, which enabled the SMM molecules to serve as channels to conduct spin-dependent transport. The SMM channels yielded a region of long-range magnetic ordering around these engineered molecular junctions. Our SMM possessed a hexanuclear [Mn6(μ3-O)2(H2N-sao)6(6-atha)2(EtOH)6] [H2N-saoH = salicylamidoxime, 6-atha = 6-acetylthiohexanoate] complex and thiols end groups to form bonds with metal films. SMM-doped MTJs were shown to exhibit a solar cell effect and yielded ≈ 80 mV open-circuit voltage and ≈ 10 mA/cm2 saturation current density under illumination from one sun equivalent radiation dose. A room temperature Kelvin Probe AFM (KPAFM) study provided direct evidence that the SMM transformed the electronic properties of the MTJ's electrodes over a lateral area in excess of several thousand times larger in extent than the area spanned by the molecular junctions themselves. The decisive factor in observing this spin photovoltaic effect is the formation of SMM spin channels between the two different ferromagnetic electrodes, which in turn is able to catalyze the long-range transformation in each electrode around the junction area. 

A device architecture utilizing a single-molecule magnet (SMM) as a device element between two ferromagnetic electrodes may open vast opportunities to create novel molecular spintronics devices. Here, we report a method of connecting an SMM to the ferromagnetic electrodes. We utilized a nickel (Ni)–AlO x –Ni magnetic tunnel junction (MTJ) with the exposed side edges as a test bed. In the present work, we utilized an SMM with a hexanuclear [Mn 6 (μ 3 -O) 2 (H 2 N-sao) 6 (6-atha) 2 (EtOH) 6 ] [H 2 N-saoH = salicylamidoxime, 6-atha = 6-acetylthiohexanoate] complex that is attached to alkane tethers terminated with thiols. These Mn-based molecules were electrochemically bonded between the two Ni electrodes of an exposed-edge tunnel junction, which was produced by the lift-off method. The SMM-treated MTJ exhibited current enhancement and transitory current suppression at room temperature. Monte Carlo simulation was utilized to understand the transport properties of our molecular spintronics device.