Interplay of trapped species and absence of electron capture in Moir\'{e} heterobilayers

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 reques

Bosonic Mott insulator in WSe2/WS2 moir\'e superlattice

A panoply of unconventional electronic states is recently observed in moir\'e superlattices. On the other hand, similar opportunities to engineer bosonic phases remain largely unexplored. Here we report the observation of a bosonic Mott insulator in WSe2/WS2 moir\'e superlattices composed of excitons, i.e., tightly bound electron-hole pairs. Using a novel pump probe spectroscopy, we find an exciton incompressible state at exciton filling v_ex = 1 and charge neutrality, which we assign to a bosonic Mott insulator. When further varying charge density, the bosonic Mott insulator continuously transitions into an electron Mott insulator at charge filling v_e = 1, suggesting a mixed Mott insulating state in between. Our observations are well captured by a mixed Hubbard model involving both fermionic and bosonic components, from which we extract the on-site Coulomb repulsion to be 15meV and 35meV for exciton-exciton and electron-exciton interactions, respectively. Our studies establish semiconducting moir\'e superlattices as intriguing platforms for engineering novel bosonic phases.Comment: 25 pages, 4+10 figure

Wigner Molecular Crystals from Multi-electron Moir\'e Artificial Atoms

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

Reaching the Excitonic Limit in 2D Janus Monolayers by In Situ Deterministic Growth.

Named after the two-faced Roman god of transitions, transition metal dichalcogenide (TMD) Janus monolayers have two different chalcogen surfaces, inherently breaking the out-of-plane mirror symmetry. The broken mirror symmetry and the resulting potential gradient lead to the emergence of quantum properties such as the Rashba effect and the formation of dipolar excitons. Experimental access to these quantum properties, however, hinges on the ability to produce high-quality 2D Janus monolayers. Here, these results introduce a holistic 2D Janus synthesis technique that allows real-time monitoring of the growth process. This prototype chamber integrates in situ spectroscopy, offering fundamental insights into the structural evolution and growth kinetics, that allow the evaluation and optimization of the quality of Janus monolayers. The versatility of this method is demonstrated by synthesizing and monitoring the conversion of SWSe, SNbSe, and SMoSe Janus monolayers. Deterministic conversion and real-time data collection further aid in conversion of exfoliated TMDs to Janus monolayers and unparalleled exciton linewidth values are reached, compared to the current best standard. The results offer an insight into the process kinetics and aid in the development of new Janus monolayers with high optical quality, which is much needed to access their exotic properties

Revealing the order parameter dynamics of 1T-TiSe[Formula: see text] following optical excitation.

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[Formula: see text] 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[Formula: see text]* 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[Formula: see text] and place it in the same context of other quantum materials where a pseudogap phase appears to be a precursor of long-range order

Charge Transfer Dynamics in MoSe2/hBN/WSe2 Heterostructures.

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 MoSe2 and WSe2 monolayers. We observe the hole transfer from MoSe2 to WSe2 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

Correlated insulator of excitons in WSe2/WS2 moiré superlattices

A panoply of unconventional electronic states has been observed in moiré superlattices. Engineering similar bosonic phases remains, however, largely unexplored. We report the observation of a bosonic correlated insulator in tungsten diselenide/tungsten disulfide (WSe2/WS2) moiré superlattices composed of excitons, that is, tightly bound electron-hole pairs. We develop a pump probe spectroscopy method that we use to observe an exciton incompressible state at exciton filling νex = 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 νe = 1, suggesting a mixed correlated insulating state between the two limits. Our studies establish semiconducting moiré superlattices as an intriguing platform for engineering bosonic phases

Charge transfer dynamics in MoSe2_{2}/hBN/WSe2_{2} heterostructures

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

Charge Transfer Dynamics in MoSe₂/hBN/WSe₂ Heterostructures

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 MoSe2 and WSe2 monolayers. We observe the hole transfer from MoSe2 to WSe2 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