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Local electronic and magnetic properties of the doped topological insulators Bi$_{2}$Se$_{3}$:Ca and Bi$_{2}$Te$_{3}$:Mn investigated using ion-implanted $^{8}$Li $beta$-NMR

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 Added by Ryan McFadden
 Publication date 2019
  fields Physics
and research's language is English




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We report $beta$-detected nuclear magnetic resonance ($beta$-NMR) measurements in Bi$_{2}$Se$_{3}$:Ca (BSC) and Bi$_{2}$Te$_{3}$:Mn (BTM) single crystals using $^{8}$Li$^{+}$ implanted to depths on the order of 100 nm. Above $sim 200$ K, spin-lattice relaxation (SLR) reveals diffusion of $^{8}$Li$^{+}$, with activation energies of $sim 0.4$ eV ($sim 0.2$ eV) in BSC (BTM). At lower temperatures, the nuclear magnetic resonance (NMR) properties are those of a heavily doped semiconductor in the metallic limit, with Korringa relaxation and a small, negative, temperature-dependent Knight shift in BSC. From this, we make a detailed comparison with the isostructural tetradymite Bi$_{2}$Te$_{2}$Se (BTS) [McFadden et al., Phys Rev. B 99, 125201 (2019)]. In the magnetic BTM, the effects of the dilute Mn moments predominate, but remarkably the $^{8}$Li signal is not wiped out through the magnetic transition at 13 K, with a prominent critical peak in the SLR that is suppressed in a high applied field. This detailed characterization of the $^{8}$Li NMR response is an important step towards using depth-resolved $beta$-NMR to study the low-energy properties of the chiral topological surface state (TSS). With the bulk NMR response now established in several Bi$_{2}$Ch$_{3}$ tetradymite topological insulators (TIs), the prospect of directly probing their chiral TSS using the depth resolution afforded by $beta$-NMR remains strong.



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We report measurements on the high temperature ionic and low temperature electronic properties of the 3D topological insulator Bi$_2$Te$_2$Se using ion-implanted $^8$Li $beta$-detected nuclear magnetic relaxation and resonance. With implantation energies in the range 5-28 keV, the probes penetrate beyond the expected range of the topological surface state, but are still within 250 nm of the surface. At temperatures above ~150 K, spin-lattice relaxation measurements reveal isolated $^8$Li$^{+}$ diffusion with an activation energy $E_{A} = 0.185(8)$ eV and attempt frequency $tau_{0}^{-1} = 8(3) times 10^{11}$ s$^{-1}$ for atomic site-to-site hopping. At lower temperature, we find a linear Korringa-like relaxation mechanism with a field dependent slope and intercept, which is accompanied by an anomalous field dependence to the resonance shift. We suggest that these may be related to a strong contribution from orbital currents or the magnetic freezeout of charge carriers in this heavily compensated semiconductor, but that conventional theories are unable to account for the extent of the field dependence. Conventional NMR of the stable host nuclei may help elucidate their origin.
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We present a first-principles study of the electronic, magnetic, and transport properties of the topological insulator Bi$_{2}$Te$_{3}$ doped with Mn atoms in substitutional (Mn$_{rm Bi}$) and interstitial van der Waals gap positions (Mn$_{rm i}$), which act as acceptors and donors, respectively. The effect of native Bi$_{rm Te}$- and Te$_{rm Bi}$-antisite defects and their influence on calculated electronic transport properties is also investigated. We have studied four models representing typical cases, namely (i) Bi$_{2}$Te$_{3}$ with and without native defects, (ii) Mn$_{rm Bi}$ defects with and without native defects, (iii) the same but for Mn$_{rm i}$ defects, and (iv) the combined presence of Mn$_{rm Bi}$ and Mn$_{rm i}$. It was found that lattice relaxations around Mn$_{rm Bi}$ defects play an important role for both magnetic and transport properties. The resistivity is strongly influenced by the amount of carriers, their type, and by the relative positions of the Mn-impurity energy levels and the Fermi energy. Our results indicate strategies to tune bulk resistivities, and also help to uncover the location of Mn atoms in measured samples. Calculations indicate that at least two of the considered defects have to be present simultaneously in order to explain the experimental observations, and the role of interstitials may be more important than expected.
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.
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We used low-energy, momentum-resolved inelastic electron scattering to study surface collective modes of the three-dimensional topological insulators Bi$_2$Se$_3$ and Bi$_{0.5}$Sb$_{1.5}$Te$_{3-x}$Se$_{x}$. Our goal was to identify the spin plasmon predicted by Raghu and co-workers [S. Raghu, et al., Phys. Rev. Lett. 104, 116401 (2010)]. Instead, we found that the primary collective mode is a surface plasmon arising from the bulk, free carrers in these materials. This excitation dominates the spectral weight in the bosonic function of the surface, $chi (textbf{q},omega)$, at THz energy scales, and is the most likely origin of a quasiparticle dispersion kink observed in previous photoemission experiments. Our study suggests that the spin plasmon may mix with this other surface mode, calling for a more nuanced understanding of optical experiments in which the spin plasmon is reported to play a role.
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