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Hydrogen, the smallest and most abundant element in nature, can be efficiently incorporated within a solid and drastically modify its electronic and structural state. In most semiconductors interstitial hydrogen binds to defects and is known to be amphoteric, namely it can act either as a donor (H⁺) or an acceptor (H⁻) of charge, nearly always counteracting the prevailing conductivity type. Here we demonstrate that hydrogenation resolves an outstanding challenge in chalcogenide classes of three-dimensional (3D) topological insulators and magnets — the control of intrinsic bulk conduction that denies access to quantum surface transport, imposing severe thickness limits on the bulk. With electrons donated by a reversible binding of H⁺ions to Te(Se) chalcogens, carrier densities are reduced by over 10²⁰cm⁻³, allowing tuning the Fermi level into the bulk bandgap to enter surface/edge current channels without altering carrier mobility or the bandstructure. The hydrogen-tuned topological nanostructures are stable at room temperature and tunable disregarding bulk size, opening a breadth of device platforms for harnessing emergent topological states.

 

Abstract MnBi 2 Te 4 /(Bi 2 Te 3 ) n materials system has recently generated strong interest as a natural platform for the realization of the quantum anomalous Hall (QAH) state. The system is magnetically much better ordered than substitutionally doped materials, however, the detrimental effects of certain disorders are becoming increasingly acknowledged. Here, from compiling structural, compositional, and magnetic metrics of disorder in ferromagnetic (FM) MnBi 2 Te 4 /(Bi 2 Te 3 ) n it is found that migration of Mn between MnBi 2 Te 4 septuple layers (SLs) and otherwise non-magnetic Bi 2 Te 3 quintuple layers (QLs) has systemic consequences—it induces FM coupling of Mn-depleted SLs with Mn-doped QLs, seen in ferromagnetic resonance as an acoustic and optical resonance mode of the two coupled spin subsystems. Even for a large SL separation ( n ≳ 4 QLs) the structure cannot be considered as a stack of uncoupled two-dimensional layers. Angle-resolved photoemission spectroscopy and density functional theory studies show that Mn disorder within an SL causes delocalization of electron wave functions and a change of the surface band structure as compared to the ideal MnBi 2 Te 4 /(Bi 2 Te 3 ) n . These findings highlight the critical importance of inter- and intra-SL disorder towards achieving new QAH platforms as well as exploring novel axion physics in intrinsic topological magnets.