Tunable Single-Photon Emission with Wafer-Scale Plasmonic Array.

Bright, scalable, and deterministic single-photon emission (SPE) is essential for quantum optics, nanophotonics, and optical information systems. Recently, SPE from hexagonal boron nitride (h-BN) has attracted intense interest because it is optically active and stable at room temperature. Here, we demonstrate a tunable quantum emitter array in h-BN at room temperature by integrating a wafer-scale plasmonic array. The transient voltage electrophoretic deposition (EPD) reaction is developed to effectively enhance the filling of single-crystal nanometals in the designed patterns without aggregation, which ensures the fabricated array for tunable performances of these single-photon emitters. An enhancement of ∼500% of the SPE intensity of the h-BN emitter array is observed with a radiative quantum efficiency of up to 20% and a saturated count rate of more than 4.5 × 106 counts/s. These results suggest the integrated h-BN-plasmonic array as a promising platform for scalable and controllable SPE photonics at room temperature.

The effect of critical coupling constants on superconductivity enhancement.

In this study, we propose a phenomenological model to extend McMillan's results on a coupling strength equal to 2. We investigate possible strategies to enhance superconductivity by tuning the phonon frequency, carrier number, or pressure. In particular, we show that the critical coupling constants corresponding to the phonon frequency, carrier number, or pressure determine whether the variation of the critical temperature is positive or negative. These observations explain the contrasting behavior between weak and strong coupling superconductors and are consistent with experimental observations. We also demonstrate the dome observed in the carrier number effect and pressure effect. Additionally, these critical coupling constants systematically separate superconductivity into three regions: weak, intermediate, and strong coupling. We find that the enhancement strategies for weak and strong coupling regions are opposite, but both inevitably bring superconductivity into the intermediate coupling region. Finally, we propose general zigzag methods for intermediate coupling superconductors to further enhance the critical temperature.

Passivated Interfacial Traps of Monolayer MoS2 with Bipolar Electrical Pulse.

Heterogeneous integration of monolayers is an emergent route of spatially combining materials with available platforms for unprecedented properties. A long-standing challenge along this route is to manipulate interfacial configurations of each unit in stacking architecture. A monolayer of transition metal dichalcogenides (TMDs) offers an embodiment of studying interface engineering of integrated systems because optoelectronic performances generally trade off with each other due to interfacial trap states. While ultrahigh photoresponsivity of TMDs phototransistors has been realized, a long response time commonly appears and hinders applications. Here, fundamental processes in excitation and relaxation of the photoresponse are studied and correlated with interfacial traps of the monolayer MoS2. A mechanism for the onset of saturation photocurrent and the reset behavior in the monolayer photodetector is illustrated based on device performances. Electrostatic passivation of interfacial traps is achieved with the bipolar gate pulse and significantly reduces the response time for photocurrent to reach saturated states. This work paves the way toward fast-speed and ultrahigh-gain devices of stacked two-dimensional monolayers.

Visualization of Band Shifting and Interlayer Coupling in WxMo1-xS2 Alloys Using Near-Field Broadband Absorption Microscopy.

Beyond-diffraction-limit optical absorption spectroscopy provides in-depth information on the graded band structures of composition-spread and stacked two-dimensional materials, in which direct/indirect bandgap, interlayer coupling, and defects significantly modify their optoelectronic functionalities such as photoluminescence efficiency. We here visualize the spatially varying band structure of monolayer and bilayer transition metal dichalcogenide alloys by using near-field broadband absorption microscopy. The near-field spectral and spatial information manifests the excitonic band shift that results from the interplay of composition spreading and interlayer coupling. These results enable us to identify, notably, the top layer of the bilayer alloy as pure WS2. We also use the aberration-free near-field transmission images to demarcate the exact boundaries of alloyed and pure transition metal dichalcogenides. This technology can offer valuable insights on various layered structures in the era of "stacking science" in the quest of quantum optoelectronic devices.

Near-field spectroscopic imaging of exciton quenching at atomically sharp MoS2/WS2 lateral heterojunctions.

Heterojunctions made by laterally stitching two different transition metal dichalcogenide monolayers create a unique one-dimensional boundary with intriguing local optical properties that can only be characterized by nanoscale-spatial-resolution spectral tools. Here, we use near-field photoluminescence (NF-PL) to reveal the narrowest region (105 nm) ever reported of photoluminescence quenching at the junction of a laterally stitched WS2/MoS2 monolayer. We attribute this quenching to the atomically sharp band offset that generates a strong electric force at the junction to easily dissociate excitons. Besides the sharp heterojunction, a model considering various widths of the alloying interfacial region under low or high optical pumping is presented. With a spatial resolution six times better than that of confocal microscopy, NF-PL provides an unprecedented spectral tool for non-scalable 1D lateral heterojunctions.

Scalable Moiré Lattice with Oriented TMD Monolayers.

Moiré lattice in artificially stacked monolayers of two-dimensional (2D) materials effectively modulates the electronic structures of materials, which is widely highlighted. Formation of the electronic Moiré superlattice promises the prospect of uniformity among different moiré cells across the lattice, enabling a new platform for novel properties, such as unconventional superconductivity, and scalable quantum emitters. Recently, epitaxial growth of the monolayer transition metal dichalcogenide (TMD) is achieved on the sapphire substrate by chemical vapor deposition (CVD) to realize scalable growth of highly-oriented monolayers. However, fabrication of the scalable Moiré lattice remains challenging due to the lack of essential manipulation of the well-aligned monolayers for clean interface quality and precise twisting angle control. Here, scalable and highly-oriented monolayers of TMD are realized on the sapphire substrates by using the customized CVD process. Controlled growth of the epitaxial monolayers is achieved by promoting the rotation of the nuclei-like domains in the initial growth stage, enabling aligned domains for further grain growth in the steady-state stage. A full coverage and distribution of the highly-oriented domains are verified by second-harmonic generation (SHG) microscopy. By developing the method for clean monolayer manipulation, hetero-stacked bilayer (epi-WS2/epi-MoS2) is fabricated with the specific angular alignment of the two major oriented monolayers at the edge direction of 0°/ ± 60°. On account of the optimization for scalable Moiré lattice with a high-quality interface, the observation of interlayer exciton at low temperature illustrates the feasibility of scalable Moiré superlattice based on the oriented monolayers.

Nonlinear valley phonon scattering under the strong coupling regime.

Research efforts of cavity quantum electrodynamics have focused on the manipulation of matter hybridized with photons under the strong coupling regime1-3. This has led to striking discoveries including polariton condensation2 and single-photon nonlinearity3, where the phonon scattering plays a critical role1-9. However, resolving the phonon scattering remains challenging for its non-radiative complexity. Here we demonstrate nonlinear phonon scattering in monolayer MoS2 that is strongly coupled to a plasmonic cavity mode. By hybridizing excitons and cavity photons, the phonon scattering is equipped with valley degree of freedom and boosted with superlinear enhancement to a stimulated regime, as revealed by Raman spectroscopy and our theoretical model. The valley polarization is drastically enhanced and sustained throughout the stimulated regime, suggesting a coherent scattering process enabled by the strong coupling. Our findings clarify the feasibility of valley-cavity-based systems for lighting, imaging, optical information processing and manipulating quantum correlations in cavity quantum electrodynamics2,3,10-17.

Tuning of Two-Dimensional Plasmon-Exciton Coupling in Full Parameter Space: A Polaritonic Non-Hermitian System.

Non-Hermitian photonic systems with gains and/or losses have recently emerged as a powerful approach for topology-protected optical transport and novel device applications. To date, most of these systems employ coupled optical systems of diffraction-limited dielectric waveguides or microcavities, which exchange energy spatially or temporally. Here, we introduce a diffraction-unlimited approach using a plasmon-exciton coupling (polariton) system with tunable plasmonic resonance (energy and line width) and coupling strength. By designing a chirped silver nanogroove cavity array and coupling a single tungsten disulfide monolayer with a large contrast in resonance line width, we show the tuning capability through energy level anticrossing and plasmon-exciton hybridization (line width crossover), as well as spontaneous symmetry breaking across the exceptional point at zero detuning. This two-dimensional hybrid material system can be applied as a scalable and integratable platform for non-Hermitian photonics, featuring seamless integration of two-dimensional materials, broadband tuning, and operation at room temperature.

Epitaxial Aluminum Surface-Enhanced Raman Spectroscopy Substrates for Large-Scale 2D Material Characterization.

Surface-enhanced Raman spectroscopy (SERS) is an ultrasensitive technique to identify vibrational fingerprints of trace analytes. However, present SERS techniques suffer from the lack of uniform, reproducible, and stable substrates to control the plasmonic hotspots in a wide spectral range. Here, we report the promising application of epitaxial aluminum films as a scalable plasmonic platform for SERS applications. To assess the uniformity of aluminum substrates, atomically thin transition metal dichalcogenide monolayers are used as the benchmark analyte due to their inherent two-dimensional homogeneity. Besides the distinctive spectral capability of aluminum in the ultraviolet (325 nm), we demonstrate that the aluminum substrates can even perform comparably with the silver counterparts made from single-crystalline colloidal silver crystals using the same SERS substrate design in the visible range (532 nm). This is unexpected from the prediction solely based on optical dielectric functions and illustrate the superior surface and interface properties of epitaxial aluminum SERS substrates.

Selective Growth of WSe2 with Graphene Contacts.

Nanoelectronics of two-dimensional (2D) materials and related applications are hindered with critical contact issues with the semiconducting monolayers. To solve these issues, a fundamental challenge is selective and controllable fabrication of p-type or ambipolar transistors with a low Schottky barrier. Most p-type transistors are demonstrated with tungsten selenides (WSe2) but a high growth temperature is required. Here, we utilize seeding promoter and low pressure CVD process to enhance sequential WSe2 growth with a reduced growth temperature of 800 °C for reduced compositional fluctuations and high hetero-interface quality. Growth behavior of the sequential WSe2 growth at the edge of patterned graphene is discussed. With optimized growth conditions, high-quality interface of the laterally stitched WSe2-graphene is achieved and characterized with transmission electron microscopy (TEM). Device fabrication and electronic performances of the laterally stitched WSe2-graphene are presented.

Lineshape characterization of excitons in monolayer WS2 by two-dimensional electronic spectroscopy.

The optical properties of monolayer transition metal dichalcogenides (TMDCs), an important family of two-dimensional (2D) semiconductors for optoelectronic applications, are dominated by two excitons A (XA) and B (XB) located at K/K's valleys. The lineshape of the excitons is an indicator of the interaction of the excitons with other particles and also largely determines the performance of TMDC-based optoelectronic devices. In this work, we apply 2D electronic spectroscopy (2DES), which enables separation of the intrinsic homogeneous linewidth and the extrinsic inhomogeneous linewidth, to dissect the lineshape of XA in monolayer WS2. With a home-built broadband optical parametric amplifier, the 2D spectra give the exciton linewidth values for extensive ranges of excitation densities and temperatures, reflecting inter-exciton and exciton-phonon interactions. Meanwhile, the time-domain evolution of the lineshape reveals a similar rate of spectral diffusion to that in quantum wells (QWs) based on III-V semiconductors.

Tunable Moiré Superlattice of Artificially Twisted Monolayers.

Twisting between two stacked monolayers modulates periodic potentials and forms the Moiré electronic superlattices, which offers an additional degree of freedom to alter material property. Considerable unique observations, including unconventional superconductivity, coupled spin-valley states, and quantized interlayer excitons are correlated to the electronic superlattices but further study requires reliable routes to study the Moiré in real space. Scanning tunneling microscopy (STM) is ideal to precisely probe the Moiré superlattice and correlate coupled parameters among local electronic structures, strains, defects, and band alignment at atomic scale. Here, a clean route is developed to construct twisted lattices using synthesized monolayers for fundamental studies. Diverse Moiré superlattices are predicted and successfully observed with STM at room temperature. Electrical tuning of the Moiré superlattice is achieved with stacked TMD on graphite.

A gate-free monolayer WSe2 pn diode.

Interest in bringing p- and n-type monolayer semiconducting transition metal dichalcogenides (TMD) into contact to form rectifying pn diode has thrived since it is crucial to control the electrical properties in two-dimensional (2D) electronic and optoelectronic devices. Usually this involves vertically stacking different TMDs with pn heterojunction or, laterally manipulating carrier density by gate biasing. Here, by utilizing a locally reversed ferroelectric polarization, we laterally manipulate the carrier density and created a WSe2 pn homojunction on the supporting ferroelectric BiFeO3 substrate. This non-volatile WSe2 pn homojunction is demonstrated with optical and scanning probe methods and scanning photoelectron micro-spectroscopy. A homo-interface is a direct manifestation of our WSe2 pn diode, which can be quantitatively understood as a clear rectifying behavior. The non-volatile confinement of carriers and associated gate-free pn homojunction can be an addition to the 2D electron-photon toolbox and pave the way to develop laterally 2D electronics and photonics.

Efficient Defect Healing of Transition Metal Dichalcogenides by Metallophthalocyanine.

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted great attention as alternatives to graphene with semiconducting band gaps. Mono- or few-layer TMDCs can be prepared by various methods, but regardless of the fabrication methods [such as mechanical exfoliation and chemical vapor deposition (CVD)], TMDCs contain many structural defects, which significantly affect their physical properties and limit their performance in applications. Metallophthalocyanines (MPcs) are organic semiconductors, and as dopants, they are capable of modulating the optical and electrical properties of other semiconducting materials. Here, we report that besides the ability to modulate the optoelectronic properties of 2D TMDCs, MPc molecules can be used to heal defects and improve the physicochemical properties of TMDCs. Doping of planar MPc molecules to TMDCs is achieved by a simple solution dip-coating method and results in a significant improvement in the optical properties and thermal responses of CVD-grown TMDCs, even comparable to those of mechanically exfoliated counterparts. Study of carrier dynamics shows that the adsorption of MPc on the TMDC surface leads to the complete suppression of the mid-gap defect-induced absorption in TMDCs. Furthermore, MPc molecules with a large lateral size are found to effectively reduce the point defects in mechanically exfoliated TMDCs introduced during the preparation process. Our results not only clarify the optoelectronic modulation mechanism of chemical doping but also offer a simple method to control the nanosized defects in 2D TMDCs.

Observation of Exciton-Exciton Interaction Mediated Valley Depolarization in Monolayer MoSe2.

The valley pseudospin in monolayer transition metal dichalcogenides (TMDs) has been proposed as a new way to manipulate information in various optoelectronic devices. This relies on a large valley polarization that remains stable over long time scales (hundreds of nanoseconds). However, time-resolved measurements report valley lifetimes of only a few picoseconds. This has been attributed to mechanisms such as phonon-mediated intervalley scattering and a precession of the valley pseudospin through electron-hole exchange. Here we use transient spin grating to directly measure the valley depolarization lifetime in monolayer MoSe2. We find a fast valley decay rate that scales linearly with the excitation density at different temperatures. This establishes the presence of strong exciton-exciton Coulomb exchange interactions enhancing the valley depolarization. Our work highlights the microscopic processes inhibiting the efficient use of the exciton valley pseudospin in monolayer TMDs.

Synthesis of In-Plane Artificial Lattices of Monolayer Multijunctions.

Recently, monolayers of van der Waals materials, including transition metal dichalcogenides (TMDs), are considered ideal building blocks for constructing 2D artificial lattices and heterostructures. Heterostructures with multijunctions of more than two monolayer TMDs are intriguing for exploring new physics and materials properties. Obtaining in-plane heterojunctions of monolayer TMDs with atomically sharp interfaces is very significant for fundamental research and applications. Currently, multistep synthesis for more than two monolayer TMDs remains a challenge because decomposition or compositional alloying is thermodynamically favored at the high growth temperature. Here, a multistep chemical vapor deposition (CVD) synthesis of the in-plane multijunctions of monolayer TMDs is presented. A low growth temperature synthesis is developed to avoid compositional fluctuations of as-grown TMDs, defects formations, and interfacial alloying for high heterointerface quality and thermal stability of monolayer TMDs. With optimized parameters, atomically sharp interfaces are successfully achieved in the synthesis of in-plane artificial lattices of the WS2 /WSe2 /MoS2 at reduced growth temperatures. Growth behaviors as well as the heterointerface quality are carefully studied in varying growth parameters. Highly oriented strain patterns are found in the second harmonic generation imaging of the TMD multijunctions, suggesting that the in-plane heteroepitaxial growth may induce distortion for unique material symmetry.

Autocatalytic surface reduction and its role in controlling seed-mediated growth of colloidal metal nanocrystals.

The growth of colloidal metal nanocrystals typically involves an autocatalytic process, in which the salt precursor adsorbs onto the surface of a growing nanocrystal, followed by chemical reduction to atoms for their incorporation into the nanocrystal. Despite its universal role in the synthesis of colloidal nanocrystals, it is still poorly understood and controlled in terms of kinetics. Through the use of well-defined nanocrystals as seeds, including those with different types of facets, sizes, and internal twin structure, here we quantitatively analyze the kinetics of autocatalytic surface reduction in an effort to control the evolution of nanocrystals into predictable shapes. Our kinetic measurements demonstrate that the activation energy barrier to autocatalytic surface reduction is highly dependent on both the type of facet and the presence of twin boundary, corresponding to distinctive growth patterns and products. Interestingly, the autocatalytic process is effective not only in eliminating homogeneous nucleation but also in activating and sustaining the growth of octahedral nanocrystals. This work represents a major step forward toward achieving a quantitative understanding and control of the autocatalytic process involved in the synthesis of colloidal metal nanocrystals.

Strong and Broadly Tunable Plasmon Resonances in Thick Films of Aligned Carbon Nanotubes.

Low-dimensional plasmonic materials can function as high quality terahertz and infrared antennas at deep subwavelength scales. Despite these antennas' strong coupling to electromagnetic fields, there is a pressing need to further strengthen their absorption. We address this problem by fabricating thick films of aligned, uniformly sized semiconducting carbon nanotubes and showing that their plasmon resonances are strong, narrow, and broadly tunable. With thicknesses ranging from 25 to 250 nm, our films exhibit peak attenuation reaching 70%, ensemble quality factors reaching 9, and electrostatically tunable peak frequencies by a factor of 2.3. Excellent nanotube alignment leads to the attenuation being 99% linearly polarized along the nanotube axis. Increasing the film thickness blueshifts the plasmon resonators down to peak wavelengths as low as 1.4 µm, a new near-infrared regime in which they can both overlap the S11 nanotube exciton energy and access the technologically important infrared telecom band.

Coherent Plasmon and Phonon-Plasmon Resonances in Carbon Nanotubes.

Carbon nanotubes provide a rare access point into the plasmon physics of one-dimensional electronic systems. By assembling purified nanotubes into uniformly sized arrays, we show that they support coherent plasmon resonances, that these plasmons couple to nanotube and substrate phonons, and that the resulting phonon-plasmon resonances have quality factors as high as 10. Because nanotube plasmons intensely strengthen electromagnetic fields and light-matter interactions, they provide a compelling platform for surface-enhanced spectroscopy and tunable optical devices at deep-subwavelength scales.

Cascaded exciton energy transfer in a monolayer semiconductor lateral heterostructure assisted by surface plasmon polariton.

Atomically thin lateral heterostructures based on transition metal dichalcogenides have recently been demonstrated. In monolayer transition metal dichalcogenides, exciton energy transfer is typically limited to a short range (~1 µm), and additional losses may be incurred at the interfacial regions of a lateral heterostructure. To overcome these challenges, here we experimentally implement a planar metal-oxide-semiconductor structure by placing a WS2/MoS2 monolayer heterostructure on top of an Al2O3-capped Ag single-crystalline plate. We find that the exciton energy transfer range can be extended to tens of microns in the hybrid structure mediated by an exciton-surface plasmon polariton-exciton conversion mechanism, allowing cascaded exciton energy transfer from one transition metal dichalcogenides region supporting high-energy exciton resonance to a different transition metal dichalcogenides region in the lateral heterostructure with low-energy exciton resonance. The realized planar hybrid structure combines two-dimensional light-emitting materials with planar plasmonic waveguides and offers great potential for developing integrated photonic and plasmonic devices.Exciton energy transfer in monolayer transition metal dichalcogenides is limited to short distances. Here, Shi et al. fabricate a planar metal-oxide-semiconductor structure and show that exciton energy transfer can be extended to tens of microns, mediated by an exciton-surface-plasmon-polariton-exciton conversion mechanism.