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The behavior of two-dimensional electron gas (2DEG) in extreme coupling limits are reasonably well-understood, but our understanding of intermediate region remains limited. Strongly interacting electrons crystalize into a solid phase known as the Wigner crystal at very low densities, and these evolve to a Fermi liquid at high densities. At intermediate densities, however, where the Wigner crystal melts into a strongly correlated electron fluid that is poorly understood partly due to a lack of microscopic probes for delicate quantum phases. Here we report the first imaging of a disordered Wigner solid and its quantum densification and quantum melting behavior in a bilayer MoSe2 using a non-invasive scanning tunneling microscopy (STM) technique. We observe a Wigner solid with nanocrystalline domains pinned by local disorder at low hole densities. With slightly increasing electrostatic gate voltages, the holes are added quantum mechanically during the densification of the disordered Wigner solid. As the hole density is increased above a threshold (p ~ 5.7 * 10e12 (cm-2)), the Wigner solid is observed to melt locally and create a mixed phase where solid and liquid regions coexist. With increasing density, the liquid regions gradually expand and form an apparent percolation network. Local solid domains appear to be pinned and stabilized by local disorder over a range of densities. Our observations are consistent with a microemulsion picture of Wigner solid quantum melting where solid and liquid domains emerge spontaneously and solid domains are pinned by local disorder.

Semiconductor moir\'e superlattices provide a versatile platform to engineer new quantum solids composed of artificial atoms on moir\'e sites. Previous studies have mostly focused on the simplest correlated quantum solid - the Fermi-Hubbard model - where intra-atom interactions are simplified to a single onsite repulsion energy U. These studies have revealed novel quantum phases ranging from Mott insulators to quantum anomalous Hall insulators at a filling of one electron per moir\'e unit cell. New types of quantum solids should arise at even higher filling factors where the multi-electron configuration of moir\'e artificial atoms provides new degrees of freedom. Here we report the experimental observation of Wigner molecular crystals emerging from multi-electron artificial atoms in twisted bilayer WS2 moir\'e superlattices. Moir\'e artificial atoms, unlike natural atoms, can host qualitatively different electron states due to the interplay between quantized energy levels and Coulomb interactions. Using scanning tunneling microscopy (STM), we demonstrate that Wigner molecules appear in multi-electron artificial atoms when Coulomb interactions dominate. Three-electron Wigner molecules, for example, are seen to exhibit a characteristic trimer pattern. The array of Wigner molecules observed in a moir\'e superlattice comprises a new crystalline phase of electrons: the Wigner molecular crystal. We show that these Wigner molecular crystals are highly tunable through mechanical strain, moir\'e period, and carrier charge type. Our study presents new opportunities for exploring quantum phenomena in moir\'e quantum solids composed of multi-electron artificial atoms.

Moir\'e superlattices provide a highly tunable and versatile platform to explore novel quantum phases and exotic excited states ranging from correlated insulators1-17 to moir\'e excitons7-10,18. Scanning tunneling microscopy has played a key role in probing microscopic behaviors of the moir\'e correlated ground states at the atomic scale1,11-15,19. Atomic-resolution imaging of quantum excited state in moir\'e heterostructures, however, has been an outstanding experimental challenge. Here we develop a novel photocurrent tunneling microscopy by combining laser excitation and scanning tunneling spectroscopy (laser-STM) to directly visualize the electron and hole distribution within the photoexcited moir\'e exciton in a twisted bilayer WS2 (t-WS2). We observe that the tunneling photocurrent alternates between positive and negative polarities at different locations within a single moir\'e unit cell. This alternating photocurrent originates from the exotic in-plane charge-transfer (ICT) moir\'e exciton in the t-WS2 that emerges from the competition between the electron-hole Coulomb interaction and the moir\'e potential landscape. Our photocurrent maps are in excellent agreement with our GW-BSE calculations for excitonic states in t-WS2. The photocurrent tunneling microscopy creates new opportunities for exploring photoexcited non-equilibrium moir\'e phenomena at the atomic scale.

Moir\'e heterobilayers host interlayer excitons in a natural, periodic array of trapping potentials. Recent work has elucidated the structure of the trapped interlayer excitons and the nature of photoluminescence (PL) from trapped and itinerant charged complexes such as interlayer trions in these structures. In this paper, our results serve to add to the understanding of the nature of PL emission and explain its characteristic blueshift with increasing carrier density, along with demonstrating a significant difference between the interlayer exciton-trion conversion efficiency as compared to both localized and itinerant intra-layer species in conventional monolayers. Our results show the absence of optical generation of trions in these materials, which we suggest arises from the highly localized, near sub-nm confinement of trapped species in these Moir\'e potentials., Comment: 3 figures, Supplementary information available on request

Ultrafast charge transfer processes provide a facile way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated heterostructures composed of TMD/hBN/TMD enable new ways to control interlayer exciton properties and achieve novel exciton phenomena, such as exciton insulators and condensates, where longer lifetimes are desired. In this work, we experimentally study the charge transfer dynamics in a heterostructure composed of a 1 nm thick hBN spacer between MoSe$_{2}$ and WSe$_{2}$ monolayers. We observe the hole transfer from MoSe$_{2}$ to WSe$_{2}$ through the hBN barrier with a time constant of 500 ps, which is over 3 orders of magnitude slower than that between TMD layers without a spacer. Furthermore, we observe strong competition between the interlayer charge transfer and intralayer exciton-exciton annihilation processes at high excitation densities. Our work opens possibilities to understand charge transfer pathways in TMD/hBN/TMD heterostructures for the efficient generation and control of interlayer excitons.

Transition metal dichalcogenide-based moire superlattices exhibit very strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. Here we describe a new scanning single-electron charging (SSEC) spectroscopy technique with nanometer spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS2 moire heterostructures. High-resolution SSEC spectroscopy was achieved by combining scanning tunneling microscopy (STM) with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of order 50meV exist for the 1/3 and 2/3 generalized Wigner crystal states.

The formation of a charge density wave state is characterized by an order parameter. The way it is established provides unique information on both the role that correlation plays in driving the charge density wave formation and the mechanism behind its formation. Here we use time and angle resolved photoelectron spectroscopy to optically perturb the charge-density phase in 1T-TiSe$_2$ and follow the recovery of its order parameter as a function of energy, momentum and excitation density. Our results reveal that two distinct orders contribute to the gap formation, a CDW order and pseudogap-like order, manifested by an overall robustness to optical excitation. A detailed analysis of the magnitude of the the gap as a function of excitation density and delay time reveals the excitonic long-range nature of the CDW gap and the short-range Jahn-Teller character of the pseudogap order. In contrast to the gap, the intensity of the folded Se$_{4p}$* band can only give access to the excitonic order. These results provide new information into the the long standing debate on the origin of the gap in TiSe$_2$ and place it in the same context of other quantum materials where a pseudogap phase appears to be a precursor of long-range order., Comment: 6 pages, 4 figures

A panoply of unconventional electronic states has been observed in moir\'e superlattices. Engineering similar bosonic phases remains, however, largely unexplored. We report the observation of a bosonic correlated insulator in WSe2/WS2 moir\'e superlattices composed of excitons, i.e., tightly bound electron-hole pairs. We develop a pump probe spectroscopy method that we use to observe an exciton incompressible state at exciton filling {\nu}_ex = 1 and charge neutrality, indicating a correlated insulator of excitons. With varying charge density, the bosonic correlated insulator continuously transitions into an electron correlated insulator at charge filling {\nu}_e = 1, suggesting a mixed correlated insulating state between the two limits. Our studies establish semiconducting moir\'e superlattices as an intriguing platform for engineering bosonic phases., Comment: Science (2023)

Charge density waves (CDW) are states of broken symmetry with a periodic modulation of charge and lattice typically leading to the opening of a gap in the band structure. In the model CDW system 1T-TiSe$_2$ such a gap opens up between its Se$_{4p}$ valence and Ti$_{3d}$ conduction band, accompanied by a change of dispersion. These changes are crucial in understanding the CDW phase, as they provide a measure of the Se$_{4p}$-Ti$_{3d}$ hybridization strength and characteristic mechanistic features. Using time- and angle-resolved photoelectron spectroscopy (trARPES), the unoccupied band structure is populated with near-infrared (NIR) pump pulses which allows to to directly visualize the parabolically-shaped Ti$_{3d}$ conduction band. Furthermore, we observe a transient change of effective mass in the Se$_{4p}$ valence band following photoexcitation. This occurs alongside an overall reduction due to weakening of the CDW phase and is accompanied by an oscillating component with the frequency of the characteristic A$_{1g}$ phonon. These observations, enabled by trAPRES, highlight the importance of the lattice contributions in establishing the CDW order in 1T-TiSe$_2$., Comment: 4 figures