Near Room-Temperature Intrinsic Exchange Bias in an Fe Intercalated ZrSe₂ Spin Glass

Abstract

Some magnetic systems display a shift in the center of their magnetic hysteresis loop away from zero field, a phenomenon termed exchange bias. Despite the extensive use of the exchange bias effect, particularly in magnetic multilayers, for the design of spin-based memory/electronics devices, a comprehensive mechanistic understanding of this effect remains a longstanding problem. Recent work has shown that disorder-induced spin frustration might play a key role in exchange bias, suggesting new materials design approaches for spin-based electronic devices that harness this effect. Here, we design a spin glass with strong spin frustration induced by magnetic disorder by exploiting the distinctive structure of Fe intercalated ZrSe 2 , where Fe(II) centers are shown to occupy both octahedral and tetrahedral interstitial sites and to distribute between ZrSe 2 layers without long-range structural order. Notably, we observe behavior consistent with a magnetically frustrated and multidegenerate ground state in these Fe 0.17 ZrSe 2 single crystals, which persists above room temperature. Moreover, this magnetic frustration leads to a robust and tunable exchange bias up to 250 K. These results not only offer important insights into the effects of magnetic disorder and frustration in magnetic materials generally, but also highlight as design strategy the idea that a large exchange bias can arise from an inhomogeneous microscopic environment without discernible long-range magnetic order. In addition, these results show that intercalated TMDs like Fe 0.17 ZrSe 2 hold potential for spintronic technologies that can achieve room temperature applications.

Intrinsic exchange biased anomalous Hall effect in an uncompensated antiferromagnet MnBi2Te4

“…Recently, the exchange bias effect has been found to stabilize in single compounds with complex magnetic phases 26 , 29 – 31 . The exchange bias effect in single-component magnetic material on a non-magnetic substrate or without an additional antiferromagnetic layer can be a candidate for the intrinsic exchange bias effect 32 , 33 . An interesting example is bulk Co 3 Sn 2 S 2 , which exhibits an exchange bias anomalous Hall effect driven by fluctuations originating from its spin glass phase 29 .…”

Unraveling the Stability of Layered Intercalation Compounds through First-Principles Calculations: Establishing a Linear Free Energy Relationship with Aqueous Ions

“…Layered intercalation compounds, which have a structure in which atoms or molecules (intercalants) are inserted into layered compounds (hosts), have been extensively studied because of their characteristic physical properties and the wide variety of synthetic methods available. Due to their ability to intercalate/deintercalate ions and molecules, , they are being investigated for applications in energy storage, and various properties resulting from their two-dimensional nature, such as superconductivity, − spin glass, and topological electronic states, have also been studied. Other novel phenomena have also been reported, such as the change in host electrowetting response and manipulation of magnetism due to molecule intercalation.…”

Unraveling the Stability of Layered Intercalation Compounds through First Principles Calculations: Establishing a Linear Free Energy Relationship with Aqueous Ions

“…Layered intercalation compounds, which have a structure in which atoms or molecules (intercalants) are inserted into layered compounds (hosts), have been extensively studied because of their characteristic physical properties and the wide variety of synthetic methods available. Due to their ability to intercalate/de-intercalate ions and molecules, 1,2 they are being investigated for applications in energy storage, and various properties resulting from their two-dimensional nature, such as superconductivity, [3][4][5] spin glass, 6 topological electronic states, 7 have also been studied. Other novel phenomena have also been reported, such as the change in host electrowetting response 8 and manipulation of magnetism 9 due to molecule intercalation.…”