Superior Visible Photoelectric Response with Au/Cu2NiSnS4 Core-Shell Nanocrystals.

The incorporation of plasmonic metal nanostructures into semiconducting chalcogenides in the form of core-shell structures provides a promising approach to enhancing the performance of photodetectors. In this study, we combined Au nanoparticles with newly developed copper-based chalcogenides Cu2NiSnS4 (Au/CNTS) to achieve an ultrahigh optoelectronic response in the visible regime. The high-quality Au/CNTS core-shell nanocrystals (NCs) were synthesized by developing a unique colloidal hot-injection method, which allowed for excellent control over sizes, shapes, and elemental compositions. The as-synthesized Au/CNTS hybrid core-shell NCs exhibited enhanced optical absorption, carrier extraction efficiency, and improved photosensing performance owing to the plasmonic-induced resonance energy transfer effect of the Au core. This effect led to a significant increase in the carrier density of the Au/CNTS NCs, resulting in a measured responsivity of 1.2 × 103 AW-1, a specific detectivity of 6.2 × 1011 Jones, and an external quantum efficiency of 3.8 × 105 % at an incident power density of 318.5 µW cm-2. These results enlighten a new era in the development of plasmonic core-shell nanostructure-based visible photodetectors.

Ultralow Auger-Assisted Interlayer Exciton Annihilation in WS2/WSe2 Moiré Heterobilayers.

Transition metal dichalcogenide (TMD) heterobilayers have emerged as a promising platform for exploring solid-state quantum simulators and many-body quantum phenomena. Their type II band alignment, combined with the moiré superlattice, inevitably leads to nontrivial exciton interactions and dynamics. Here, we unveil the distinct Auger annihilation processes for delocalized interlayer excitons in WS2/WSe2 moiré heterobilayers. By fitting the characteristic efficiency droop and bimolecular recombination rate, we quantitatively determine an ultralow Auger coefficient of 1.3 × 10-5 cm2 s-1, which is >100-fold smaller than that of excitons in TMD monolayers. In addition, we reveal selective exciton upconversion into the WSe2 layer, which highlights the significance of intralayer electron Coulomb interactions in dictating the microscopic scattering pathways. The distinct Auger processes arising from spatial electron-hole separation have important implications for TMD heterobilayers while endowing interlayer excitons and their strongly correlated states with unique layer degrees of freedom.

Room-Temperature Gate Voltage Modulation of Plasmonic Nanolasers.

Stable electrical modulation of plasmonic nanolasers is achieved on a hybrid graphene-insulator-metal (GIM) platform at room temperature. To support surface plasmon polariton (SPP) resonance, a zinc oxide (ZnO) nanowire is placed on the GIM platform to create a plasmonic cavity with a compact mode volume of 2.6 × 10-2 λ3, and the graphene layer is used as a transparent electrode for electrical modulation. When a gate voltage is applied, the surface electron density of Al varied, which results in the shifting of its plasma frequency and thus affects its SPP dispersion. In particular, this variation strongly changes the internal loss of the SPP mode; thus, the lasing thresholds of the ZnO nanowire plasmonic nanolasers on the GIM platform can be modulated by the gate voltage. This study demonstrates the gate voltage modulation of ZnO nanowire plasmonic nanolasers on a GIM platform at room temperature. These nanolasers can exhibit ultrahigh modulation speed on the order of terahertz. Accordingly, plasmonic nanolasers with gate voltage modulation have high potential for plasmonic circuit applications with high operation speed and versatility.

Ultrathin TiN Epitaxial Films as Transparent Conductive Electrodes.

Titanium nitride (TiN), a transition-metal compound with tight covalent Ti-N bonding, has a high melting temperature and superior mechanical and chemical stabilities compared to noble metals. With a reduction in thickness, the optical transmittance of TiN films can be drastically increased, and in combination with its excellent electrical conductivity, the ultrathin and continuous TiN film can be considered as an ideal alternative of the metal oxide electrodes. However, the deposition of ultrathin and continuous metallic layer with a smooth surface morphology is a major challenge for typical deposition methods such as thermal evaporation or reactive sputtering. In particular, defects mainly related with oxygen contents and surface scattering can significantly limit the performance of ultrathin TiN films. In this work, ultrathin TiN films with 2-10 nm in thickness are grown by using the nitrogen plasma-assisted molecular-beam epitaxy (MBE) method in an ultrahigh vacuum environment. Excellent surface morphology with a root-mean-square roughness of ≤0.12 nm and a high optical transparency of 75% over the whole visible regime are achieved for ultrathin TiN epitaxial films. The dielectric properties determined by the spectroscopic ellipsometry and the electrical properties measured by the terahertz spectroscopy and the Hall effect method reveal that the percolation thickness of the TiN epitaxial film is less than 2.4 nm and its electrical conductivity is higher than 1.1 × 104 Ω-1 cm-1. These features make MBE-grown ultrathin TiN epitaxial films a good candidate for robust, low cost, and large-area transparent conductive electrodes.

Flexible Plasmonics Using Aluminum and Copper Epitaxial Films on Mica.

We demonstrate here the growth of aluminum (Al), copper (Cu), gold (Au), and silver (Ag) epitaxial films on two-dimensional, layered muscovite mica (Mica) substrates via van der Waals (vdW) heteroepitaxy with controllable film thicknesses from a few to hundreds of nanometers. In this approach, the mica thin sheet acts as a flexible and transparent substrate for vdW heteroepitaxy, which allows for large-area formation of atomically smooth, single-crystalline, and ultrathin plasmonic metals without the issue of film dewetting. The high-quality plasmonic metal films grown on mica enable us to design and fabricate well-controlled Al and Cu plasmonic nanostructures with tunable surface plasmon resonances ranging from visible to the near-infrared spectral region. Using these films, two kinds of plasmonic device applications are reported, including (1) plasmonic sensors with high effective index sensitivities based on surface plasmon interferometers fabricated on the Al/Mica film and (2) Cu/Mica nanoslit arrays for plasmonic color filters in the visible and near-infrared regions. Furthermore, we show that the responses of plasmonic nanostructures fabricated on the Mica substrates remain unaltered under large substrate bending conditions. Therefore, the metal-on-mica vdW heteroepitaxy platform is suitable for flexible plasmonics based on their bendable properties.

Demonstration of a Superior Deep-UV Surface-Enhanced Resonance Raman Scattering (SERRS) Substrate and Single-Base Mutation Detection in Oligonucleotides.

In life science, rapid mutation detection in oligonucleotides is in a great demand for genomic and medical screening. To satisfy this demand, surface-enhanced resonance Raman spectroscopy (SERRS) in the deep-UV (DUV) regime offers a promising solution due to its merits of label-free nature, strong electromagnetic confinement, and charge transfer effect. Here, we demonstrate an epitaxial aluminum (Al) DUV-SERRS substrate that resonates effectively with the incident Raman laser and the ss-DNA at 266 nm, yielding significant SERRS signals of the detected analytes. For the first time, to the best of our knowledge, we obtaine SERRS spectra for all bases of oligonucleotides, not only revealing maximum characteristic Raman peaks but also recording the highest enhancement factor of up to 106 for a 1 nm thick adenine monomer. Moreover, our epitaxial Al DUV-SERRS substrate is able to enhance the Raman signal of all four bases of 12-mer ss-DNA and to further linearly quantify the single-base mutation in the 12-mer ss-DNA.

Enhanced Spontaneous Emission of Monolayer MoS2 on Epitaxially Grown Titanium Nitride Epsilon-Near-Zero Thin Films.

Room-temperature photoluminescence enhancement of molybdenum disulfide (MoS2) monolayers on epitaxial titanium nitride (TiN) thin films grown by molecular-beam-epitaxy as well as magnetron-sputtered TiN films is observed by a confocal laser scanning microscope with excitation wavelengths covering the transition of TiN's macroscopic optical properties from dielectric to plasmonic. The photoluminescence enhancement increases as TiN becomes more metallic, and strong enhancement is obtained at the excitation wavelengths equal to or longer than the epsilon-near-zero (ENZ) wavelength of TiN films. A good agreement is observed between measured and calculated enhancements. The enhancement is attributed to the increased excitation field in MoS2 at TiN's ENZ wavelength and interference effects for thick spacers that separate the MoS2 flakes from TiN films in the metallic regime. This study enriches the fundamental understanding of emission properties on ENZ substrates that could be important for the development of advanced nanoscale lasers/light sources, optical/biosensors, and nano-optoelectronic devices.

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.

An Ultrasensitive Gateless Photodetector Based on the 2D Bilayer MoS2-1D Si Nanowire-0D Ag Nanoparticle Hybrid Structure.

Atomically thin transition metal dichalcogenides (TMDC) have received much attention due to their wide variety of optical and electronic properties. Among various TMDC materials, molybdenum disulfide (MoS2) has been intensely studied owing to its potential applications in nanoelectronics and optoelectronics. However, two-dimensional MoS2 photodetectors suffer from low responsivity due to low optical cross section. Combining MoS2 with plasmonic nanostructures can drastically increase scattering cross section and enhance local light-matter interaction. Moreover, suspended MoS2 has been shown to exhibit higher photoluminescence intensity and strong photogating effect, which can be employed in photodetectors. Herein, we propose an approach to utilize plasmonic nanostructures and physical suspension for 2D MoS2 photosensing enhancement by hybridizing 2D bilayer MoS2, 1D silicon nanowires, and 0D silver nanoparticles. The hybrid structure shows a gateless responsivity of 402.4 A/W at a wavelength of 532 nm, which represents the highest value among the ever reported gateless plasmonic MoS2 photodetector. The great responsivity and large active area results in an exceptional detectivity of 2.34 × 1012 Jones. This study provides a new approach for designing high-performance 2D TMDC-based optoelectronic devices.

Engineering Giant Rabi Splitting via Strong Coupling between Localized and Propagating Plasmon Modes on Metal Surface Lattices: Observation of √N Scaling Rule.

We present a strong coupling system realized by coupling the localized surface plasmon mode in individual silver nanogrooves and propagating surface plasmon modes launched by periodic nanogroove arrays with varied periodicities on a continuous silver medium. When the propagating modes are in resonance with the localized mode, we observe a √N scaling of Rabi splitting energy, where N is the number of propagating modes coupled to the localized mode. Here, we confirm a giant Rabi splitting on the order of 450-660 meV (N = 2) in the visible spectral range, and the corresponding coupling strength is 160-235 meV. In some of the strong coupling cases studied by us, the coupling strength is about 10% of the mode energy, reaching the ultrastrong coupling regime.

Current Modulation of Plasmonic Nanolasers by Breaking Reciprocity on Hybrid Graphene-Insulator-Metal Platforms.

A hybrid graphene-insulator-metal (GIM) platform is proposed with a supported surface plasmon polariton (SPP) wave that can be manipulated by breaking Lorentz reciprocity. The ZnO SPP nanowire lasers on the GIM platforms are demonstrated up to room temperature to be actively modulated by applying external current to graphene, which transforms the cavity mode from the standing to propagation wave pattern. With applying 100 mA external current, the laser threshold increases by ≈100% and a 1.2 nm Doppler shift is observed due to the nonreciprocal propagation characteristic. The nanolaser performance also depends on the orientation of the nanowire with respect to the current flow direction. The GIM platform can be a promising platform for integrated plasmonic system functioning laser generation, modulation, and detection.

Aluminum Plasmonics Enriched Ultraviolet GaN Photodetector with Ultrahigh Responsivity, Detectivity, and Broad Bandwidth.

Plasmonics have been well investigated on photodetectors, particularly in IR and visible regimes. However, for a wide range of ultraviolet (UV) applications, plasmonics remain unavailable mainly because of the constrained optical properties of applicable plasmonic materials in the UV regime. Therefore, an epitaxial single-crystalline aluminum (Al) film, an abundant metal with high plasma frequency and low intrinsic loss is fabricated, on a wide bandgap semiconductive gallium nitride (GaN) to form a UV photodetector. By deliberately designing a periodic nanohole array in this Al film, localized surface plasmon resonance and extraordinary transmission are enabled; hence, the maximum responsivity (670 A W-1) and highest detectivity (1.48 × 1015 cm Hz1/2 W-1) is obtained at the resonance wavelength of 355 nm. In addition, owing to coupling among nanoholes, the bandwidth expands substantially, encompassing the entire UV range. Finally, a Schottky contact is formed between the single-crystalline Al nanohole array and the GaN substrate, resulting in a fast temporal response with a rise time of 51 ms and a fall time of 197 ms. To the best knowledge, the presented detectivity is the highest compared with those of other reported GaN photodetectors.

Low-loss aluminum epitaxial film for scalable and sustainable plasmonics: direct comparison with silver epitaxial film.

Aluminum is a plasmonic material well known for its excellent stability, complementary metal-oxide-semiconductor compatibility and wide availability as compared to popular plasmonic materials such as gold and silver. Aluminum can support surface plasmon resonances in a broad spectral range, including the deep ultra-violet, a regime where no other plasmonic materials can work. However, conventional aluminum films suffer from high losses in the visible region and low fidelity and reproducibility in nanofabrication, making aluminum plasmonics non-ideal for applications. Herein, we report the experimental results of consistent surface plasmon propagation length measurements for epitaxially grown aluminum and silver films (epifilms), using three different methods (white light interferometry, laser scattering and spectroscopic ellipsometry) in the full visible spectrum. In order to avoid losses caused by inferior material quality, we used single-crystalline aluminum and silver films for direct comparison. We found that, on directly comparing with the silver epifilm, the aluminum epifilm possesses reasonably long plasmon propagation lengths in the full visible range and outperforms silver in the deep blue region. These results illustrate the great potential of epitaxial aluminum films for visible-spectrum plasmonic applications, resulting from their superior crystallinity and excellent surface and interface properties.

ZnO Nanowires on Single-Crystalline Aluminum Film Coupled with an Insulating WO3 Interlayer Manifesting Low Threshold SPP Laser Operation.

ZnO nanowire-based surface plasmon polariton (SPP) nanolasers with metal-insulator-semiconductor hierarchical nanostructures have emerged as potential candidates for integrated photonic applications. In the present study, we demonstrated an SPP nanolaser consisting of ZnO nanowires coupled with a single-crystalline aluminum (Al) film and a WO3 dielectric interlayer. High-quality ZnO nanowires were prepared using a vapor phase transport and condensation deposition process via catalyzed growth. Subsequently, prepared ZnO nanowires were transferred onto a single-crystalline Al film grown by molecular beam epitaxy (MBE). Meanwhile, a WO3 dielectric interlayer was deposited between the ZnO nanowires and Al film, via e-beam technique, to prevent the optical loss from dominating the metallic region. The metal-oxide-semiconductor (MOS) structured SPP laser, with an optimal WO3 insulating layer thickness of 3.6 nm, demonstrated an ultra-low threshold laser operation (lasing threshold of 0.79 MW cm-2). This threshold value was nearly eight times lower than that previously reported in similar ZnO/Al2O3/Al plasmonic lasers, which were ≈2.4 and ≈3 times suppressed compared to the SPP laser, with WO3 insulating layer thicknesses of 5 nm and 8 nm, respectively. Such suppression of the lasing threshold is attributed to the WO3 insulating layer, which mediated the strong confinement of the optical field in the subwavelength regime.

Moiré potential impedes interlayer exciton diffusion in van der Waals heterostructures.

The properties of van der Waals heterostructures are drastically altered by a tunable moiré superlattice arising from periodically varying atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers suggested that carriers and excitons exhibit long diffusion, a rich variety of scenarios can exist. In a moiré crystal with a large supercell and deep potential, interlayer excitons may be completely localized. As the moiré period reduces at a larger twist angle, excitons can tunnel between supercells and diffuse over a longer lifetime. The diffusion should be the longest in commensurate heterostructures where the moiré superlattice is completely absent. Here, we experimentally demonstrate the rich phenomena of interlayer exciton diffusion in WSe2/MoSe2 heterostructures by comparing several samples prepared with chemical vapor deposition and mechanical stacking with accurately controlled twist angles.

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.

Chiral Second-Harmonic Generation from Monolayer WS2/Aluminum Plasmonic Vortex Metalens.

Two-dimensional spiral plasmonic structures have emerged as a versatile approach to generate near-field vortex fields with tunable topological charges. We demonstrate here a far-field approach to observe the chiral second-harmonic generation (SHG) at designated visible wavelengths from a single plasmonic vortex metalens. This metalens comprises an Archimedean spiral slit fabricated on atomically flat aluminum epitaxial film, which allows for precise tuning of plasmonic resonances and subsequent transfer of two-dimensional materials on top of the spiral slit. The nonlinear optical measurements show a giant SHG circular dichroism. Furthermore, we have achieved an enhanced chiral SHG conversion efficiency (about an order of magnitude greater than the bare aluminum lens) from monolayer tungsten disulfide (WS2)/aluminum metalens, which is designed at the C-exciton resonance of WS2. Since the C-exciton is not a valley exciton, the enhanced chiral SHG in this hybrid system originates from the plasmonic vortex field-enhanced SHG under the optical spin-orbit interaction.

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.

Plasmonic Nanolasers Enhanced by Hybrid Graphene-Insulator-Metal Structures.

Graphene is a two-dimensional (2D) structure that creates a linear relationship between energy and momentum that not only forms massless Dirac fermions with extremely high group velocity but also exhibits a broadband transmission from 300 to 2500 nm that can be applied to many optoelectronic applications, such as solar cells, light-emitting devices, touchscreens, ultrafast photodetectors, and lasers. Although the plasmonic resonance of graphene occurs in the terahertz band, graphene can be combined with a noble metal to provide a versatile platform for supporting surface plasmon waves. In this study, we propose a hybrid graphene-insulator-metal (GIM) structure that can modulate the surface plasmon polariton (SPP) dispersion characteristics and thus influence the performance of plasmonic nanolasers. Compared with values obtained when graphene is not used on an Al template, the propagation length of SPP waves can be increased 2-fold, and the threshold of nanolasers is reduced by 50% when graphene is incorporated on the template. The GIM structure can be further applied in the future to realize electrical control or electrical injection of plasmonic devices through graphene.

Epitaxial Growth of Optically Thick, Single Crystalline Silver Films for Plasmonics.

Single crystalline Ag films on dielectric substrates have received tremendous attention recently due to their technological potentials as low loss plasmonic materials. Two different growth approaches have been used to produce single crystalline Ag films previously. One approach is based on repetitive cycles of a two-step process (low temperature deposition followed by RT annealing) using molecular beam epitaxy (MBE), which is extremely time-consuming due to the need for repeat growth cycles. Another approach is based on rapid e-beam deposition which is capable of growing thick single crystalline Ag films (>300 nm) but lacks the precision in thickness control of thin epitaxial films. Here, we report a universal approach to grow atomically smooth epitaxial Ag films by eliminating the repetitive cycles used in the previous two-step MBE method while maintaining the precise thickness control from a few monolayers to the optically thick regime, thus overcoming the limitations of the two aforementioned methods. In addition, we develop an in situ growth of aluminum oxide as the capping layer to protect the epitaxial Ag films. The quality of the epitaxial Ag films was evaluated using a variety of techniques, and the superior optical performance of the films is demonstrated by measuring the propagation length of surface plasmon polaritons (∼80 µm at 632 nm) as well as their capability to support a plasmonic nanolaser in infrared incorporating an InGaAsP quantum well as the gain media.