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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. 

Abstract In this study, a novel deposition technique that utilizes diethylzinc (C₄H₁₀ZnO) with H₂O to form a ZnO adhesion layer was proposed. This technique was followed by the deposition of vaporized nickel(II) 1-dimethylamino-2-methyl-2-butoxide (Ni(dmamb)₂) and H₂gas to facilitate the deposit of uniform layers of nickel on the ZnO adhesion layer using atomic layer deposition. Deposition temperatures ranged from 220 to 300 °C. Thickness, composition, and crystallographic structure results were analyzed using spectroscopic ellipsometry, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD), respectively. An average growth rate of approximately 0.0105 angstroms per cycle at 260 °C was observed via ellipsometry. Uniform deposition of ZnO with less than 1% of Ni was displayed by utilizing the elemental analysis function via SEM, thereby providing high-quality images. XPS revealed ionizations consistent with nickel and ZnO through the kinetic and binding energies of each detected electron. XRD provided supplemental information regarding the validity of ZnO by exhibiting crystalline attributes, revealing the presence of its hexagonal wurtzite structure. 

Abstract Nearly 70 years old dream of incorporating molecule as the device element is still challenged by competing defects in almost every experimentally tested molecular device approach. This paper focuses on the magnetic tunnel junction (MTJ) based molecular spintronics device (MTJMSD) method. An MTJMSD utilizes a tunnel barrier to ensure a robust and mass-producible physical gap between two ferromagnetic electrodes. MTJMSD approach may benefit from MTJ's industrial practices; however, the MTJMSD approach still needs to overcome additional challenges arising from the inclusion of magnetic molecules in conjunction with competing defects. Molecular device channels are covalently bonded between two ferromagnets across the insulating barrier. An insulating barrier may possess a variety of potential defects arising during the fabrication or operational phase. This paper describes an experimental and theoretical study of molecular coupling between ferromagnets in the presence of the competing coupling via an insulating tunnel barrier. We discuss the experimental observations of hillocks and pinhole-type defects producing inter-layer coupling that compete with molecular device elements. We performed theoretical simulations to encompass a wide range of competition between molecules and defects. Monte Carlo Simulation (MCS) was used for investigating the defect-induced inter-layer coupling on MTJMSD. Our research may help understand and design molecular spintronics devices utilizing various insulating spacers such as aluminum oxide (AlOx) and magnesium oxide (MgO) on a wide range of metal electrodes. This paper intends to provide practical insights for researchers intending to investigate the molecular device properties via the MTJMSD approach and do not have a background in magnetic tunnel junction fabrication. 

The hysteresis loop investigations of different size magnetic tunnel junction molecular spintronics devices (MTJMSD) have been done by Monte Carlo simulation (MCS). We employed a continuous MCS algorithm to investigate single-molecule magnet SMM’s spin state’s impact as a function of molecular exchange coupling strength. The applied magnetic fields were ramped at a variety of ranges of increments, unfolding physics behind the magnetization nature of each MTJMSD. The magnetic moment changes with applied magnetic fields exhibit the characteristics of devices being studied. The MTJMSDs were studied for ferromagnetic and antiferromagnetic exchange couplings. The magnetic moment saturation, retentivity, coercivity, and permeability are studied. 

The magnetic tunnel junction (MTJ) based molecular spintronics device (MTJMSD) approach is suitable for mass production. This approach provides solutions to fabrication difficulties related to reliably connecting molecular device elements to the ferromagnets (FMs). To producing MTJMSD, the molecular channels are bridged across the insulator of an MTJ testbed with exposed side edges. In an MTJMSD, two FMs are simultaneously connected by an insulator film and the molecular channels along the exposed sides. In our prior experimental studies, we observed that molecules could produce strong coupling between ferromagnets in the presence of the competing coupling via an insulator. In this paper, our Monte Carlo Simulation (MCS) was used to study the impact of coupling variation via insulator (a.k.a. Ji) on the magnetic properties of an MTJMSD. We studied the effect of Ji while varying the molecule induced antiferromagnetic exchange coupling. The ferromagnetic or antiferromagnetic nature and magnitude of Ji determined the resultant effect. Antiferromagnetic Ji enhanced the pre-existing antiferromagnetic molecular coupling effect. Ferromagnetic Ji competed with the opposite nature of antiferromagnetic molecular coupling. Our MCS may help to understand the impact of insulator thickness and defects on the molecular spintronics device performance and design process.