Coherent Modulation of Two-Dimensional Moiré States with On-Chip THz Waves.

van der Waals (vdW) structures host a broad range of physical phenomena. New opportunities arise if different functional layers are remotely modulated or coupled in a device structure. Here we demonstrate the in situ coherent modulation of moiré excitons and correlated Mott insulators in transition metal dichalcogenide (TMD) moirés with on-chip terahertz (THz) waves. Using common dual-gated device structures of a TMD moiré bilayer sandwiched between two few-layer graphene (fl-Gr) gates with hexagonal boron nitride (h-BN) spacers, we launch coherent phonon wavepackets at ∼0.4-1 THz from the fl-Gr gates by femtosecond laser excitation. The waves travel through the h-BN spacer, arrive at the TMD bilayer with precise timing, and coherently modulate the moiré excitons or Mott states. These results demonstrate that the fl-Gr gates, often used for electrical control, can serve as on-chip opto-elastic transducers to generate THz waves for coherent control and vibrational entanglement of functional layers in moiré devices.

Two-Dimensional Moiré Polaronic Electron Crystals.

Two-dimensional moiré materials have emerged as the most versatile platform for realizing quantum phases of electrons. Here, we explore the stability origins of correlated states in WSe_{2}/WS_{2} moiré superlattices. We find that ultrafast electronic excitation leads to partial melting of the Mott states on timescales 5 times longer than predictions from the charge hopping integrals and that the melting rates are thermally activated, with activation energies of 18±3 and 13±2 meV for the one- and two-hole Mott states, respectively, suggesting significant electron-phonon coupling. A density functional theory calculation of the one-hole Mott state confirms polaron formation and yields a hole-polaron binding energy of 16 meV. These findings reveal a close interplay of electron-electron and electron-phonon interactions in stabilizing the polaronic Mott insulators at transition metal dichalcogenide moiré interfaces.

Enabling Waveguide Optics in Rhombohedral-Stacked Transition Metal Dichalcogenides with Laser-Patterned Grating Couplers.

Waveguides play a key role in the implementation of on-chip optical elements and, therefore, lie at the heart of integrated photonics. To add the functionalities of layered materials to existing technologies, dedicated fabrication protocols are required. Here, we build on laser writing to pattern grating structures into bulk noncentrosymmetric transition metal dichalcogenides with grooves as sharp as 250 nm. Using thin flakes of 3R-MoS2 that act as waveguides for near-infrared light, we demonstrate the functionality of the grating couplers with two complementary experiments: first, nano-optical imaging is used to visualize transverse electric and magnetic modes, whose directional outcoupling is captured by finite element simulations. Second, waveguide second-harmonic generation is demonstrated by grating-coupling femtosecond pulses into the slabs in which the radiation partially undergoes frequency doubling throughout the propagation. Our work provides a straightforward strategy for laser patterning of van der Waals crystals, demonstrates the feasibility of compact frequency converters, and examines the tuning knobs that enable optimized coupling into layered waveguides.

Visualizing moiré ferroelectricity via plasmons and nano-photocurrent in graphene/twisted-WSe2 structures.

Ferroelectricity, a spontaneous and reversible electric polarization, is found in certain classes of van der Waals (vdW) materials. The discovery of ferroelectricity in twisted vdW layers provides new opportunities to engineer spatially dependent electric and optical properties associated with the configuration of moiré superlattice domains and the network of domain walls. Here, we employ near-field infrared nano-imaging and nano-photocurrent measurements to study ferroelectricity in minimally twisted WSe2. The ferroelectric domains are visualized through the imaging of the plasmonic response in a graphene monolayer adjacent to the moiré WSe2 bilayers. Specifically, we find that the ferroelectric polarization in moiré domains is imprinted on the plasmonic response of the graphene. Complementary nano-photocurrent measurements demonstrate that the optoelectronic properties of graphene are also modulated by the proximal ferroelectric domains. Our approach represents an alternative strategy for studying moiré ferroelectricity at native length scales and opens promising prospects for (opto)electronic devices.

Visualizing delocalized correlated electronic states in twisted double bilayer graphene.

The discovery of interaction-driven insulating and superconducting phases in moiré van der Waals heterostructures has sparked considerable interest in understanding the novel correlated physics of these systems. While a significant number of studies have focused on twisted bilayer graphene, correlated insulating states and a superconductivity-like transition up to 12 K have been reported in recent transport measurements of twisted double bilayer graphene. Here we present a scanning tunneling microscopy and spectroscopy study of gate-tunable twisted double bilayer graphene devices. We observe splitting of the van Hove singularity peak by ~20 meV at half-filling of the conduction flat band, with a corresponding reduction of the local density of states at the Fermi level. By mapping the tunneling differential conductance we show that this correlated system exhibits energetically split states that are spatially delocalized throughout the different regions in the moiré unit cell, inconsistent with order originating solely from onsite Coulomb repulsion within strongly-localized orbitals. We have performed self-consistent Hartree-Fock calculations that suggest exchange-driven spontaneous symmetry breaking in the degenerate conduction flat band is the origin of the observed correlated state. Our results provide new insight into the nature of electron-electron interactions in twisted double bilayer graphene and related moiré systems.

Ultrahigh-resolution scanning microwave impedance microscopy of moiré lattices and superstructures.

Two-dimensional heterostructures composed of layers with slightly different lattice vectors exhibit new periodic structure known as moiré lattices, which, in turn, can support novel correlated and topological phenomena. Moreover, moiré superstructures can emerge from multiple misaligned moiré lattices or inhomogeneous strain distributions, offering additional degrees of freedom in tailoring electronic structure. High-resolution imaging of the moiré lattices and superstructures is critical for understanding the emerging physics. Here, we report the imaging of moiré lattices and superstructures in graphene-based samples under ambient conditions using an ultrahigh-resolution implementation of scanning microwave impedance microscopy. Although the probe tip has a gross radius of ~100 nm, spatial resolution better than 5 nm is achieved, which allows direct visualization of the structural details in moiré lattices and the composite super-moiré. We also demonstrate artificial synthesis of novel superstructures, including the Kagome moiré arising from the interplay between different layers.