Showing papers by "James Hone published in 2021"

Moiré heterostructures as a condensed-matter quantum simulator

Abstract: Twisted van der Waals heterostructures have latterly received prominent attention for their many remarkable experimental properties and the promise that they hold for realizing elusive states of matter in the laboratory We propose that these systems can, in fact, be used as a robust quantum simulation platform that enables the study of strongly correlated physics and topology in quantum materials Among the features that make these materials a versatile toolbox are the tunability of their properties through readily accessible external parameters such as gating, straining, packing and twist angle; the feasibility to realize and control a large number of fundamental many-body quantum models relevant in the field of condensed-matter physics; and finally, the availability of experimental readout protocols that directly map their rich phase diagrams in and out of equilibrium This general framework makes it possible to robustly realize and functionalize new phases of matter in a modular fashion, thus broadening the landscape of accessible physics and holding promise for future technological applications Moire heterostructures have latterly captured the attention of condensed-matter physicists This Review Article explores the idea of adopting them as a quantum simulation platform that enables the study of strongly correlated physics and topology in quantum materials

Evidence of high-temperature exciton condensation in 2D atomic double layers

Abstract: A Bose-Einstein condensate is the ground state of a dilute gas of bosons, such as atoms cooled to temperatures close to absolute zero. With much smaller mass, excitons (bound electron-hole pairs) are expected to condense at significantly higher temperatures. Here we study electrically generated interlayer excitons in MoSe2/WSe2 atomic double layers with density up to 10^12 cm-2. The interlayer tunneling current depends only on exciton density, indicative of correlated electron-hole pair tunneling. Strong electroluminescence (EL) arises when a hole tunnels from WSe2 to recombine with electron in MoSe2. We observe a critical threshold dependence of the EL intensity on exciton density, accompanied by a super-Poissonian photon statistics near threshold, and a large EL enhancement peaked narrowly at equal electron-hole densities. The phenomenon persists above 100 K, which is consistent with the predicted critical condensation temperature. Our study provides compelling evidence for interlayer exciton condensation in two-dimensional atomic double layers and opens up exciting opportunities for exploring condensate-based optoelectronics and exciton-mediated high-temperature superconductivity.

Stripe phases in WSe2/WS2 moiré superlattices

Abstract: Stripe phases, in which the rotational symmetry of charge density is spontaneously broken, occur in many strongly correlated systems with competing interactions1-11. However, identifying and studying such stripe phases remains challenging. Here we uncover stripe phases in WSe2/WS2 moire superlattices 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 an insulating stripe crystal phase. Wide-field imaging reveals domain configurations with 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, and compressible electronic liquid crystal states at incommensurate fillings. Our results demonstrate that two-dimensional semiconductor moire superlattices are a highly tunable platform from which to study the stripe phases and their interplay with other symmetry breaking ground states.

Quantum Criticality in Twisted Transition Metal Dichalcogenides

Abstract: In moir\'e heterostructures, gate-tunable insulating phases driven by electronic correlations have been recently discovered. Here, we use transport measurements to characterize the gate-driven metal-insulator transitions and the metallic phase in twisted WSe$_2$ near half filling of the first moir\'e subband. We find that the metal-insulator transition as a function of both density and displacement field is continuous. At the metal-insulator boundary, the resistivity displays strange metal behaviour at low temperature with dissipation comparable to the Planckian limit. Further into the metallic phase, Fermi-liquid behaviour is recovered at low temperature which evolves into a quantum critical fan at intermediate temperatures before eventually reaching an anomalous saturated regime near room temperature. An analysis of the residual resistivity indicates the presence of strong quantum fluctuations in the insulating phase. These results establish twisted WSe$_2$ as a new platform to study doping and bandwidth controlled metal-insulator quantum phase transitions on the triangular lattice.

Deep moiré potentials in twisted transition metal dichalcogenide bilayers

Abstract: In twisted bilayers of semiconducting transition metal dichalcogenides, a combination of structural rippling and electronic coupling gives rise to periodic moire potentials that can confine charged and neutral excitations1–5. Here we show that the moire potential in these bilayers at small angles is unexpectedly large, reaching values above 300 meV for the valence band and 150 meV for the conduction band—an order of magnitude larger than theoretical estimates based on interlayer coupling alone. We further demonstrate that the moire potential is a non-monotonic function of moire wavelength, reaching a maximum at a moire period of ~13 nm . This non-monotonicity coincides with a change in the structure of the moire pattern from a continuous variation of stacking order at small moire wavelengths to a one-dimensional soliton-dominated structure at large moire wavelengths. We show that the in-plane structure of the moire pattern is captured by a continuous mechanical relaxation model, and find that the moire structure and internal strain, rather than the interlayer coupling, are the dominant factors in determining the moire potential. Our results demonstrate the potential of using precision moire structures to create deeply trapped carriers or excitations for quantum electronics and opto-electronics. The electrical potential created by a moire pattern in twisted transition metal dichalcogenide bilayers can be surprisingly deep, trapping electrons that can possibly be used for opto-electronic or quantum simulation applications.

Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides

Abstract: Van der Waals (vdW) materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit emergent physical properties absent in the parent compounds through interlayer interactions. Here we report on a new family of emergent, nanometer-thick, semiconductor 2D ferroelectrics, where the individual constituents are well-studied non-ferroelectric monolayer transition metal dichalcogenides (TMDs), namely WSe2, MoSe2, WS2, and MoS2. By stacking two identical monolayer TMDs in parallel, we obtain electrically switchable rhombohedral-stacking configurations, with out-of-plane polarization that is flipped by in-plane sliding motion. Fabricating nearly-parallel stacked bilayers enables the visualization of moir\'e ferroelectric domains as well as electric-field-induced domain wall motion with piezoelectric force microscopy (PFM). Furthermore, by using a nearby graphene electronic sensor in a ferroelectric field transistor geometry, we quantify the ferroelectric built-in interlayer potential, in good agreement with first-principles calculations. The novel semiconducting ferroelectric properties of these four new TMDs opens up the possibility of studying the interplay between ferroelectricity and their rich electric and optical properties.

Moiré metrology of energy landscapes in van der Waals heterostructures.

Abstract: The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moire superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moire metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moire domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moire metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked MoSe2/WSe2. Moire metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers. Here, a combined experiment-theory framework based on different nano-imaging techniques and first-principle calculations is used to analyse the shapes of moire patterns in twisted van der Waals structures, enabling an accurate description of the coupling between the atomically thin layers.

Tuning layer-hybridized moiré excitons by the quantum-confined Stark effect.

Abstract: Moire superlattices offer an unprecedented opportunity for tailoring interactions between quantum particles1-11 and their coupling to electromagnetic fields12-18. Strong superlattice potentials generate moire minibands of excitons16-18-bound pairs of electrons and holes that reside either in a single layer (intralayer excitons) or in two separate layers (interlayer excitons). Twist-angle-controlled interlayer electronic hybridization can also mix these two types of exciton to combine their strengths13,19,20. Here we report the direct observation of layer-hybridized moire excitons in angle-aligned WSe2/WS2 and MoSe2/WS2 superlattices by optical reflectance spectroscopy. These excitons manifest a hallmark signature of strong coupling in WSe2/WS2, that is, energy-level anticrossing and oscillator strength redistribution under a vertical electric field. They also exhibit doping-dependent renormalization and hybridization that are sensitive to the electronic correlation effects. Our findings have important implications for emerging many-body states in two-dimensional semiconductors, such as exciton condensates21 and Bose-Hubbard models22, and optoelectronic applications of these materials.

Optical parametric amplification by monolayer transition metal dichalcogenides

Abstract: Optical parametric amplification is a second-order nonlinear process whereby an optical signal is amplified by a pump via the generation of an idler field1. This mechanism is inherently related to spontaneous parametric down-conversion, which currently constitutes the building block for entangled photon pair generation2, a process that is exploited in modern quantum technologies. Here we demonstrate single-pass optical parametric amplification at the ultimate thickness limit; using semiconducting transition metal dichalcogenides3,4, we show that amplification can be attained over propagation through a single atomic layer. Such a second-order nonlinear interaction at the two-dimensional limit bypasses phase-matching requirements5 and achieves ultrabroad amplification bandwidths. In agreement with first-principle calculations, we observe that the amplification process is independent of the in-plane polarization of signal and pump fields. By the use of AA-stacked multilayers, we present a clear pathway towards the scaling of conversion efficiency. Our results pave the way for the development of atom-sized tunable sources of radiation with potential applications in nanophotonics and quantum information technology. Single-pass optical parametric amplification is demonstrated following propagation though an atomically thin semiconducting transition metal dichalcogenide. The demonstration may lead to atom-sized tunable light sources.

Enhanced tunable second harmonic generation from twistable interfaces and vertical superlattices in boron nitride homostructures.

Abstract: Broken symmetries induce strong even-order nonlinear optical responses in materials and at interfaces. Unlike conventional covalently bonded nonlinear crystals, van der Waals (vdW) heterostructures feature layers that can be stacked at arbitrary angles, giving complete control over the presence or lack of inversion symmetry at a crystal interface. Here, we report highly tunable second harmonic generation (SHG) from nanomechanically rotatable stacks of bulk hexagonal boron nitride (BN) crystals and introduce the term twistoptics to describe studies of optical properties in twistable vdW systems. By suppressing residual bulk effects, we observe SHG intensity modulated by a factor of more than 50, and polarization patterns determined by moire interface symmetry. Last, we demonstrate greatly enhanced conversion efficiency in vdW vertical superlattice structures with multiple symmetry-broken interfaces. Our study paves the way for compact twistoptics architectures aimed at efficient tunable frequency conversion and demonstrates SHG as a robust probe of buried vdW interfaces.

Moiréless correlations in ABCA graphene.

Abstract: Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene--a simple material that also exhibits a flat electronic band edge but without the need of having a moire superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3-5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.

Diffusivity Reveals Three Distinct Phases of Interlayer Excitons in MoSe 2 /WSe 2 Heterobilayers

Abstract: Charge separated interlayer excitons in transition metal dichalcogenide heterobilayers are being explored for moir\'e exciton lattices and exciton condensates. The presence of permanent dipole moments and the poorly screened Coulomb interaction make many-body interactions particularly strong for interlayer excitons. Here we reveal two distinct phase transitions for interlayer excitons in the ${\mathrm{MoSe}}_{2}/{\mathrm{WSe}}_{2}$ heterobilayer using time and spatially resolved photoluminescence imaging: from trapped excitons in the moir\'e potential to the modestly mobile exciton gas as exciton density increases to ${n}_{ex}\ensuremath{\sim}{10}^{11}\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}2}$ and from the exciton gas to the highly mobile charge separated electron-hole plasma for ${n}_{ex}g{10}^{12}\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}2}$. The latter is the Mott transition and is confirmed in photoconductivity measurements. These findings set fundamental limits for achieving quantum states of interlayer excitons.

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2.

Abstract: Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe2) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼[Formula: see text] which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.

Programmable hyperbolic polaritons in van der Waals semiconductors.

Abstract: Collective electronic modes or lattice vibrations usually prohibit propagation of electromagnetic radiation through the bulk of common materials over a frequency range associated with these oscillations. However, this textbook tenet does not necessarily apply to layered crystals. Highly anisotropic materials often display nonintuitive optical properties and can permit propagation of subdiffractional waveguide modes, with hyperbolic dispersion, throughout their bulk. Here, we report on the observation of optically induced electronic hyperbolicity in the layered transition metal dichalcogenide tungsten diselenide (WSe2). We used photoexcitation to inject electron-hole pairs in WSe2 and then visualized, by transient nanoimaging, the hyperbolic rays that traveled along conical trajectories inside of the crystal. We establish here the signatures of programmable hyperbolic electrodynamics and assess the role of quantum transitions of excitons within the Rydberg series in the observed polaritonic response.

Enhanced Superconductivity in Monolayer Td-MoTe2

Abstract: Crystalline two-dimensional (2D) superconductors (SCs) with low carrier density are an exciting new class of materials in which electrostatic gating can tune superconductivity, electronic interactions play a prominent role, and electrical transport properties may directly reflect the topology of the Fermi surface. Here, we report the dramatic enhancement of superconductivity with decreasing thickness in semimetallic Td-MoTe2, with critical temperature (Tc) increasing up to 7.6 K for monolayers, a 60-fold increase with respect to the bulk Tc. We show that monolayers possess a similar electronic structure and density of states (DOS) as the bulk, implying that electronic interactions play a strong role in the enhanced superconductivity. Reflecting the low carrier density, the critical temperature, magnetic field, and current density are all tunable by an applied gate voltage. The response to high in-plane magnetic fields is distinct from that of other 2D SCs and reflects the canted spin texture of the electron pockets.

Creation of moiré bands in a monolayer semiconductor by spatially periodic dielectric screening.

Abstract: Moire superlattices of two-dimensional van der Waals materials have emerged as a powerful platform for designing electronic band structures and discovering emergent physical phenomena. A key concept involves the creation of long-wavelength periodic potential and moire bands in a crystal through interlayer electronic hybridization or atomic corrugation when two materials are overlaid. Here we demonstrate a new approach based on spatially periodic dielectric screening to create moire bands in a monolayer semiconductor. This approach relies on reduced dielectric screening of the Coulomb interactions in monolayer semiconductors and their environmental dielectric-dependent electronic band structure. We observe optical transitions between moire bands in monolayer WSe2 when it is placed close to small-angle-misaligned graphene on hexagonal boron nitride. The moire bands are a result of long-range Coulomb interactions, which are strongly gate tunable, and can have versatile superlattice symmetries independent of the crystal lattice of the host material. Our result also demonstrates that monolayer semiconductors are sensitive local dielectric sensors.

Long-Lived Phonon Polaritons in Hyperbolic Materials

Abstract: Natural hyperbolic materials with dielectric permittivities of opposite signs along different principal axes can confine long-wavelength electromagnetic waves down to the nanoscale, well below the diffraction limit. Confined electromagnetic waves coupled to phonons in hyperbolic dielectrics including hexagonal boron nitride (hBN) and α-MoO3 are referred to as hyperbolic phonon polaritons (HPPs). HPP dissipation at ambient conditions is substantial, and its fundamental limits remain unexplored. Here, we exploit cryogenic nanoinfrared imaging to investigate propagating HPPs in isotopically pure hBN and naturally abundant α-MoO3 crystals. Close to liquid-nitrogen temperatures, losses for HPPs in isotopic hBN drop significantly, resulting in propagation lengths in excess of 8 μm, with lifetimes exceeding 5 ps, thereby surpassing prior reports on such highly confined polaritonic modes. Our nanoscale, temperature-dependent imaging reveals the relevance of acoustic phonons in HPP damping and will be instrumental in mitigating such losses for miniaturized mid-infrared technologies operating at liquid-nitrogen temperatures.

Hyperbolic enhancement of photocurrent patterns in minimally twisted bilayer graphene.

Abstract: Quasi-periodic moire patterns and their effect on electronic properties of twisted bilayer graphene have been intensely studied. At small twist angle θ, due to atomic reconstruction, the moire superlattice morphs into a network of narrow domain walls separating micron-scale AB and BA stacking regions. We use scanning probe photocurrent imaging to resolve nanoscale variations of the Seebeck coefficient occurring at these domain walls. The observed features become enhanced in a range of mid-infrared frequencies where the hexagonal boron nitride substrate is optically hyperbolic. Our results illustrate the capabilities of the nano-photocurrent technique for probing nanoscale electronic inhomogeneities in two-dimensional materials. Here, the authors use scanning probe photocurrent imaging to resolve nanoscale variations of the Seebeck coefficient occurring at domain walls separating micron-scale AB and BA stacking regions in twisted bilayer graphene, and observe hyperbolic enhancement of the photocurrent pattern.

High carrier mobility in graphene doped using a monolayer of tungsten oxyselenide

Abstract: Doped graphene could be of use in next-generation electronic and photonic devices. However, chemical doping cannot be precisely controlled in the material and leads to external disorder that diminishes carrier mobility and conductivity. Here we show that graphene can be efficiently doped using a monolayer of tungsten oxyselenide (TOS) that is created by oxidizing a monolayer of tungsten diselenide. When the TOS monolayer is in direct contact with graphene, a room-temperature mobility of 2,000 cm2 V−1 s−1 at a hole density of 3 × 1013 cm−2 is achieved. Hole density and mobility can also be controlled by inserting tungsten diselenide interlayers between TOS and graphene, where increasing the layers reduces the disorder. With four layers, a mobility value of around 24,000 cm2 V−1 s−1 is observed, approaching the limit set by acoustic phonon scattering, resulting in a sheet resistance below 50 Ω sq−1. To illustrate the potential of our approach, we show that TOS-doped graphene can be used as a transparent conductor in a near-infrared (1,550 nm) silicon nitride photonic waveguide and ring resonator. A monolayer of tungsten oxyselenide, created by oxidizing a layer of tungsten diselenide, can be used to efficiently dope graphene, leading to a room-temperature mobility of 2,000 cm2 V–1 s–1 at a hole density of 3 × 1013 cm–2.

Nanoscale Lattice Dynamics in Hexagonal Boron Nitride Moiré Superlattices

Abstract: Twisted two-dimensional van der Waals (vdW) heterostructures have unlocked a new means for manipulating the properties of quantum materials. The resulting mesoscopic moire superlattices are accessible to a wide variety of scanning probes. To date, spatially-resolved techniques have prioritized electronic structure visualization, with lattice response experiments only in their infancy. Here, we therefore investigate lattice dynamics in twisted layers of hexagonal boron nitride (hBN), formed by a minute twist angle between two hBN monolayers assembled on a graphite substrate. Nano-infrared (nano-IR) spectroscopy reveals systematic variations of the in-plane optical phonon frequencies amongst the triangular domains and domain walls in the hBN moire superlattices. Our first-principles calculations unveil a local and stacking-dependent interaction with the underlying graphite, prompting symmetry-breaking between the otherwise identical neighboring moire domains of twisted hBN. Here, the authors investigate the lattice dynamics of twisted hexagonal boron nitride layers via nano-infrared spectroscopy, showing local and stacking-dependent variations of the optical phonon frequencies associated to the interaction with the graphite substrate.

Intrinsic donor-bound excitons in ultraclean monolayer semiconductors.

Abstract: The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2 These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns) Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellites' photoluminescence Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors

Dual-Gated Graphene Devices for Near-Field Nano-imaging.

Abstract: Graphene-based heterostructures display a variety of phenomena that are strongly tunable by electrostatic local gates. Monolayer graphene (MLG) exhibits tunable surface plasmon polaritons, as revealed by scanning nano-infrared experiments. In bilayer graphene (BLG), an electronic gap is induced by a perpendicular displacement field. Gapped BLG is predicted to display unusual effects such as plasmon amplification and domain wall plasmons with significantly larger lifetime than MLG. Furthermore, a variety of correlated electronic phases highly sensitive to displacement fields have been observed in twisted graphene structures. However, applying perpendicular displacement fields in nano-infrared experiments has only recently become possible [Li, H.; Nano Lett. 2020, 20, 3106-3112]. In this work, we fully characterize two approaches to realizing nano-optics compatible top gates: bilayer MoS2 and MLG. We perform nano-infrared imaging on both types of structures and evaluate their strengths and weaknesses. Our work paves the way for comprehensive near-field experiments of correlated phenomena and plasmonic effects in graphene-based heterostructures.

Enhanced Photoluminescence of Multiple Two-Dimensional van der Waals Heterostructures Fabricated by Layer-by-Layer Oxidation of MoS2

Abstract: Monolayer transition metal dichalcogenides (TMDs) are promising for optoelectronics because of their high optical quantum yield and strong light-matter interaction. In particular, the van der Waals (vdW) heterostructures consisting of monolayer TMDs sandwiched by large gap hexagonal boron nitride have shown great potential for novel optoelectronic devices. However, a complicated stacking process limits scalability and practical applications. Furthermore, even though lots of efforts, such as fabrication of vdW heterointerfaces, modification of the surface, and structural phase transition, have been devoted to preserve or modulate the properties of TMDs, high environmental sensitivity and damage-prone characteristics of TMDs make it difficult to achieve a controllable technique for surface/interface engineering. Here, we demonstrate a novel way to fabricate multiple two-dimensional (2D) vdW heterostructures consisting of alternately stacked MoS2 and MoOx with enhanced photoluminescence (PL). We directly oxidized multilayer MoS2 to a MoOx/1 L-MoS2 heterostructure with atomic layer precision through a customized oxygen plasma system. The monolayer MoS2 covered by MoOx showed an enhanced PL intensity 3.2 and 6.5 times higher in average than the as-exfoliated 1 L- and 2 L-MoS2 because of preserved crystallinity and compensated dedoping by MoOx. By using layer-by-layer oxidation and transfer processes, we fabricated the heterostructures of MoOx/MoS2/MoOx/MoS2, where the MoS2 monolayers are separated by MoOx. The heterostructures showed the multiplied PL intensity as the number of embedded MoS2 layers increases because of suppression of the nonradiative trion formation and interlayer decoupling between stacked MoS2 layers. Our work shows a novel way toward the fabrication of 2D material-based multiple vdW heterostructures and our layer-by-layer oxidation process is beneficial for the fabrication of high performance 2D optoelectronic devices.

Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

Abstract: Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse controls, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task. Here, we use a scattering-type scanning near-field optical microscope (s-SNOM) to acquire exciton spectra in atomically thin transition metal dichalcogenide microcrystals with previously unattainable 20 nm resolution. Our nano-optical data revealed material- and stacking-dependent exciton spectra of MoSe2, WSe2, and their heterostructures. Furthermore, we extracted the complex dielectric function of these prototypical vdW semiconductors. s-SNOM hyperspectral images uncovered how the dielectric screening modifies excitons at length scales as short as few nanometers. This work paves the way towards understanding and manipulation of excitons in atomically thin layers at the nanoscale.

Damage-Free Atomic Layer Etch of WSe2: A Platform for Fabricating Clean Two-Dimensional Devices.

Abstract: The development of a controllable, selective, and repeatable etch process is crucial for controlling the layer thickness and patterning of two-dimensional (2D) materials. However, the atomically thin dimensions and high structural similarity of different 2D materials make it difficult to adapt conventional thin-film etch processes. In this work, we propose a selective, damage-free atomic layer etch (ALE) that enables layer-by-layer removal of monolayer WSe2 without altering the physical, optical, and electronic properties of the underlying layers. The etch uses a top-down approach where the topmost layer is oxidized in a self-limited manner and then removed using a selective etch. Using a comprehensive set of material, optical, and electrical characterization, we show that the quality of our ALE processed layers is comparable to that of pristine layers of similar thickness. The ALE processed WSe2 layers preserve their bright photoluminescence characteristics and possess high room-temperature hole mobilities of 515 cm2/V·s, essential for fabricating high-performance 2D devices. Further, using graphene as a testbed, we demonstrate the fabrication of ultra-clean 2D devices using a sacrificial monolayer WSe2 layer to protect the channel during processing, which is etched in the final process step in a technique we call sacrificial WSe2 with ALE processing (SWAP). The graphene transistors made using the SWAP technique demonstrate high room-temperature field-effect mobilities, up to 200,000 cm2/V·s, better than previously reported unencapsulated graphene devices.

Tunable Exciton-Optomechanical Coupling in Suspended Monolayer MoSe2.

Abstract: The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here, we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observed optical damping and antidamping of mechanical vibrations as well as the optical spring effect. The exciton-optomechanical coupling strength is also gate-tunable. Our observations can be understood in a model based on photothermal backaction and gate-induced mirror symmetry breaking in the device structure. The observation of gate-tunable exciton-optomechanical coupling in a monolayer semiconductor may find applications in nanoelectromechanical systems (NEMS) and in exciton-optomechanics.

Hyperbolic Cooper-Pair Polaritons in Planar Graphene/Cuprate Plasmonic Cavities

Abstract: Hyperbolic Cooper-pair polaritons (HCP) in cuprate superconductors are of fundamental interest due to their potential for providing insights into the nature of unconventional superconductivity. Her...

Bilayer WSe$_2$ as a natural platform for interlayer exciton condensates in the strong coupling limit

Abstract: Exciton condensates (EC) are macroscopic coherent states arising from condensation of electron-hole pairs. Bilayer heterostructures, consisting of two-dimensional electron and hole layers separated by a tunnel barrier, provide a versatile platform to realize and study EC. The tunnel barrier suppresses recombination yielding long-lived excitons. However, this separation also reduces interlayer Coulomb interactions, limiting the exciton binding strength. Here, we report the observation of EC in naturally occurring 2H-stacked bilayer WSe$_2$. In this system, the intrinsic spin-valley structure suppresses interlayer tunneling even when the separation is reduced to the atomic limit, providing access to a previously unattainable regime of strong interlayer coupling. Using capacitance spectroscopy, we investigate magneto-EC, formed when partially filled Landau levels (LL) couple between the layers. We find that the strong-coupling EC show dramatically different behaviour compared with previous reports, including an unanticipated variation of the EC robustness with the orbital number, and find evidence for a transition between two types of low-energy charged excitations. Our results provide a demonstration of tuning EC properties by varying the constituent single-particle wavefunctions.