We present two-dimensional Mg(OH)₂ sheets and their vertical heterojunctions with CVD-MoS₂ for the first time as flexible 2D insulators with anomalous lattice vibration and chemical and physical properties. New hydrothermal crystal growth technique enabled isolation of environmentally stable monolayer Mg(OH)₂ sheets. Raman spectroscopy and vibrational calculations reveal that the lattice vibrations of Mg(OH)₂ have fundamentally different signature peaks and dimensionality effects compared to other 2D material systems known to date. Sub-wavelength electron energy-loss spectroscopy measurements and theoretical calculations show that Mg(OH)₂ is a 6 eV direct-gap insulator in 2D, and its optical band gap displays strong band renormalization effects from monolayer to bulk, marking the first experimental confirmation of confinement effects in 2D insulators. Interestingly, 2D-Mg(OH)₂ sheets possess rather strong surface polarization (charge) effects which is in contrast to electrically neutral h-BN materials. Using 2D-Mg(OH)₂ sheets together with CVD-MoS₂ in the vertical stacking shows that a strong change transfer occurs from n-doped CVD-MoS₂ sheets to Mg(OH)₂, naturally depleting the semiconductor, pushing towards intrinsic doping limit and enhancing overall optical performance of 2D semiconductors. Results not only establish unusual confinement effects in 2D-Mg(OH)₂, but also offer novel 2D-insulating material with unique physical, vibrational, and chemical properties for potential applications in flexible optoelectronics.

The valley degree of freedom in two-dimensional (2D) crystals recently emerged as a novel information carrier in addition to spin and charge. The intrinsic valley lifetime in 2D transition metal dichalcogenides (TMD) is expected to be markedly long due to the unique spin-valley locking behavior, where the intervalley scattering of the electron simultaneously requires a large momentum transfer to the opposite valley and a flip of the electron spin. However, the experimentally observed valley lifetime in 2D TMDs has been limited to tens of nanoseconds thus far. We report efficient generation of microsecond-long-lived valley polarization in WSe₂/MoS₂ heterostructures by exploiting the ultrafast charge transfer processes in the heterostructure that efficiently creates resident holes in the WSe₂ layer. These valley-polarized holes exhibit near-unity valley polarization and ultralong valley lifetime: We observe a valley-polarized hole population lifetime of more than 1 μs and a valley depolarization lifetime (that is, intervalley scattering lifetime) of more than 40 μs at 10 K. The near-perfect generation of valley-polarized holes in TMD heterostructures, combined with ultralong valley lifetime, which is orders of magnitude longer than previous results, opens up new opportunities for novel valleytronics and spintronics applications.

The strong light-matter interaction and the valley selective optical selection rules make monolayer (ML) MoS₂ an exciting 2D material for fundamental physics and optoelectronics applications. But, so far, optical transition linewidths even at low temperature are typically as large as a few tens of meV and contain homogeneous and inhomogeneous contributions. This prevented in-depth studies, in contrast to the better-characterized ML materials MoSe₂ and WSe₂. In this work, we show that encapsulation of ML MoS₂ in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as we measure in photoluminescence and reflectivity a FWHM down to 2 meV at T = 4 K. Narrow optical transition linewidths are also observed in encapsulated WS₂, WSe₂, and MoSe₂ MLs. This indicates that surface protection and substrate flatness are key ingredients for obtaining stable, high-quality samples. Among the new possibilities offered by the well-defined optical transitions, we measure the homogeneous broadening induced by the interaction with phonons in temperature-dependent experiments. We uncover new information on spin and valley physics and present the rotation of valley coherence in applied magnetic fields perpendicular to the ML.