Mihalyuk, Alexey N.Alexey N.MihalyukBondarenko, Leonid V.Leonid V.BondarenkoTupchaya, Alexandra Y.Alexandra Y.TupchayaVekovshinin, Yuriy E.Yuriy E.VekovshininUtas, Tatyana V.Tatyana V.UtasGruznev, Dimitry V.Dimitry V.GruznevJYH PIN CHOUEremeev, Sergey V.Sergey V.EremeevZotov, Andrey V.Andrey V.ZotovSaranin, Alexander A.Alexander A.Saranin2024-09-182024-09-182023https://www.scopus.com/record/display.uri?eid=2-s2.0-85153191417&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/721388Article number 100372The quantum effects confined in the ultimate two-dimensional limit are able to address the challenges and provide advances in high-performance spintronic devices. In the paper we show a successful strategy to enrich the electronic properties of thallene, a new honeycomb analogue of graphene, through the interface engineering, which opens a great potential of thallene as an advanced spintronics material. While the thallene has been experimentally realized recently on NiSi2/Si(111) substrate, there remains a lack of attractive electronic properties due to the strong thallene-substrate coupling. This challenge is addressed here through the decoration of thallene/NiSi2 interface by Sn interlayer, which allows to eliminate the thallene-substrate coupling and produce a high-quality large-scale thallene monolayer with exotic electron bands demonstrating colossal spin-polarization just above the Fermi level. It is demonstrated that appropriate electron doping or external electric field are enable the spin-transport regime. The discovered band structure regulation boosts the functionality of the 2D-Tl Xene and makes it a highly attractive material for spintronics applications. © 2023 The Authors2D materialsSiliconSpin-orbit couplingSpintronicsXenesjournal article10.1016/j.mtadv.2023.1003722-s2.0-85153191417