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Register a new userAtomic reconstruction in twisted bilayers of transition metal dichalcogenides
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Van der Waals heterostructures form a massive interdisciplinary research field, fueled by the rich material science opportunities presented by layer assembly of artificial solids with controlled composition, order and relative rotation of adjacent atomic planes. Here we use atomic resolution transmission electron microscopy and multiscale modeling to show that the lattice of MoS$_2$ and WS$_2$ bilayers twisted to a small angle, $theta<3^{circ}$, reconstructs into energetically favorable stacking domains separated by a network of stacking faults. For crystal alignments close to 3R stacking, a tessellated pattern of mirror reflected triangular 3R domains emerges, separated by a network of partial dislocations which persist to the smallest twist angles. Scanning tunneling measurements show that the electronic properties of those 3R domains appear qualitatively different from 2H TMDs, featuring layer-polarized conduction band states caused by lack of both inversion and mirror symmetry. In contrast, for alignments close to 2H stacking, stable 2H domains dominate, with nuclei of an earlier unnoticed metastable phase limited to $sim$ 5nm in size. This appears as a kagome-like pattern at $thetasim 1^{circ}$, transitioning at $thetarightarrow 0$ to a hexagonal array of screw dislocations separating large-area 2H domains.
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We apply a multiscale modeling approach to study lattice reconstruction in marginally twisted bilayers of transition metal dichalcogenides (TMD). For this, we develop DFT-parametrized interpolation formulae for interlayer adhesion energies of MoSe$_2$, WSe$_2$, MoS$_2$, and WS$_2$, combine those with elasticity theory, and analyze the bilayer lattice relaxation into mesoscale domain structures. Paying particular attention to the inversion asymmetry of TMD monolayers, we show that 3R and 2H stacking domains, separated by a network of dislocations develop for twist angles $theta^{circ}<theta^{circ}_Psim 2.5^{circ}$ and $theta^{circ}<theta^{circ}_{AP}sim 1^{circ}$ for, respectively, bilayers with parallel (P) and antiparallel (AP) orientation of the monolayer unit cells and suggest how the domain structures would manifest itself in local probe scanning of marginally twisted P- and AP-bilayers.
In moire heterostructures, gate-tunable insulating phases driven by electronic correlations have been recently discovered. Here, we use transport measurements to characterize the gate-driven metal-insulator transitions and the metallic phase in twisted WSe$_2$ near half filling of the first moire subband. We find that the metal-insulator transition as a function of both density and displacement field is continuous. At the metal-insulator boundary, the resistivity displays strange metal behaviour at low temperature with dissipation comparable to the Planckian limit. Further into the metallic phase, Fermi-liquid behaviour is recovered at low temperature which evolves into a quantum critical fan at intermediate temperatures before eventually reaching an anomalous saturated regime near room temperature. An analysis of the residual resistivity indicates the presence of strong quantum fluctuations in the insulating phase. These results establish twisted WSe$_2$ as a new platform to study doping and bandwidth controlled metal-insulator quantum phase transitions on the triangular lattice.
The long wavelength moire superlattices in twisted 2D structures have emerged as a highly tunable platform for strongly correlated electron physics. We study the moire bands in twisted transition metal dichalcogenide homobilayers, focusing on WSe$_2$, at small twist angles using a combination of first principles density functional theory, continuum modeling, and Hartree-Fock approximation. We reveal the rich physics at small twist angles $theta<4^circ$, and identify a particular magic angle at which the top valence moire band achieves almost perfect flatness. In the vicinity of this magic angle, we predict the realization of a generalized Kane-Mele model with a topological flat band, interaction-driven Haldane insulator, and Mott insulators at the filling of one hole per moire unit cell. The combination of flat dispersion and uniformity of Berry curvature near the magic angle holds promise for realizing fractional quantum anomalous Hall effect at fractional filling. We also identify twist angles favorable for quantum spin Hall insulators and interaction-induced quantum anomalous Hall insulators at other integer fillings.
Fabricating van der Waals (vdW) bilayer heterostructures (BL-HS) by stacking the same or different two-dimensional (2D) layers, offers a unique physical system with rich electronic and optical properties. Twist-angle between component layers has emerged as a remarkable parameter that can control the period of lateral confinement, and nature of the exciton (Coulomb bound electron-hole pair) in reciprocal space thus creating exotic physical states including moire excitons. In this review article, we focus on opto-electronic properties of excitons in transition metal dichalcogenide (TMD) semiconductor twisted BL-HS. We look at existing evidence of moire excitons in localized and strongly correlated states, and at nanoscale mapping of moire superlattice and lattice-reconstruction. This review will be helpful in guiding the community as well as motivating work in areas such as near-field optical measurements and controlling the creation of novel physical states.
In twisted bilayers of semiconducting transition metal dichalcogenides (TMDs), a combination of structural rippling and electronic coupling gives rise to periodic moire potentials that can confine charged and neutral excitations. Here, we report experimental measurements of the structure and spectroscopic properties of twisted bilayers of WSe2 and MoSe2 in the H-stacking configuration using scanning tunneling microscopy (STM). Our experiments reveal that the moire potential in these bilayers at small angles is unexpectedly large, reaching values of above 300 meV for the valence band and 150 meV for the conduction band - an order of magnitude larger than theoretical estimates based on interlayer coupling alone. We further demonstrate that the moire potential is a non-monotonic function of moire wavelength, reaching a maximum at around a 13nm moire period. This non-monotonicity coincides with a drastic change in the structure of the moire pattern from a continuous variation of stacking order at small moire wavelengths to a one-dimensional soliton dominated structure at large moire wavelengths. We show that the in-plane structure of the moire pattern is captured well by a continuous mechanical relaxation model, and find that the moire structure and internal strain rather than the interlayer coupling is the dominant factor in determining the moire potential. Our results demonstrate the potential of using precision moire structures to create deeply trapped carriers or excitations for quantum electronics and optoelectronics.
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