The magnetic and electronic properties of the magnetically doped topological insulator Bi$_{rm 2-x}$Mn$_{rm x}$Te$_3$ were studied using electron spin resonance (ESR) and measurements of static magnetization and electrical transport. The investigated high quality single crystals of Bi$_{rm 2-x}$Mn$_{rm x}$Te$_3$ show a ferromagnetic phase transition for $xgeq 0.04$ at $T_{C}approx 12$ K. The Hall measurements reveal a p-type finite charge-carrier density. Measurements of the temperature dependence of the ESR signal of Mn dopants for different orientations of the external magnetic field give evidence that the localized Mn moments interact with the mobile charge carriers leading to a Ruderman-Kittel-Kasuya-Yosida-type ferromagnetic coupling between the Mn spins of order 2-3 meV. Furthermore, ESR reveals a low-dimensional character of magnetic correlations that persist far above the ferromagnetic ordering temperature.
The ferromagnetic topological insulator V:(Bi,Sb)$_2$Te$_3$ has been recently reported as a quantum anomalous Hall (QAH) system. Yet the microscopic origins of the QAH effect and the ferromagnetism remain unclear. One key aspect is the contribution of the V atoms to the electronic structure. Here the valence band of V:(Bi,Sb)$_2$Te$_3$ thin films was probed in an element-specific way by resonant photoemission spectroscopy. The signature of the V $3d$ impurity band was extracted, and exhibits a high density of states near Fermi level. First-principles calculations support the experimental results and indicate the coexistence of ferromagnetic superexchange and double exchange interactions. The observed impurity band is thus expected to contribute to the ferromagnetism via the interplay of different mechanisms.
Rare earth ions typically exhibit larger magnetic moments than transition metal ions and thus promise the opening of a wider exchange gap in the Dirac surface states of topological insulators. Yet, in a recent photoemission study of Eu-doped Bi$_2$Te$_3$ films, the spectra remained gapless down to $T = 20;text{K}$. Here, we scrutinize whether the conditions for a substantial gap formation in this system are present by combining spectroscopic and bulk characterization methods with theoretical calculations. For all studied Eu doping concentrations, our atomic multiplet analysis of the $M_{4,5}$ x-ray absorption and magnetic circular dichroism spectra reveals a Eu$^{2+}$ valence and confirms a large magnetic moment, consistent with a $4f^7 ; {^8}S_{7/2}$ ground state. At temperatures below $10;text{K}$, bulk magnetometry indicates the onset of antiferromagnetic (AFM) ordering. This is in good agreement with density functional theory, which predicts AFM interactions between the Eu impurities. Our results support the notion that antiferromagnetism can coexist with topological surface states in rare-earth doped Bi$_2$Te$_3$ and call for spectroscopic studies in the kelvin range to look for novel quantum phenomena such as the quantum anomalous Hall effect.
We investigate the properties of a single substitutional Mn impurity and its associated acceptor state on the (111) surface of Bi$_2$Se$_3$ topological insulator. Combining ab initio calculations with microscopic tight-binding modeling, we identify the effects of inversion-symmetry and time-reversal-symmetry breaking on the electronic states in the vicinity of the Dirac point. In agreement with experiments, we find evidence that the Mn ion is in the ${+2}$-valence state and introduces an acceptor in the bulk band gap. The Mn-acceptor has predominantly $p$-character, and is localized mainly around the Mn impurity and its nearest-neighbor Se atoms. Its electronic structure and spin-polarization are determined by the hybridization between the Mn $d$-levels and the $p$-levels of surrounding Se atoms, which is strongly affected by electronic correlations at the Mn site. The opening of the gap at the Dirac point depends crucially on the quasi-resonant coupling and the strong real-space overlap between the spin-chiral surface states and the mid-gap spin-polarized Mn-acceptor states.
Doping Bi$_2$Se$_3$ by magnetic ions represents an interesting problem since it may break the time reversal symmetry needed to maintain the topological insulator character. Mn dopants in Bi$_2$Se$_3$ represent one of the most studied examples here. However, there is a lot of open questions regarding their magnetic ordering. In the experimental literature different Curie temperatures or no ferromagnetic order at all are reported for comparable Mn concentrations. This suggests that magnetic ordering phenomena are complex and highly susceptible to different growth parameters, which are known to affect material defect concentrations. So far theory focused on Mn dopants in one possible position, and neglected relaxation effects as well as native defects. We have used ab initio methods to calculate the Bi$_2$Se$_3$ electronic structure influenced by magnetic Mn dopants, and exchange interactions between them. We have considered two possible Mn positions, the substitutional and interstitial one, and also native defects. We have found a sizable relaxation of atoms around Mn, which affects significantly magnetic interactions. Surprisingly, very strong interactions correspond to a specific position of Mn atoms separated by van der Waals gap. Based on the calculated data we performed spin dynamics simulations to examine systematically the resulting magnetic order for various defect contents. We have found under which conditions the experimentally measured Curie temperatures ${T_{rm{C}}}$ can be reproduced, noticing that interstitial Mn atoms appear to be important here. Our theory predicts the change of ${T_{rm{C}}}$ with a shift of Fermi level, which opens the way to tune the system magnetic properties by selective doping.
Alloys of Bi$_2$Te$_3$ and Sb$_2$Te$_3$ ((Bi$_{1-x}$Sb$_x$)$_2$Te$_3$) have played an essential role in the exploration of topological surface states, allowing us to study phenomena that would otherwise be obscured by bulk contributions to conductivity. Thin films of these alloys have been particularly important for tuning the energy of the Fermi level, a key step in observing spin-polarized surface currents and the quantum anomalous Hall effect. Previous studies reported the chemical tuning of the Fermi level to the Dirac point by controlling the Sb:Bi composition ratio, but the optimum ratio varies widely across various studies with no consensus. In this work, we use scanning tunneling microscopy and Landau level spectroscopy, in combination with X-ray photoemission spectroscopy to isolate the effects of growth factors such as temperature and composition, and to provide a microscopic picture of the role that disorder and composition play in determining the carrier density of epitaxially grown (Bi,Sb)$_2$Te$_3$ thin films. Using Landau level spectroscopy, we determine that the ideal Sb concentration to place the Fermi energy to within a few meV of the Dirac point is $xsim 0.7$. However, we find that the post- growth annealing temperature can have a drastic impact on microscopic structure as well as carrier density. In particular, we find that when films are post-growth annealed at high temperature, better crystallinity and surface roughness are achieved; but this also produces a larger Te defect density, adding n-type carriers. This work provides key information necessary for optimizing thin film quality in this fundamentally and technologically important class of materials.
S. Zimmermann
,F. Steckel
,C. Hess
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(2016)
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"Spin dynamics and magnetic interactions of Mn dopants in the topological insulator Bi$_2$Te$_3$"
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Stephan Zimmermann
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