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Instability of the topological surface state in Bi$_2$Se$_3$ upon deposition of gold

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 Publication date 2018
  fields Physics
and research's language is English




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Momentum resolved photoemission spectroscopy indicates the instability of the Dirac surface state upon deposition of gold on the (0001) surface of the topological insulator Bi$_2$Se$_3$. Based on the structure model derived from extended x-ray absorption fine structure experiments showing that gold atoms substitute bismuth atoms, first principles calculations provide evidence that a gap appears due to hybridization of the surface state with gold d-states near the Fermi level. Our findings provide new insights into the mechanisms affecting the stability of the surface state.

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The interaction between magnetic impurities and the gapless surface state is of critical importance for realizing novel quantum phenomena and new functionalities in topological insulators. By combining angle-resolved photoemission spectroscopic experiments with density functional theory calculations, we show that surface deposition of Cr atoms on Bi$_2$Se$_3$ does not lead to gap opening of the surface state at the Dirac point, indicating the absence of long-range out-of-plane ferromagnetism down to our measurement temperature of 15 K. This is in sharp contrast to bulk Cr doping, and the origin is attributed to different Cr occupation sites. These results highlight the importance of nanoscale configuration of doped magnetic impurities in determining the electronic and magnetic properties of topological insulators.
Using scanning tunneling spectroscopy we have studied the effects of nitrogen gas exposure on the bismuth selenide density of states. We observe a shift in the Dirac point which is qualitatively consistent with theoretical modeling of nitrogen binding to selenium vacancies. In carefully controlled measurements, Bi$_2$Se$_3$ crystals were initially cleaved in a helium gas environment and then exposed to a 22 SCFH flow of ultra-high purity N$_2$ gas. We observe a resulting change in the spectral curves, with the exposure effect saturating after approximately 50 minutes, ultimately bringing the Dirac point about 50 meV closer to the Fermi level. These results are compared to density functional theoretical calculations, which support a picture of $N_2$ molecules physisorbing near Se vacancies and dissociating into individual N atoms which then bind strongly to Se vacancies. In this interpretation, the binding of the N atom to a Se vacancy site removes the surface defect state created by the vacancy and changes the position of the Fermi energy with respect to the Dirac point.
We study the fate of the surface states of Bi$_2$Se$_3$ under disorder with strength larger than the bulk gap, caused by neon sputtering and nonmagnetic adsorbates. We find that neon sputtering introduces strong but dilute defects, which can be modeled by a unitary impurity distribution, whereas adsorbates, such as water vapor or carbon monoxide, are best described by Gaussian disorder. Remarkably, these two disorder types have a dramatically different effect on the surface states. Our soft x-ray ARPES measurements combined with numerical simulations show that unitary surface disorder pushes the Dirac state to inward quintuplet layers, burying it below an insulating surface layer. As a consequence, the surface spectral function becomes weaker, but retains its quasiparticle peak. This is in contrast to Gaussian disorder, which smears out the quasiparticle peak completely. At the surface of Bi$_2$Se$_3$, the effects of Gaussian disorder can be reduced by removing surface adsorbates using neon sputtering, which, however, introduces unitary scatterers. Since unitary disorder has a weaker effect than Gaussian disorder, the ARPES signal of the Dirac surface state becomes sharper upon sputtering.
Achieving true bulk insulating behavior in Bi$_2$Se$_3$, the archetypal topological insulator with a simplistic one-band electronic structure and sizable band gap, has been prohibited by a well-known self-doping effect caused by selenium vacancies, whose extra electrons shift the chemical potential into the bulk conduction band. We report a new synthesis method for achieving stoichiometric Bi$_2$Se$_3$ crystals that exhibit nonmetallic behavior in electrical transport down to low temperatures. Hall effect measurements indicate the presence of both electron- and hole-like carriers, with the latter identified with surface state conduction and the achievement of ambipolar transport in bulk Bi$_2$Se$_3$ crystals without gating techniques. With carrier mobilities surpassing the highest values yet reported for topological surface states in this material, the achievement of ambipolar transport via upward band bending is found to provide a key method to advancing the potential of this material for future study and applications.
178 - A. Kogar , S. Vig , A. Thaler 2015
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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