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Metallic solids such as crystals of copper, aluminum, and iron are formed by metal atoms. The structure of metallic crystals is often described as a uniform distribution of atomic nuclei within a “sea” of delocalized electrons. The atoms within such a metallic solid are held together by a unique force known as metallic bonding that gives rise to many useful and varied bulk properties.
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The coupling interactions of nuclei across four or more bonds are usually weak, with J values less than 1 Hz. While these are usually not observed in spectra, the presence of multiple bonds along the coupling pathway can result in observable long-range coupling.
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Polytypism and unexpected strong interlayer coupling in two-dimensional layered ReS2.

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Anisotropic layered materials like rhenium disulfide (ReS2) exhibit distinct stacking orders. This study reveals strong interlayer coupling in multilayer ReS2, challenging previous assumptions and opening new avenues for material property tuning.

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Nanotechnology

Background:

  • Anisotropic two-dimensional (2D) van der Waals (vdW) layered materials offer tunable physical properties through stacking order.
  • Multilayer rhenium disulfide (ReS2) was previously thought to lack significant interlayer coupling and exhibit random stacking.

Purpose of the Study:

  • To investigate the stacking orders and interlayer coupling in multilayer ReS2.
  • To identify stable stacking configurations and their impact on material properties.

Main Methods:

  • Utilized ultralow- and high-frequency Raman spectroscopy.
  • Employed photoluminescence spectroscopy.
  • Performed first-principles density functional theory calculations.

Main Results:

  • Identified two stable stacking orders in multilayer ReS2: isotropic-like (IS) and anisotropic-like (AI).
  • Observed distinct interlayer shear modes (two in AI-NL-ReS2, one in IS-NL-ReS2), confirming anisotropic and isotropic stacking, respectively.
  • Demonstrated unexpectedly strong interlayer coupling in both IS- and AI-NL-ReS2, with force constants comparable to multilayer MoS2.

Conclusions:

  • Multilayer ReS2 exhibits stable stacking orders with significant interlayer coupling, contrary to prior expectations.
  • The discovered polytypism and strong coupling in ReS2 provide a foundation for engineering properties of other anisotropic 2D materials through stacking control.