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Register a new userObservation of Moire Excitons in WSe2/WS2 Heterostructure Superlattices
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Moire superlattices provide a powerful tool to engineer novel quantum phenomena in two-dimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moire superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moire superlattices. In addition to their dramatic effects on the single particle states, moire superlattices were recently predicted to host novel excited states, such as moire exciton bands. Here we report the first observation of moire superlattice exciton states in nearly aligned WSe2/WS2 heterostructures. These moire exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe2 monolayers and in large-twist-angle WSe2/WS2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moire potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moire exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.
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Stripe phases, in which the rotational symmetry of charge density is spontaneously broken, occur in many strongly correlated systems with competing interactions. One representative example is the copper-oxide superconductors, where stripe order is thought to be relevant to the mechanism of high-temperature superconductivity. Identifying and studying the stripe phases in conventional strongly correlated systems are, however, challenging due to the complexity and limited tunability of these materials. Here we uncover stripe phases in WSe2/WS2 moire superlattices with continuously gate-tunable charge densities by combining optical anisotropy and electronic compressibility measurements. We find strong electronic anisotropy over a large doping range peaked at 1/2 filling of the moire superlattice. The 1/2-state is incompressible and assigned to a (insulating) stripe crystal phase. It can be continuously melted by thermal fluctuations around 35 K. The domain configuration revealed by wide-field imaging shows a preferential alignment along the high-symmetry axes of the moire superlattice. Away from 1/2 filling, we observe additional stripe crystals at commensurate filling 1/4, 2/5 and 3/5. The anisotropy also extends into the compressible regime of the system at incommensurate fillings, indicating the presence of electronic liquid crystal states. The observed filling-dependent stripe phases agree with the theoretical phase diagram of the extended Hubbard model on a triangular lattice in the flat band limit. Our results demonstrate that two-dimensional semiconductor moire superlattices are a highly tunable platform to study the stripe phases and their interplay with other symmetry breaking ground states.
Moire superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moire flat bands and strong, long-range Coulomb interactions1-5. However, microscopic knowledge of the atomically-reconstructed moire superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moire phenomena. Here we quantitatively study the moire flat bands in three-dimensional (3D) reconstructed WSe2/WS2 moire superlattices by comparing scanning tunneling spectroscopy (STS) of high quality exfoliated TMD heterostructure devices with ab initio simulations of TMD moire superlattices. A strong 3D buckling reconstruction accompanied by large in-plane strain redistribution is identified in our WSe2/WS2 moire heterostructures. STS imaging demonstrates that this results in a remarkably narrow and highly localized K-point moire flat band at the valence band edge of the heterostructure. A series of moire flat bands are observed at different energies that exhibit varying degrees of localization. Our observations contradict previous simplified theoretical models but agree quantitatively with ab initio simulations that fully capture the 3D structural reconstruction. Here the strain redistribution and 3D buckling dominate the effective moire potential and result in moire flat bands at the Brillouin zone K points.
We report the nanoscale conductivity imaging of correlated electronic states in angle-aligned WSe2/WS2 heterostructures using microwave impedance microscopy. The noncontact microwave probe allows us to observe the Mott insulating state with one hole per moire unit cell that persists for temperatures up to 150 K, consistent with other characterization techniques. In addition, we identify for the first time a Mott insulating state at one electron per moire unit cell. Appreciable inhomogeneity of the correlated states is directly visualized in the hetero-bilayer region, indicative of local disorders in the moire superlattice potential or electrostatic doping. Our work provides important insights on 2D moire systems down to the microscopic level.
Transition metal dichalcogenide (TMD) moire heterostructures provide an ideal platform to explore the extended Hubbard model1 where long-range Coulomb interactions play a critical role in determining strongly correlated electron states. This has led to experimental observations of Mott insulator states at half filling2-4 as well as a variety of extended Wigner crystal states at different fractional fillings5-9. Microscopic understanding of these emerging quantum phases, however, is still lacking. Here we describe a novel scanning tunneling microscopy (STM) technique for local sensing and manipulation of correlated electrons in a gated WS2/WSe2 moire superlattice that enables experimental extraction of fundamental extended Hubbard model parameters. We demonstrate that the charge state of local moire sites can be imaged by their influence on STM tunneling current, analogous to the charge-sensing mechanism in a single-electron transistor. In addition to imaging, we are also able to manipulate the charge state of correlated electrons. Discharge cascades of correlated electrons in the moire superlattice are locally induced by ramping the STM bias, thus enabling the nearest-neighbor Coulomb interaction (UNN) to be estimated. 2D mapping of the moire electron charge states also enables us to determine onsite energy fluctuations at different moire sites. Our technique should be broadly applicable to many semiconductor moire systems, offering a powerful new tool for microscopic characterization and control of strongly correlated states in moire superlattices.
Moire superlattices are emerging as a new route for engineering strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states in magic-angle twisted bilayer graphene and ABC trilayer graphene/boron nitride moire superlattices. Transition metal dichalcogenide (TMDC) moire heterostructures provide another exciting model system to explore correlated quantum phenomena, with the addition of strong light-matter interactions and large spin-orbital coupling. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moire superlattices. Our sensitive optical detection technique reveals a Mott insulator state at one hole per superlattice site ({ u} = 1), and surprising insulating phases at fractional filling factors { u} = 1/3 and 2/3, which we assign to generalized Wigner crystallization on an underlying lattice. Furthermore, the unique spin-valley optical selection rules of TMDC heterostructures allow us to optically create and investigate low-energy spin excited states in the Mott insulator. We reveal an especially slow spin relaxation lifetime of many microseconds in the Mott insulating state, orders-of-magnitude longer than that of charge excitations. Our studies highlight novel correlated physics that can emerge in moire superlattices beyond graphene.
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