Paramagnetic single-molecule magnets (SMMs) interacting with the ferromagnetic electrodes of a magnetic tunnel junction (MTJ) produce a new system. The properties and future scope of new systems differ dramatically from the properties of isolated molecules and ferromagnets. However, it is unknown how far deep in the ferromagnetic electrode the impact of the paramagnetic molecule and ferromagnet interactions can travel for various levels of molecular spin states. Our prior experimental studies showed two types of paramagnetic SMMs, the hexanuclear Mn 6 and octanuclear Fe–Ni molecular complexes, covalently bonded to ferromagnets produced unprecedented strong antiferromagnetic coupling between two ferromagnets at room temperature leading to a number of intriguing observations (P. Tyagi, et al. , Org. Electron. , 2019, 64 , 188–194. P. Tyagi, et al. , RSC Adv. , 2020, 10 , (22), 13006–13015). This paper reports a Monte Carlo Simulations (MCS) study focusing on the impact of the molecular spin state on a cross junction shaped MTJ based molecular spintronics device (MTJMSD). Our MCS study focused on the Heisenberg model of MTJMSD and investigated the impact of various molecular coupling strengths, thermal energy, and molecular spin states. To gauge the impact of the molecular spin state on the region of ferromagnetic electrodes, we examined the spatial distribution of molecule-ferromagnet correlated phases. Our MCS study shows that under a strong coupling regime, the molecular spin state should be ∼30% of the ferromagnetic electrode's atomic spins to create long-range correlated phases. 
                        more » 
                        « less   
                    
                            
                            Dramatic Effects of Electrode Metal on Tunnel Junction-Based Molecular Spintronic Devices
                        
                    
    
            Magnetic tunnel junction (MTJ) can serve as an excellent testbed for connecting Molecule between two ferromagnetic electrodes. A paramagnetic molecule covalently bonded to two ferromagnetic electrodes with two thiol functional groups can produce intriguing transport and magnetic properties. We have chemically bonded paramagnetic molecules between two ferromagnetic electrodes of a MTJ along the exposed side edges. In this paper we discussed the observation of Molecule induced dramatic changes in the magnetic and transport properties of the conventional magnetic tunnel junctions. Paramagnetic molecules were chemically bonded to ferromagnetic electrodes to bridge them across the insulating spacer along the exposed edges. Paramagnetic molecular channels along the tunnel junction edges decreased the overall current, through tunnel barrier and molecular channels, > 5 orders of magnitude below the leakage current of the bare tunnel junction at room temperature. These molecules caused significant changes in the spin density of states due to potential spin filtering effect. Also, paramagnetic molecules produced antiferromagnetic coupling between the affected magnetic electrodes. In this state spin transport in the magnetic tunnel junction based molecular devices plummeted by several orders. It is also noteworthy that our experimental studies provide a platform to connect a vast variety of ferromagnetic leads to the even broader array of high potential molecules such as single molecular magnets, porphyrin, and single ion molecules. The strength of exchange coupling between ferromagnetic electrodes and molecules can be tailored by utilizing different tethers and terminal functional groups. The MTJMSD can provide an advanced form of logic and memory devices, including a testbed for the Molecule based quantum computation devices. Future study about the interaction between molecular magnets and ferromagnets and interaction of thiol ended alkanes with ferromagnets will be of very valuable. This study indicates the potential of magnetic molecules as a mean to transforming conventional magnetic tunnel junctions and producing unprecedented magnetic and transport properties. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 1914751
- PAR ID:
- 10333107
- Date Published:
- Journal Name:
- MRS 2022, Hawaii
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            Abstract Magnetic tunnel junction-based molecular spintronics device (MTJMSD) may enable novel magnetic metamaterials by chemically bonding magnetic molecules and ferromagnets (FM) with a vast range of magnetic anisotropy. MTJMSD have experimentally shown intriguing microscopic phenomenon such as the development of highly contrasting magnetic phases on a ferromagnetic electrode at room temperature. This paper focuses on Monte Carlo Simulations (MCS) on MTJMSD to understand the potential mechanism and explore fundamental knowledge about the impact of magnetic anisotropy. The selection of MCS is based on our prior study showing the potential of MCS in explaining experimental results (Tyagi et al. in Nanotechnology 26:305602, 2015). In this paper, MCS is carried out on the 3D Heisenberg model of cross-junction-shaped MTJMSDs. Our research represents the experimentally studied cross-junction-shaped MTJMSD where paramagnetic molecules are covalently bonded between two FM electrodes along the exposed side edges of the magnetic tunnel junction (MTJ). We have studied atomistic MTJMSDs properties by simulating a wide range of easy-axis anisotropy for the case of experimentally observed predominant molecule-induced strong antiferromagnetic coupling. Our study focused on understanding the effect of anisotropy of the FM electrodes on the overall MTJMSDs at various temperatures. This study shows that the multiple domains of opposite spins start to appear on an FM electrode as the easy-axis anisotropy increases. Interestingly, MCS results resembled the experimentally observed highly contrasted magnetic zones on the ferromagnetic electrodes of MTJMSD. The magnetic phases with starkly different spins were observed around the molecular junction on the FM electrode with high anisotropy.more » « less
- 
            Magnetic tunnel junctions (MTJs) can integrate novel single molecular device elements to overcome long-standing fabrication challenges, thus unlocking their novel potential. This study employs magnetic force microscopy (MFM) to demonstrate that organometallic molecules, when placed between two ferromagnetic electrodes along cross-junction shaped MTJ edges, dramatically altered the magnetic properties of the electrodes, affecting areas several hundred microns in size around the molecular junction vicinity at room temperature. These findings are supported by magnetic resonance and magnetometer studies on ∼7000 MTJ pillars. MFM on the pillar sample showed an almost complete disappearance of the magnetic contrast. The spatial magnetic image suggests that molecular channels significantly impacted the spin density of states in the ferromagnetic electrodes. This advancement in MTJ-based molecular devices paves the way for a new generation of commercially viable logic and memory devices controlled by molecular quantum states at near-room temperatures.more » « less
- 
            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.more » « less
- 
            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.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
 
                                    