<p>Controlling the crystal phase of two-dimensional (2D) transition metal dichalcogenides (TMDs) is essential for tailoring their optical and electronic properties. While phase transitions in monolayer TMDs and semiconductor-to-metal conversions have been widely studied, structural transitions between semiconducting polytypes - particularly in bilayer (2L) systems - remain underexplored. Here, we demonstrate a tungsten (W) doping-induced phase transition from non-centrosymmetric AA stacking to centrosymmetric AB’ in 2L MoS<sub>2</sub> synthesized by chemical vapor deposition (CVD). Using polarization-resolved second harmonic generation (SHG) and low-frequency Raman spectroscopy, we identify a phase transition correlated with increasing W concentration. The dilute W-doped 2 L system exhibits a vanishing SHG signal and a stiffening of the layer-breathing (LB) vibrational mode, in contrast to undoped samples with strong SHG and a softer LB mode. Aberration corrected scanning transmission electron microscopy (AC-STEM) demonstrates the spatial distribution of W concentration and associated structural changes. These findings highlight W-doping as an effective strategy for inducing phase transitions in 2L TMDs, opening new possibilities for engineered heterostructures, phase-controlled device applications or as a source of single photon emitters.</p>

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Tungsten doping-induced phase transition in CVD-grown MoS2 bilayers

  • Ana Senkić,
  • Rachael Keneipp,
  • Petra Ivatović,
  • Namrata Pradeep,
  • Vincent Meunier,
  • Marko Kralj,
  • Marija Drndić,
  • Nataša Vujičić

摘要

Controlling the crystal phase of two-dimensional (2D) transition metal dichalcogenides (TMDs) is essential for tailoring their optical and electronic properties. While phase transitions in monolayer TMDs and semiconductor-to-metal conversions have been widely studied, structural transitions between semiconducting polytypes - particularly in bilayer (2L) systems - remain underexplored. Here, we demonstrate a tungsten (W) doping-induced phase transition from non-centrosymmetric AA stacking to centrosymmetric AB’ in 2L MoS2 synthesized by chemical vapor deposition (CVD). Using polarization-resolved second harmonic generation (SHG) and low-frequency Raman spectroscopy, we identify a phase transition correlated with increasing W concentration. The dilute W-doped 2 L system exhibits a vanishing SHG signal and a stiffening of the layer-breathing (LB) vibrational mode, in contrast to undoped samples with strong SHG and a softer LB mode. Aberration corrected scanning transmission electron microscopy (AC-STEM) demonstrates the spatial distribution of W concentration and associated structural changes. These findings highlight W-doping as an effective strategy for inducing phase transitions in 2L TMDs, opening new possibilities for engineered heterostructures, phase-controlled device applications or as a source of single photon emitters.