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Register a new userEvidence of Spin-Glass state in Molecular Exchange-Bias System
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In conventional exchange-bias system comprising of a bilayer film of ferromagnet (FM) and antiferromagnet (AFM), investigating the role of spin-disorder and spin-frustration inside the AFM and at the interface has been crucial in understanding the fundamental mechanism controlling the exchange-bias -- an effect that leads to a horizontal shift in the magnetization hysteresis response of the FM. Similarly, in the recently reported monolayer molecular exchange-bias effect requiring no AFM layer, probing magnetic-disorder at the FM/molecule interface or inside the FM layer can provide new insights into the origin of molecular exchange-bias and the associated physics. In this article, by cooling the Fe/metal-phthalocyanine devices in oscillating magnetic field, we demonstrate a characteristic temperature dependent response of exchange-bias shift and ferromagnet coercivity that is supportive of a spin-glass behavior. Here, the origin of spin-glass is attributed to the spin frustration created in the magnetic structure of the Fe layer, which was absent in our reference-Fe studies. These results highlight the strong influence of FM/molecule interface pi-d hybridization on the magnetic exchange interactions extending deeper into the FM layer.
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SrTi0.5Mn0.5O3 (STMO) is a chemically disordered perovskite having random distribution of Ti and Mn over 1b site. Striking discrepancies about the structural and magnetic properties of STMO demands detailed analysis which is addressed. To explore the magnetic ground state of STMO, static and dynamic magnetic properties were studied over a broad temperature range (2-300 K). The dc, ac magnetization show a cusp like peak at Tf ~ 14 K, which exhibits field and frequency dependence. The thermoremanent magnetization is characterized by using stretched exponential function and characteristic time suggests the existence of spin clusters. Also the other features observed in magnetic memory effect, muon spin resonance/rotation and neutron powder diffraction confirm the existence of cluster spin glass state in STMO, rather than the long range ordered ground state. Intriguingly, the observed spin relaxation can be attributed to the dilute magnetism due to non-magnetic doping at Mn-site and competing antiferromagnetic and ferromagnetic interactions resulting from the site disorder.
We performed SQUID and FMR magnetometry experiments to clarify the relationship between two reported magnetic exchange effects arising from interfacial spin-polarized charge transfer within ferromagnetic metal (FM)/molecule bilayers: the magnetic hardening effect, and spinterface-stabilized molecular spin chains. To disentangle these effects, both of which can affect the FM magnetization reversal, we tuned the metal phthalocyanine molecule central sites magnetic moment to selectively enhance or suppress the formation of spin chains within the molecular film. We find that both effects are distinct, and additive. In the process, we 1) extended the list of FM/molecule candidate pairs that are known to generate magnetic exchange effects, 2) experimentally confirmed the predicted increase in anisotropy upon molecular adsorption; and 3) showed that spin chains within the molecular film can enhance magnetic exchange. This magnetic ordering within the organic layer implies a structural ordering. Thus, by distengangling the magnetic hardening and exchange bias contributions, our results confirm, as an echo to progress regarding inorganic spintronic tunnelling, that the milestone of spintronic tunnelling across structurally ordered organic barriers has been reached through previous magnetotransport experiments. This paves the way for solid-state devices studies that exploit the quantum physical properties of spin chains, notably through external stimuli.
The ground-state magnetic properties of hexagonal equiatomic alloy of nominal composition Mn_{0.8}Fe_{0.2}NiGe were investigated through dc magnetization and heat capacity measurements. The alloy undergoes first order martensitic transition below 140 K with simultaneous development of long range ferromagnetic ordering from the high temperature paramagnetic phase. The undoped compound MnNiGe has an antiferromagnetic ground state and it shows martensitic like structural instability well above room temperature. Fe doping at the Mn site not only brings down the martensitic transition temperature, it also induces ferromagnetism in the sample. Our study brings out two important aspects regarding the sample, namley (i) the observation of exchange bias at low temperature, and (ii) spin glass like ground state which prevails below the martensitic and magnetic transition points. In addition to the observed usual relaxation behavior the spin glass state is confirmed by zero field cooled memory experiment, thereby indicating cooperative freezing of spin and/or spin clusters rather than uncorrelated dynamics of superparamagnetic like spin clusters. We believe that doping disorder can give rise to some islands of antiferromagnetic clusters in the otherwise ferromagnetic background which can produce interfacial frustration and exchange pinning responsible for spin glass and exchange bias effect. A comparison is made with doped rare-earth manganites where similar phase separation can lead to glassy ground state.
As a sister compound and isostructural of MnBi2Te4, the high quality MnSb2Te4 single crystals are grown via solid-state reaction where prolonged annealing and narrow temperature window play critical roles on account of its thermal metastability. X-ray diffraction analysis on MnSb2Te4 single crystals reveals pronounced cation intermixing, 28.9(7)% Sb antisite defects on the Mn (3a) site and 19.3(6)% Mn antisite defects on the Sb (6c) site, compared with MnBi2Te4. Unlike antiferromagnetic (AFM) nature MnBi2Te4, MnSb2Te4 contains magnetic and antiferromagnetic competition and exhibits a spin glass (SG) state below 24 K. Its magnetic hysteresis, anisotropy, and relaxation process are investigated in detail with DC and AC magnetization measurements. Moreover, anomalous Hall effect as a p-type conductor is demonstrated through transport measurements. This work grants MnSb2Te4 a possible access to the future exploration of exotic quantum physics by removing the odd/even layer number restraint in intrinsic AFM MnBi2Te4-family materials as a result of the crossover between its magnetism and potential topology in the Sb-Te layer.
Electrically induced ionic motion offers a new way to realize voltage-controlled magnetism, opening the door to a new generation of logic, sensor, and data storage technologies. Here, we demonstrate an effective approach to magneto-ionically and electrically tune exchange bias in Gd/Ni$_{1-x}$Co$_{x}$O thin films (x=0.50, 0.67), where neither of the layers alone is ferromagnetic at room temperature. The Gd capping layer deposited onto antiferromagnetic Ni$_{1-x}$Co$_{x}$O initiates a solid-state redox reaction that reduces an interfacial region of the oxide to ferromagnetic NiCo. Exchange bias is established after field cooling, which can be enhanced by up to 35% after a voltage conditioning and subsequently reset with a second field cooling. These effects are caused by the presence of an interfacial ferromagnetic NiCo layer, which further alloys with the Gd layer upon field cooling and voltage application, as confirmed by electron microscopy and polarized neutron reflectometry studies. These results highlight the viability of the solid-state magneto-ionic approach to achieve electric control of exchange bias, with potentials for energy-efficient magneto-ionic devices.
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