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Two-dimensional semiconductors and their moir\'e superlattices have emerged as important platforms for investigating correlated electrons. However, many key properties of these systems, such as the frequency-dependent conductivity, remain experimentally inaccessible because of the mesoscopic sample size. Here we report a technique to directly measure the complex conductivity of electrostatically gated two-dimensional semiconductors in the terahertz frequency range. Applying this technique to a WSe2 monolayer encapsulated in hBN, we observe clear Drude-like response between 0.1 and 1 THz, in a density range challenging to access even in DC transport. Our work opens a new avenue for studying tunable van der Waals heterostructures using terahertz spectroscopy.

Advanced microelectronics in the future may require semiconducting channel materials beyond silicon. Two-dimensional (2D) semiconductors, characterized by their atomically thin thickness, hold immense promise for high-performance electronic devices at the nanometer scale with lower heat dissipation. One challenge for achieving high-performance 2D semiconductor field effect transistors (FET), especially for p-type materials, is the high electrical contact resistance present at the metal-semiconductor interface. In conventional bulk semiconductors, low resistance ohmic contact is realized through heavy substitutional doping with acceptor or donor impurities at the contact region. The strategy of substitutional doping, however, does not work for p-type 2D semiconductors such as monolayer tungsten diselenide (WSe$_2$).In this study, we developed highly efficient charge-transfer doping with WSe$_2$/$\alpha$-RuCl$_3$ heterostructures to achieve low-resistance ohmic contact for p-type WSe$_2$ transistors. We show that a hole doping as high as 3$\times$10$^{13}$ cm$^{-2}$ can be achieved in the WSe$_2/\alpha$-RuCl$_3$ heterostructure due to its type-III band alignment. It results in an Ohmic contact with resistance lower than 4 k Ohm $\mu$m at the p-type monolayer WSe$_2$/metal junction. at room temperature. Using this low-resistance contact, we demonstrate high-performance p-type WSe$_2$ transistors with a saturation current of 35 $\mu$A$\cdot$ $\mu$m$^{-1}$ and an I$_{ON}$/I$_{OFF}$ ratio exceeding 10$^9$ It could enable future microelectronic devices based on 2D semiconductors and contribute to the extension of Moore's law.

The combination of repulsive and attractive Coulomb interactions in a quantum electron(e)-hole(h) fluid can give rise to novel correlated phases of multiparticle charge complexes such as excitons, trions and biexcitons. Here we report the first experimental realization of an electrically controlled interlayer trion fluid in two-dimensional van der Waals heterostructures. We demonstrate that in the strong coupling regime of electron-hole bilayers, electrons and holes in separate layers can spontaneously form three-particle trion bound states that resemble positronium ions in high energy physics. The interlayer trions can assume 1e-2h and 2e-1h configurations, where electrons and holes are confined in different transition metal dichalcogenide layers. We show that the two correlated holes in 1e-2h trions form a spin-singlet state with a spin gap of ~1meV. By electrostatic gating, the equilibrium state of our system can be continuously tuned into an exciton fluid, a trion fluid, an exciton-trion mixture, a trion-charge mixture or an electron-hole plasma. Upon optical excitation, the system can host novel high-order multiparticle charge complexes including interlayer four-particle complex (tetrons) and five-particle complex (pentons). Our work demonstrates a unique platform to study novel correlated phases of tunable Bose-Fermi mixtures and opens up new opportunities to realize artificial ions/molecules in electronic devices.

Strongly coupled two-dimensional electron-hole bilayers can give rise to novel quantum Bosonic states: electrons and holes in electrically isolated layers can pair into interlayer excitons, which can form a Bose-Einstein condensate below a critical temperature at zero magnetic field. This state is predicted to feature perfect Coulomb drag, where a current in one layer must be accompanied by an equal but opposite current in the other, and counterflow superconductivity, where the excitons form a superfluid with zero viscosity. Electron-hole bilayers in the strong coupling limit with an excitonic insulator ground state have been recently achieved in semiconducting transition metal dichalcogenide heterostructures, but direct electrical transport measurements remain challenging. Here we use a novel optical spectroscopy to probe the electrical transport of correlated electron-hole fluids in MoSe2/hBN/WSe2 heterostructures. We observe perfect Coulomb drag in the excitonic insulator phase up to a temperature as high as ~15K. Strongly correlated electron and hole transport is also observed at unbalanced electron and hole densities, although the Coulomb drag is not perfect anymore. Meanwhile, the counterflow resistance of interlayer excitons remains finite. These results indicate the formation of an exciton gas in the excitonic insulator which does not condensate into a superfluid at low temperature. Our work also demonstrates that dynamic optical spectroscopy provides a powerful tool for probing novel exciton transport behavior and possible exciton superfluidity in correlated quantum electron-hole fluids.

Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton superfluids. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe2/hBN/WSe2 heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~$0.8\times {10}^{12} \mathrm{cm}^{-2}$ and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems.

Wigner crystals are predicted as the crystallization of the dilute electron gas moving in a uniform background when the electron-electron Coulomb energy dominates the kinetic energy. The Wigner crystal has previously been observed in the ultraclean two-dimensional electron gas (2DEG) present on the surface of liquid helium and in semiconductor quantum wells at high magnetic field. More recently, Wigner crystals have also been reported in WS2/WSe2 moir\'e heterostructures. ABC-stacked trilayer graphene on boron nitride (ABC-TLG/hBN) moir\'e superlattices provide a unique tunable platform to explore Wigner crystal states where the electron correlation can be controlled by electric and magnetic field. Here we report the observation of magnetic field stabilized Wigner crystal states in a ABC-TLG/hBN moir\'e superlattice. We show that correlated insulating states emerge at multiple fractional and integer fillings corresponding to v = 1/3, 2/3, 1, 4/3, 5/3 and 2 electrons per moir\'e lattice site under a magnetic field. These correlated insulating states can be attributed to generalized Mott states for the integer fillings (v = 1, 2) and generalized Wigner crystal states for the fractional fillings (v = 1/3, 2/3, 4/3, 5/3). The generalized Wigner crystal states are stabilized by a vertical magnetic field, and they are strongest at one magnetic flux quantum per three moir\'e superlattices. The correlated insulating states at v = 2 persists up to 30 Tesla, which can be described by a Mott-Hofstadter transition at high magnetic field. The tunable Mott and Wigner crystal states in the ABC-TLG/hBN highlight the opportunities to discover new correlated quantum phases due to the interplay between the magnetic field and moir\'e flatbands., Comment: 19 pages, 6 figures

Moir\'e potentials in two-dimensional materials have been proven to be of fundamental importance to fully understand the electronic structure of van der Waals heterostructures, from superconductivity to correlated excitonic states. However, understanding how the moir\'e phonons, so-called phasons, affect the properties of the system still remains an uncharted territory. In this work, we demonstrate how phasons are integral to properly describing and understanding low-temperature interlayer exciton diffusion in WS2/WSe2 heterostructure. We perform photoluminescence (PL) spectroscopy to understand how the coupling between the layers, affected by their relative orientation, impacts the excitonic properties of the system. Samples fabricated with stacking angles of 0{\deg} and 60{\deg} are investigated taking into account the stacking angle dependence of the two common moir\'e potential profiles. Additionally, we present spatially and time-resolved exciton diffusion measurements, looking at the photoluminescence emission in a temperature range from 30 K to 250 K. An accurate potential for the two configurations are computed via density functional theory (DFT) calculations. Finally, we perform molecular dynamics simulation in order to visualize the phasons motion, estimating the phason speed at different temperatures, providing novel insights into the mechanics of exciton propagation at low temperatures that cannot be explained within the frame of classical exciton diffusion alone., Comment: A. Rossi, J. Zipfel, and I. Maity contributed equally

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.

Moir\'e patterns of transition metal dichalcogenide (TMD) heterobilayers have proven to be an ideal platform to host unusual correlated electronic phases, emerging magnetism, and correlated exciton physics. While the existence of novel moir\'e excitonic states is established through optical measurements, the microscopic nature of these states is still poorly understood, often relying on empirically fit models. Here, combining large-scale first-principles GW-BSE calculations and micro-reflection spectroscopy, we identify the nature of the exciton resonances in WSe$_2$/WS$_2$ moir\'e superlattices, discovering a surprisingly rich set of moir\'e excitons that cannot be even qualitatively captured by prevailing continuum models. Our calculations reveal moir\'e excitons with distinct characters, including modulated Wannier excitons and previously unindentified intralayer charge-transfer excitons. Signatures of these distinct excitonic characters are confirmed experimentally via the unique carrier-density and magnetic-field dependences of different moir\'e exciton resonances. Our study highlights the highly non-trivial exciton states that can emerge in TMD moir\'e superlattices, and suggests novel ways of tuning many-body physics in moir\'e systems by engineering excited-states with specific spatial characters.

Moir\'e superlattices in van der Waals heterostructures have emerged as a powerful tool for engineering novel quantum phenomena. Here we report the observation of a correlated interlayer exciton insulator in a double-layer heterostructure composed of a WSe2 monolayer and a WS2/WSe2 moir\'e bilayer that are separated by an ultrathin hexagonal boron nitride (hBN). The moir\'e WS2/WSe2 bilayer features a Mott insulator state at hole density p/p0 = 1, where p0 corresponds to one hole per moir\'e lattice site. When electrons are added to the Mott insulator in the WS2/WSe2 moir\'e bilayer and an equal number of holes are injected into the WSe2 monolayer, a new interlayer exciton insulator emerges with the holes in the WSe2 monolayer and the electrons in the doped Mott insulator bound together through interlayer Coulomb interactions. The excitonic insulator is stable up to a critical hole density of ~ 0.5p0 in the WSe2 monolayer, beyond which the system becomes metallic. Our study highlights the opportunities for realizing novel quantum phases in double-layer moir\'e systems due to the interplay between the moir\'e flat band and strong interlayer electron interactions.

The advent of black phosphorus field-effect transistors (FETs) has brought new possibilities in the study of two-dimensional (2D) electron systems. In a black phosphorus FET, the gate induces highly anisotropic 2D electron and hole gases. Although the 2D hole gas in black phosphorus has reached high carrier mobilities that led to the observation of the integer quantum Hall effect, the improvement in the sample quality of the 2D electron gas (2DEG) has however been only moderate; quantum Hall effect remained elusive. Here, we obtain high quality black phosphorus 2DEG by defining the 2DEG region with a prepatterned graphite local gate. The graphite local gate screens the impurity potential in the 2DEG. More importantly, it electrostatically defines the edge of the 2DEG, which facilitates the formation of well-defined edge channels in the quantum Hall regime. The improvements enable us to observe precisely quantized Hall plateaus in electron-doped black phosphorus FET. Magneto-transport measurements under high magnetic fields further revealed a large effective mass and an enhanced Land\'e g-factor, which points to strong electron-electron interaction in black phosphorus 2DEG. Such strong interaction may lead to exotic many-body quantum states in the fractional quantum Hall regime., Comment: Accepted in Nano Letters

The interplay between magnetism and topology, as exemplified in the magnetic skyrmion systems, has emerged as a rich playground for finding novel quantum phenomena and applications in future information technology. Magnetic topological insulators (TI) have attracted much recent attention, especially after the experimental realization of quantum anomalous Hall effect. Future applications of magnetic TI hinge on the accurate manipulation of magnetism and topology by external perturbations, preferably with a gate electric field. In this work, we investigate the magneto transport properties of Cr doped Bi2(SexTe1-x)3 TI across the topological quantum critical point (QCP). We find that the external gate voltage has negligible effect on the magnetic order for samples far away from the topological QCP. But for the sample near the QCP, we observe a ferromagnetic (FM) to paramagnetic (PM) phase transition driven by the gate electric field. Theoretical calculations show that a perpendicular electric field causes a shift of electronic energy levels due to the Stark effect, which induces a topological quantum phase transition and consequently a magnetic phase transition. The in situ electrical control of the topological and magnetic properties of TI shed important new lights on future topological electronic or spintronic device applications., Comment: 20 pages, 4 figures, to appear in Nature Nanotechnology

Energy bandgap largely determines the optical and electronic properties of a semiconductor. Variable bandgap therefore makes versatile functionality possible in a single material. In layered material black phosphorus, the bandgap can be modulated by the number of layers; as a result, few-layer black phosphorus has discrete bandgap values that are relevant for opto-electronic applications in the spectral range from red, in monolayer, to mid-infrared in the bulk limit. Here, we further demonstrate continuous bandgap modulation by mechanical strain applied through flexible substrates. The strain-modulated bandgap significantly alters the charge transport in black phosphorus at room temperature; we for the first time observe a large piezo-resistive effect in black phosphorus field-effect transistors (FETs). The effect opens up opportunities for future development of electro-mechanical transducers based on black phosphorus, and we demonstrate strain gauges constructed from black phosphorus thin crystals.

The quantized version of the anomalous Hall effect has been predicted to occur in magnetic topological insulators, but the experimental realization has been challenging. Here, we report the observation of the quantum anomalous Hall (QAH) effect in thin films of Cr-doped (Bi,Sb)2Te3, a magnetic topological insulator. At zero magnetic field, the gate-tuned anomalous Hall resistance reaches the predicted quantized value of h/e^2,accompanied by a considerable drop of the longitudinal resistance. Under a strong magnetic field, the longitudinal resistance vanishes whereas the Hall resistance remains at the quantized value. The realization of the QAH effect may lead to the development of low-power-consumption electronics., Comment: 11 pages, 4 figures

Phosphorene, a single atomic layer of black phosphorus, has recently emerged as a new twodimensional (2D) material that holds promise for electronic and photonic technology. Here we experimentally demonstrate that the electronic structure of few-layer phosphorene varies significantly with the number of layers, in good agreement with theoretical predictions. The interband optical transitions cover a wide, technologically important spectrum range from visible to mid-infrared. In addition, we observe strong photoluminescence in few-layer phosphorene at energies that match well with the absorption edge, indicating they are direct bandgap semiconductors. The strongly layer-dependent electronic structure of phosphorene, in combination with its high electrical mobility, gives it distinct advantages over other twodimensional materials in electronic and opto-electronic applications., Comment: 17 pages, 4 figures, Likai Li, Jonghwan Kim, Chenhao Jin contributed equally to this work

Interface-enhanced high-temperature superconductivity in one unit-cell (UC) FeSe film on SrTiO3(001) (STO) substrate has recently attracted much attention in condensed matter physics and material science. Here, by ex situ transport measurements, we report on the superconductivity in FeSe ultra-thin films with different thickness on STO substrate. We find that the onset superconducting transition temperature (Tc) decreases with increasing film thickness of FeSe, which is opposite to the behavior usually observed in traditional superconductor films. By systematic post-annealing of 5 UC FeSe films, we observe an insulator to superconductor transition, which is accompanied with a sign change of the dominated charge carriers from holes to electrons at low temperatures according to the corresponding Hall measurement.

We report the Meissner effect studies on an FeSe thin film grown on Nb doped SrTiO3 substrate by molecular beam epitaxy. Two-coil mutual inductance measurement clearly demonstrates the onset of diamagnetic screening at 65 K, which is consistent with the gap opening temperature determined by previous angle resolved photoemission spectroscopy results. The applied magnetic field causes a broadening of the superconducting transition near the onset temperature, which is the typical behavior for quasi-two-dimensional superconductors. Our results provide direct evidence that FeSe thin film grown on Nb doped SrTiO3 substrate has an onset TC ~ 65 K, which is the highest among all iron based superconductors discovered so far., Comment: 9 pages, 3 figures, updated reference list

Development of new, high quality functional materials has been at the forefront of condensed matter research. The recent advent of two-dimensional black phosphorus has greatly enriched the material base of two-dimensional electron systems. Significant progress has been made to achieve high mobility black phosphorus two-dimensional electron gas (2DEG) since the development of the first black phosphorus field-effect transistors (FETs)$^{1-4}$. Here, we reach a milestone in developing high quality black phosphorus 2DEG - the observation of integer quantum Hall (QH) effect. We achieve high quality by embedding the black phosphorus 2DEG in a van der Waals heterostructure close to a graphite back gate; the graphite gate screens the impurity potential in the 2DEG, and brings the carrier Hall mobility up to 6000 $cm^{2}V^{-1}s^{-1}$. The exceptional mobility enabled us, for the first time, to observe QH effect, and to gain important information on the energetics of the spin-split Landau levels in black phosphorus. Our results set the stage for further study on quantum transport and device application in the ultrahigh mobility regime.

We report transport studies on (Bi,Sb)2Te3 topological insulator thin films with tunable electronic band structure. We find a doping and temperature regime in which the Hall coefficient is negative indicative of electron-type carriers, whereas the Seebeck coefficient is positive indicative of hole-type carriers. This sign anomaly is due to the distinct transport behaviors of the bulk and surface states: the surface Dirac fermions dominate magnetoelectric transport while the thermoelectric effect is mainly determined by the bulk states. These findings may inspire new ideas for designing topological insulator-based high efficiency thermoelectric devices., Comment: 9 figures

It is crucial for the studies of the transport properties and quantum effects related to Dirac surface states of three-dimensional topological insulators (3D TIs) to be able to simultaneously tune the chemical potentials of both top and bottom surfaces of a 3D TI thin film. We have realized this in molecular beam epitaxy-grown thin films of 3D TIs, as well as magnetic 3D TIs, by fabricating dual-gate structures on them. The films could be tuned between n-type and p-type by each gate alone. Combined application of two gates can reduce the carrier density of a TI film to a much lower level than with only one of them and enhance the film resistance by 10000 %, implying that Fermi level is tuned very close to the Dirac points of both top and bottom surface states without crossing any bulk band. The result promises applications of 3D TIs in field effect devices., Comment: 19 pages, 4 figures, accepted by Nano Letters, forthcoming

With angle-resolved photoemission spectroscopy, gap-opening is resolved at up to room temperature in the Dirac surface states of molecular beam epitaxy grown Cr-doped Bi2Se3 topological insulator films, which however show no long-range ferromagnetic order down to 1.5 K. The gap size is found decreasing with increasing electron doping level. Scanning tunneling microscopy and first principles calculations demonstrate that substitutional Cr atoms aggregate into superparamagnetic multimers in Bi2Se3 matrix, which contribute to the observed chemical potential dependent gap-opening in the Dirac surface states without long-range ferromagnetic order., Comment: 20 pages, 4 figures

The Dirac-like surface states of the topological insulators (TIs) are protected by time reversal symmetry (TRS) and exhibit a host of novel properties. Introducing magnetism into TI, which breaks the TRS, is expected to create exotic topological magnetoelectric effects. A particularly intriguing phenomenon in this case is the magnetic field dependence of electrical resistance, or magnetoresistance (MR). The intricate interplay between topological protection and broken-TRS may lead to highly unconventional MR behaviour that can find unique applications in magnetic sensing and data storage. However, so far the MR of TI with spontaneously broken TRS is still poorly understood, mainly due to the lack of well-controlled experiments. In this work, we investigate the magneto transport properties of a ferromagnetic TI thin film fabricated into a field effect transistor device. We observe an unusually complex evolution of MR when the Fermi level (EF) is tuned across the Dirac point (DP) by gate voltage. In particular, MR tends to be positive when EF lies close to the DP but becomes negative at higher energies. This trend is opposite to that expected from the Berry phase picture for localization, but is intimately correlated with the gate-tuned magnetic order. We show that the underlying physics is the competition between the topology-induced weak antilocalization and magnetism-induced negative MR. The simultaneous electrical control of magnetic order and magneto transport facilitates future TI-based spintronic devices., Comment: 4 figures, supplementary information included