Phonon Polaritons in Twisted Double-Layers of Hyperbolic van der Waals Crystals.

Controlling the twist angle between two stacked van der Waals (vdW) crystals is a powerful approach for tuning their electronic and photonic properties. Hyperbolic media have recently attracted much attention due to their ability to tailor electromagnetic waves at the subwavelength-scale which, however, usually requires complex patterning procedures. Here, we demonstrate a lithography-free approach for manipulating the hyperbolicity by harnessing the twist-dependent coupling of phonon polaritons in double-layers of vdW α-MoO3, a naturally biaxial hyperbolic crystal. The polariton isofrequency contours can be modified due to this interlayer coupling, allowing for controlling the polaritonic characteristics by adjusting the orientation angles between the two layers. Our findings provide opportunities for control of nanoscale light flow with twisted stacks of vdW crystals.

Resonance Coupling in Silicon Nanosphere-J-Aggregate Heterostructures.

Due to their optical magnetic and electric resonances associated with the high refractive index, dielectric silicon nanoparticles have been explored as novel nanocavities that are excellent candidates for enhancing various light-matter interactions at the nanoscale. Here, from both of theoretical and experimental aspects, we explored resonance coupling between excitons and magnetic/electric resonances in heterostructures composed of the silicon nanoparticle coated with a molecular J-aggregate shell. The resonance coupling was originated from coherent energy transfer between the exciton and magnetic/electric modes, which was manifested by quenching dips on the scattering spectrum due to formation of hybrid modes. The influences of various parameters, including the molecular oscillation strength, molecular absorption line width, molecular shell thickness, refractive index of the surrounding environment, and separation between the core and shell, on the resonance coupling behaviors were scrutinized. In particular, the resonance coupling can approach the strong coupling regime by choosing appropriate molecular parameters, where an anticrossing behavior with a mode splitting of 100 meV was observed on the energy diagram. Most interestingly, the hybrid modes in such dielectric heterostructure can exhibit unidirectional light scattering behaviors, which cannot be achieved by those in plexcitonic nanoparticle composed of a metal nanoparticle core and a molecular shell.

Field-Emission Energy Distribution of Carbon Nanotube Film and Single Tube under High Current.

A narrow energy distribution is a prominent characteristic of field-emission cold cathodes. When applied in a vacuum electronic device, the cold cathode is fabricated over a large area and works under a high current and current density. It is interesting to see the energy distribution of the field emitter under such a working situation. In this work, the energy distribution spectra of a single carbon nanotube (CNT) and a CNT film were investigated across a range of currents, spanning from low to high. A consistent result indicated that, at low current emission, the CNT film (area: 0.585 mm2) exhibited a narrow electron energy distribution as small as 0.5 eV, similar to that of a single CNT, while the energy distribution broadened with increased current and voltage, accompanied by a peak position shift. The influencing factors related to the electric field, Joule heating, Coulomb interaction, and emission site over a large area were discussed to elucidate the underlying mechanism. The results provide guidance for the electron source application of nano-materials in cold cathode devices.

Effect of Crystallinity on the Field Emission Characteristics of Carbon Nanotube Grown on W-Co Bimetallic Catalyst.

Carbon nanotube (CNT) is an excellent field emission material. However, uniformity and stability are the key issues hampering its device application. In this work, a bimetallic W-Co alloy was adopted as the catalyst of CNT in chemical vapor deposition process. The high melting point and stable crystal structure of W-Co helps to increase the grown CNT diameter uniformity and homogeneous crystal structure. High-crystallinity CNTs were grown on the W-Co bimetallic catalyst. Its field emission characteristics demonstrated a low turn-on field, high current density, stable current stability, and uniform emission distribution. The Fowler-Nordheim (FN) and Seppen-Katamuki (SK) analyses revealed that the CNT grown on the W-Co catalyst has a relatively low work function and high field enhancement factor. The high crystallinity and homogeneous crystal structure of CNT also reduce the body resistance and increase the emission current stability and maximum current. The result provides a way to synthesis a high-quality CNT field emitter, which will accelerate the development of cold cathode vacuum electronic device application.

A Flexible and Wearable Photodetector Enabling Ultra-Broadband Imaging from Ultraviolet to Millimeter-Wave Regimes.

Flexible and miniaturized photodetectors, offering a fast response across the ultraviolet (UV) to millimeter (MM) wave spectrum, are crucial for applications like healthcare monitoring and wearable optoelectronics. Despite their potential, developing such photodetectors faces challenges due to the lack of suitable materials and operational mechanisms. Here, the study proposes a flexible photodetector composed of a monolayer graphene connected by two distinct metal electrodes. Through the photothermoelectric effect, these asymmetric electrodes induce electron flow within the graphene channel upon electromagnetic wave illumination, resulting in a compact device with ultra-broadband and rapid photoresponse. The devices, with footprints ranging from 3 × 20 µm2 to 50 × 20 µm2, operate across a spectrum from 325 nm (UV) to 1.19 mm (MM) wave. They demonstrate a responsivity (RV) of up to 396.4 ± 5.1 mV W-1, a noise-equivalent power (NEP) of 8.6 ± 0.1 nW Hz- 0.5, and a response time as small as 0.8 ± 0.1 ms. This device facilitates direct imaging of shielded objects and material differentiation under simulated human body-wearing conditions. The straightforward device architecture, aligned with its ultra-broadband operational frequency range, is anticipated to hold significant implications for the development of miniaturized, wearable, and portable photodetectors.

A Capillary-Force-Assisted Transfer for Monolayer Transition-Metal-Dichalcogenide Crystals with High Utilization.

The capillary-force-assisted transfer has shown application potential for constructing two-dimensional (2D) electronic and optoelectronic devices for the advantage of free of spin coating the organic compound and etching the substrate. Currently, the transfer mechanism remains obscure. The capillary adhesion mechanism and capillary invasion separation mechanism were proposed independently and rarely discussed in a comprehensive manner. What is more, the integrity and utilization remain to be improved. Here, we developed the capillary-force-assisted transfer method with high utilization and integrity. Uniformity of water transport was improved by introducing water from the sidewall of the small polydimethylsiloxane (PDMS) stamp driven by capillary force. The transfer integrity rate increased, and the location of the complete samples became predictable. The transfer utilization increased as the limited water transportation minimized the impact on the surrounding WS2. The monolayer triangle WS2 crystals from adjacent areas on the sapphire substrate were transferred one after another. Besides, local mechanical exfoliation of the continuous WS2 thin films was demonstrated, implying that the capillary adhesion is strong enough to break the strong in-plane covalent bond and overcome the van der Waals force between WS2 and sapphire substrate. Finally, the water transport model between two surfaces with different hydrophobicity combinations was derived on the basis of the Young-Laplace equation. The analysis of water transport between different interfaces reveals how capillary adhesion and capillary invasion work together to achieve capillary force transfer. This study highlights the potential of the capillary-force-assisted transfer as an efficient technique for fabricating van der Waals structures based on two-dimensional atomic crystals, especially periodic structures.

Controlling and Focusing In-Plane Hyperbolic Phonon Polaritons in α-MoO3 with a Curved Plasmonic Antenna.

Hyperbolic phonon polaritons (HPhPs) sustained in polar van der Waals (vdW) crystals exhibit extraordinary confinement of long-wave electromagnetic fields to the deep subwavelength scale. In stark contrast to uniaxial vdW hyperbolic materials, recently emerged biaxial hyperbolic materials, such as α-MoO3 and α-V2 O5 , offer new degrees of freedom for controlling light in two-dimensions due to their distinctive in-plane hyperbolic dispersions. However, the control and focusing of these in-plane HPhPs remain elusive. Here, a versatile technique is proposed for launching, controlling, and focusing in-plane HPhPs in α-MoO3 with geometrically designed curved gold plasmonic antennas. It is found that the subwavelength manipulation and focusing behaviors are strongly dependent on the curvature of the antenna extremity. This strategy operates effectively in a broadband spectral region. These findings not only provide fundamental insights into the manipulation of light by biaxial hyperbolic crystals at the nanoscale but also open up new opportunities for planar nanophotonic applications.

Polariton waveguide modes in two-dimensional van der Waals crystals: an analytical model and correlative nano-imaging.

Two-dimensional van der Waals (vdW) crystals can sustain various types of polaritons with strong electromagnetic confinements, making them highly attractive for nanoscale photonic and optoelectronic applications. While extensive experimental and numerical studies have been devoted to the polaritons of the vdW crystals, analytical models are sparse. Particularly, applying the model to describe polariton behaviors that are visualized by state of the art near-field optical microscopy requires further investigations. In this study, we develop an analytical waveguide model to describe polariton propagations in vdW crystals. The dispersion contours, dispersion relations, and localized electromagnetic field distributions of polariton waveguide modes are derived. The model is verified by real-space optical nano-imaging and numerical simulation of phonon polaritons in α-MoO3, which is a vdW biaxial crystal. Although we focus on α-MoO3, the proposed model is valid for other polaritonic crystals within the vdW family given the corresponding dielectric substitutions. Our model therefore provides an analytical rationale for describing and understanding the localized electromagnetic fields in vdW crystals that are associated with polaritons.

A mid-infrared biaxial hyperbolic van der Waals crystal.

Hyperbolic media have attracted much attention in the photonics community due to their ability to confine light to arbitrarily small volumes and their potential applications to super-resolution technologies. The two-dimensional counterparts of these media can be achieved with hyperbolic metasurfaces that support in-plane hyperbolic guided modes upon nanopatterning, which, however, poses notable fabrication challenges and limits the achievable confinement. We show that thin flakes of a van der Waals crystal, α-MoO3, can support naturally in-plane hyperbolic polariton guided modes at mid-infrared frequencies without the need for patterning. This is possible because α-MoO3 is a biaxial hyperbolic crystal with three different Reststrahlen bands, each corresponding to a different crystalline axis. These findings can pave the way toward a new paradigm to manipulate and confine light in planar photonic devices.

Chemically-doped graphene with improved surface plasmon characteristics: an optical near-field study.

One of the most fascinating and important merits of graphene plasmonics is their tunability over a wide range. While chemical doping has proven to be a facile and effective way to create graphene plasmons, most of the previous studies focused on the macroscopic behaviors of the plasmons in chemically-doped graphene and little was known about their nanoscale responses and related mechanisms. Here, to the best of our knowledge, we present the first experimental near-field optical study on chemically-doped graphene with improved surface plasmon characteristics. By using a scattering-type scanning near-field optical microscope (s-SNOM), we managed to show that the graphene plasmons can be tuned and improved using a facile chemical doping method. Specifically, the plasmon interference patterns near the edge of the monolayer graphene were substantially enhanced via nitric acid (HNO3) exposure. The plasmon-related characteristics can be deduced by analyzing such plasmonic fringes, which exhibited a longer plasmon wavelength and reduced plasmon damping rate. In addition, the local carrier density and therefore the Fermi energy level (EF) of graphene can be obtained from the plasmonic nano-imaging, which indicated that the enhanced plasmon oscillation originated from the injection of free holes into graphene by HNO3. These findings were further corroborated by theoretical calculations using density functional theory (DFT). We believe that our findings provide a clear nanoscale picture on improving graphene plasmonics by chemical doping, which will be helpful for optimizing graphene plasmonics and for elucidating the mechanisms of two-dimensional light confinement by atomically thick materials.

Janus magneto-electric nanosphere dimers exhibiting unidirectional visible light scattering and strong electromagnetic field enhancement.

Steering incident light into specific directions at the nanoscale is very important for future nanophotonics applications of signal transmission and detection. A prerequisite for such a purpose is the development of nanostructures with high-efficiency unidirectional light scattering properties. Here, from both theoretical and experimental sides, we conceived and demonstrated the unidirectional visible light scattering behaviors of a heterostructure, Janus dimer composed of gold and silicon nanospheres. By carefully adjusting the sizes and spacings of the two nanospheres, the Janus dimer can support both electric and magnetic dipole modes with spectral overlaps and comparable strengths. The interference of these two modes gives rise to the narrow-band unidirectional scattering behaviors with enhanced forward scattering and suppressed backward scattering. The directionality can further be improved by arranging the dimers into one-dimensional chain structures. In addition, the dimers also show remarkable electromagnetic field enhancements. These results will be important not only for applications of light emitting devices, solar cells, optical filters, and various surface enhanced spectroscopies but also for furthering our understanding on the light-matter interactions at the nanoscale.

A centimeter-scale sub-10 nm gap plasmonic nanorod array film as a versatile platform for enhancing light-matter interactions.

Strongly coupled plasmonic nanostructures with sub-10 nm gaps can enable intense electric field enhancements which greatly benefit the various light-matter interactions. From the point view of practical applications, such nanostructures should be of low-cost, facile fabrication and processing, large-scale with high-yield of the ultrasmall gaps, and easy for integration with other functional components. However, nowadays techniques for reliable fabrication of these nanostructures usually involve complex, time-consuming, and expensive lithography procedures, which are limited either by their low-throughput or the small areas obtained. On the other hand, so far most of the studies on the sub-10 nm gap nanostructures mainly focused on the surface-enhanced Raman scattering and high-harmonic generations, while leaving other nonlinear optical properties unexplored. In this work, using a scalable process without any lithography procedures, we demonstrated a centimeter-scale ordered plasmonic nanorod array film (PNRAF) with well-defined sub-10 nm interparticle gaps as a versatile platform for strongly enhanced light-matter interactions. Specifically, we showed that due to its plasmon-induced localized electromagnetic field enhancements, the Au PNRAF could exhibit extraordinary intrinsic multi-photon avalanche luminescence (MAPL) and nonlinear saturable absorption (SA). Furthermore, the PNRAF can be easily integrated with semiconductor quantum dots (SQDs) as well as wide bandgap semiconductors to strongly enhance their fluorescence and photocurrent response, respectively. Our method can be easily generalized to nanorod array films consisting of other plasmonic metals and even semiconductor materials, which can have multiple functionalities derived from different materials. Overall, the findings in our study have offered a potential strategy for design and fabrication of nanostructures with ultrasmall gaps for future photonic and optoelectronic applications.