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Graphene/$alpha$-RuCl$_3$: An Emergent 2D Plasmonic Interface

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 Added by Daniel Rizzo
 Publication date 2020
  fields Physics
and research's language is English




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Work function-mediated charge transfer in graphene/$alpha$-RuCl$_3$ heterostructures has been proposed as a strategy for generating highly-doped 2D interfaces. In this geometry, graphene should become sufficiently doped to host surface and edge plasmon-polaritons (SPPs and EPPs, respectively). Characterization of the SPP and EPP behavior as a function of frequency and temperature can be used to simultaneously probe the magnitude of interlayer charge transfer while extracting the optical response of the interfacial doped $alpha$-RuCl$_3$. We accomplish this using scanning near-field optical microscopy (SNOM) in conjunction with first-principles DFT calculations. This reveals massive interlayer charge transfer (2.7 $times$ 10$^{13}$ cm$^{-2}$) and enhanced optical conductivity in $alpha$-RuCl$_3$ as a result of significant electron doping. Our results provide a general strategy for generating highly-doped plasmonic interfaces in the 2D limit in a scanning probe-accessible geometry without need of an electrostatic gate.



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Recent developments in twisted and lattice-mismatched bilayers have revealed a rich phase space of van der Waals systems and generated excitement. Among these systems are heterobilayers which can offer new opportunities to control van der Waals systems with strong in plane correlations such as spin-orbit-assisted Mott insulator $alpha$-RuCl$_3$. Nevertheless, a theoretical $textit{ab initio}$ framework for mismatched heterobilayers without even approximate periodicity is sorely lacking. We propose a general strategy for calculating electronic properties of such systems, mismatched interface theory (MINT), and apply it to the graphene/$alpha$-RuCl$_{3}$ (GR/$alpha$-RuCl$_{3}$) heterostructure. Using MINT, we predict uniform doping of 4.77$%$ from graphene to $alpha$-RuCl$_3$ and magnetic interactions in $alpha$-RuCl$_3$ to shift the system toward the Kitaev point. Hence we demonstrate that MINT can guide targeted materialization of desired model systems and discuss recent experiments on GR/$alpha$-RuCl$_{3}$ heterostructures.
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