Linear Electro-Optic Effect in 2D Ferroelectric for Electrically Tunable Metalens.

The advent of 2D ferroelectrics, characterized by their spontaneous polarization states in layer-by-layer domains without the limitation of a finite size effect, brings enormous promise for applications in integrated optoelectronic devices. Comparing with semiconductor/insulator devices, ferroelectric devices show natural advantages such as non-volatility, low energy consumption and high response speed. Several 2D ferroelectric materials have been reported, however, the device implementation particularly for optoelectronic application remains largely hypothetical. Here, the linear electro-optic effect in 2D ferroelectrics is discovered and electrically tunable 2D ferroelectric metalens is demonstrated. The linear electric-field modulation of light is verified in 2D ferroelectric CuInP2S6. The in-plane phase retardation can be continuously tuned by a transverse DC electric field, yielding an effective electro-optic coefficient rc of 20.28 pm V-1. The CuInP2S6 crystal exhibits birefringence with the fast axis oriented along its (010) plane. The 2D ferroelectric Fresnel metalens shows efficacious focusing ability with an electrical modulation efficiency of the focusing exceeding 34%. The theoretical analysis uncovers the origin of the birefringence and unveil its ultralow light absorption across a wide wavelength range in this non-excitonic system. The van der Waals ferroelectrics enable room-temperature electrical modulation of light and offer the freedom of heterogeneous integration with silicon and another material system for highly compact and tunable photonics and metaoptics.

Electrical Control Grain Dimensionality with Multilevel Magnetic Anisotropy.

In alignment with the increasing demand for larger storage capacity and longer data retention, the electrical control of magnetic anisotropy has been a research focus in the realm of spintronics. Typically, magnetic anisotropy is determined by grain dimensionality, which is set during the fabrication of magnetic thin films. Despite the intrinsic correlation between magnetic anisotropy and grain dimensionality, there is a lack of experimental evidence for electrically controlling grain dimensionality, thereby impairing the efficiency of magnetic anisotropy modulation. Here, we demonstrate an electric field control of grain dimensionality and prove it as the active mechanism for tuning interfacial magnetism. The reduction in grain dimensionality is associated with a transition from ferromagnetic to superparamagnetic behavior. We achieve a nonvolatile and reversible modulation of the coercivity in both the ferromagnetic and superparamagnetic regimes. Subsequent electrical and elemental analysis confirms the variation in grain dimensionality upon the application of gate voltages, revealing a transition from a multidomain to a single-domain state, accompanied by a reduction in grain dimensionality. Furthermore, we exploit the influence of grain dimensionality on domain wall motion, extending its applicability to multilevel magnetic memory and synaptic devices. Our results provide a strategy for tuning interfacial magnetism through grain size engineering for advancements in high-performance spintronics.

Giant Third-Order Nonlinear Hall Effect in Misfit Layer Compound (SnS)1.17(NbS2)3.

The nonlinear Hall effect (NLHE) holds immense significance in recognizing the band geometry and its potential applications in current rectification. Recent discoveries have expanded the study from second-order to third-order nonlinear Hall effect (THE), which is governed by an intrinsic band geometric quantity called the Berry Connection Polarizability tensor. Here we demonstrate a giant THE in a misfit layer compound, (SnS)1.17(NbS2)3. While the THE is prohibited in individual NbS2 and SnS due to the constraints imposed by the crystal symmetry and their band structures, a remarkable THE emerges when a superlattice is formed by introducing a monolayer of SnS. The angular-dependent THE and its scaling relationship indicate that the phenomenon could be correlated to the band geometry modulation, concurrently with the symmetry breaking. The resulting strength of THE is orders of magnitude higher compared to recent studies. Our work illuminates the modulation of structural and electronic geometries for novel quantum phenomena through interface engineering.

Liquid-Metal-Printed Ultrathin Oxides for Atomically Smooth 2D Material Heterostructures.

Two-dimensional (2D) semiconductors are promising channel materials for continued downscaling of complementary metal-oxide-semiconductor (CMOS) logic circuits. However, their full potential continues to be limited by a lack of scalable high-k dielectrics that can achieve atomically smooth interfaces, small equivalent oxide thicknesses (EOTs), excellent gate control, and low leakage currents. Here, large-area liquid-metal-printed ultrathin Ga2O3 dielectrics for 2D electronics and optoelectronics are reported. The atomically smooth Ga2O3/WS2 interfaces enabled by the conformal nature of liquid metal printing are directly visualized. Atomic layer deposition compatibility with high-k Ga2O3/HfO2 top-gate dielectric stacks on a chemical-vapor-deposition-grown monolayer WS2 is demonstrated, achieving EOTs of ∼1 nm and subthreshold swings down to 84.9 mV/dec. Gate leakage currents are well within requirements for ultrascaled low-power logic circuits. These results show that liquid-metal-printed oxides can bridge a crucial gap in dielectric integration of 2D materials for next-generation nanoelectronics.

Low Energy Switching of Phase Change Materials Using a 2D Thermal Boundary Layer.

The switchable optical and electrical properties of phase change materials (PCMs) are finding new applications beyond data storage in reconfigurable photonic devices. However, high power heat pulses are needed to melt-quench the material from crystalline to amorphous. This is especially true in silicon photonics, where the high thermal conductivity of the waveguide material makes heating the PCM energy inefficient. Here, we improve the energy efficiency of the laser-induced phase transitions by inserting a layer of two-dimensional (2D) material, either MoS2 or WS2, between the silica or silicon substrate and the PCM. The 2D material reduces the required laser power by at least 40% during the amorphization (RESET) process, depending on the substrate. Thermal simulations confirm that both MoS2 and WS2 2D layers act as a thermal barrier, which efficiently confines energy within the PCM layer. Remarkably, the thermal insulation effect of the 2D layer is equivalent to a ∼100 nm layer of SiO2. The high thermal boundary resistance induced by the van der Waals (vdW)-bonded layers limits the thermal diffusion through the layer interface. Hence, 2D materials with stable vdW interfaces can be used to improve the thermal efficiency of PCM-tuned Si photonic devices. Furthermore, our waveguide simulations show that the 2D layer does not affect the propagating mode in the Si waveguide; thus, this simple additional thin film produces a substantial energy efficiency improvement without degrading the optical performance of the waveguide. Our findings pave the way for energy-efficient laser-induced structural phase transitions in PCM-based reconfigurable photonic devices.

Rashba-Edelstein Effect in the h-BN Van Der Waals Interface for Magnetization Switching.

Van der Waals materials are attracting great attention in the field of spintronics due to their novel physical properties. For example, they are utilized as spin-current generating materials in spin-orbit torque (SOT) devices, which offers an electrical way to control the magnetic state and is promising for future low-power electronics. However, SOTs have mostly been demonstrated in vdW materials with strong spin-orbit coupling (SOC). Here, the observation of a current-induced SOT in the h-BN/SrRuO3 bilayer structure is reported, where the vdW material (h-BN) is an insulator with negligible SOC. Importantly, this SOT is strong enough to induce the switching of the perpendicular magnetization in SrRuO3 . First-principles calculations suggest a giant Rashba effect at the interface between vdW material and SrRuO3 (110)pc thin film, which leads to the observed SOT based on a simplified tight-binding model. Furthermore, it is demonstrated that the current-induced magnetization switching can be modulated by the electric field. This study paves the way for exploring the current-induced SOT and magnetization switching by integrating vdW materials with ferromagnets.

Aqueous Synthesis, Doping, and Processing of n-Type Ag2Se for High Thermoelectric Performance at Near-Room-Temperature.

Herein, we have successfully synthesized binary Ag2Se, composite Ag0:Ag2Se, and ternary Cu+:Ag2Se through an ambient aqueous-solution-based approach in a one-pot reaction at room temperature and atmospheric pressure without involving high-temperature heating, multiple-processes treatment, and organic solvents/surfactants. Effective controllability over phases and compositions/components are demonstrated with feasibility for large-scale production through an exquisite alteration in reaction parameters especially pH for enhancing and understanding thermoelectric properties. Thermoelectric ZT reaches 0.8-1.1 at near-room-temperature for n-type Ag2Se and Cu+ doping further improves to 0.9-1.2 over a temperature range of 300-393 K, which is the largest compared to that reported by wet chemistry methods. This improvement is related to the enhanced electrical conductivity and the suppressed thermal conductivity due to the incorporation of Cu+ into the lattice of Ag2Se at very low concentrations (x%Cu+:Ag2Se, x = 1.0, 1.5, and 2.0).

Gate-Defined Quantum Confinement in CVD 2D WS2.

Temperature-dependent transport measurements are performed on the same set of chemical vapor deposition (CVD)-grown WS2 single- and bilayer devices before and after atomic layer deposition (ALD) of HfO2 . This isolates the influence of HfO2 deposition on low-temperature carrier transport and shows that carrier mobility is not charge impurity limited as commonly thought, but due to another important but commonly overlooked factor: interface roughness. This finding is corroborated by circular dichroic photoluminescence spectroscopy, X-ray photoemission spectroscopy, cross-sectional scanning transmission electron microscopy, carrier-transport modeling, and density functional modeling. Finally, electrostatic gate-defined quantum confinement is demonstrated using a scalable approach of large-area CVD-grown bilayer WS2 and ALD-grown HfO2 . The high dielectric constant and low leakage current enabled by HfO2 allows an estimated quantum dot size as small as 58 nm. The ability to lithographically define increasingly smaller devices is especially important for transition metal dichalcogenides due to their large effective masses, and should pave the way toward their use in quantum information processing applications.

A portable SERS sensor for pyocyanin detection in simulated wound fluid and through swab sampling.

A portable surface-enhanced Raman spectroscopy (SERS) sensor for detecting pyocyanin (PYO) in simulated wound fluid and from bacteria samples was developed. Solution-phase SERS detection protocols are designed to be compatible with two different clinical practices for wound exudate collection, namely negative pressure liquid collection and swabbing. For citrate-coated metal nanoparticles of three different compositions, i.e. gold (AuNPs), alloyed silver/gold (AgAuNPs), and silver (AgNPs), we firstly confirmed their interaction with PYO in the complex wound fluid, using fluorescence quenching experiments, which rationalized the Raman enhancement effects. We then demonstrated the Raman enhancement effects of the metal nanoparticles in the order of AgNPs > AgAuNPs > AuNPs. The limit of detection (LOD) achieved for PYO is 1.1 µM (in a linear range of 0.1-25 µM by the AgNPs), 10.9 µM (in a linear range of 5-100 µM, by the AgAuNPs), and 17.7 µM (in a linear range of 10-100 µM by the AuNPs). The AgNP and AgAuNP sensors together cover the sensitivity and dynamic range requirements for the clinical detection of wound infection, where PYO is present at a concentration of 1-50 µM. In addition, sterilized cotton swabs were used to collect wound fluid and transfer samples into AgNP solution for SERS measurements. This detection protocol was completed within 5 minutes with a LOD of 23.1 µM (in a linear range of 15-100 µM). The SERS sensing protocol was validated by its successful detection of PYO in cultured Pseudomonas aeruginosa bacteria. The findings presented in this work pave the way towards point-of-care diagnostics of wound infections.

Lithium Silicide Surface Enrichment: A Solution to Lithium Metal Battery.

The propensity of lithium dendrite formation during the charging process of lithium metal batteries is linked to inhomogeneity on the lithium surface layer. The high reactivity of lithium and the complex surface structure of the native layer create "hot spots" for fast dendritic growth. Here, it is demonstrated that a fundamental restructuring of the lithium surface in the form of lithium silicide (Lix Si) can effectively eliminate the surface inhomogeneity on the lithium surface. In situ optical microscopic study is carried out to monitor the electrochemical deposition of lithium on the Lix Si-modified lithium electrodes and the bare lithium electrode. It is observed that a much more uniform lithium dissolution/deposition on the Lix Si-modified lithium anode can be achieved as compared to the bare lithium electrode. Full cells paring the modified lithium anode with sulfur and LiFePO4 cathodes show excellent electrochemical performances in terms of rate capability and cycle stability. Compatibility of the anode enrichment method with mass production process also offers a practical way for enabling lithium metal anode for next-generation lithium batteries.

Nanoelectromechanical-systems-controlled bistability of double-coupled photonic crystal cavities.

In this Letter, we report an approach to controlling the bistability of double-coupled photonic crystal cavities with a nanoelectromechanical comb drive, in which the optical force and thermo-optic effect form a feedback mechanism to the effective index of the cavities, and the gap width between the cavities is steered by the comb drive. A model based on temporal coupled mode theory is established to analyze this approach. Hysteresis loops characterizing the bistability are experimentally achieved by sweeping the gap width forward and in reverse. In addition, the experiments also demonstrate that the bistability is tunable by varying the input light power.

New approach for multilayered microstructures fabrication based on a water-soluble backing substrate.

We demonstrate a new approach for woodpile microstructure fabrication. The method involves the use of polyvinyl alcohol (PVA) as a sacrificial substrate for the transfer of SU-8 films to prepatterned structures. The surface activated PVA substrate allows good wettability of SU-8 film and its solubility in water eliminates the need of delaminating SU-8 structures from the substrate. This makes the fabrication process much simplified and we successfully demonstrate eight-layer stacking of gratings. Fourier transform infrared spectra of single-layer and four-layer grating structures show a broader transmission dip spectrum compared to their film counterparts, indicating their potential use as broadband terahertz (THz) absorbers.

Metal-assisted photonic mode for ultrasmall bending with long propagation length at visible wavelengths.

In this work, we investigate the use of metal-assisted photonic guiding in a polymer-metal waveguide as an alternative approach for high density photonic integration at visible wavelengths. We demonstrate high confinement and long propagation length in sub-wavelength dimensions down to 300nm × 200nm using leakage radiation microscopy at a wavelength of 632.8 nm. Simulations using the finite element method (FEM) show that the optimum dimension that gives good confinement and propagation length is similar to that of the predicted plasmonic mode supported in the same waveguide. Under such optimum conditions, the metal-assisted photonic mode shows a five times longer propagation length and higher transmission efficiency for all 90° bending radius down to 1 µm compared to the plasmonic mode.

High aspect subdiffraction-limit photolithography via a silver superlens.

Photolithography is the technology of choice for mass patterning in semiconductor and data storage industries. Superlenses have demonstrated the capability of subdiffraction-limit imaging and been envisioned as a promising technology for potential nanophotolithography. Unfortunately, subdiffraction-limit patterns generated by current superlenses exhibited poor profile depth far below the requirement for photolithography. Here, we report an experimental demonstration of sub-50 nm resolution nanophotolithography via a smooth silver superlens with a high aspect profile of ~45 nm, as well as grayscale subdiffraction-limit three-dimensional nanopatterning. Theoretical analysis and simulation show that smooth interfaces play a critical role. Superlens-based lithography can be integrated with conventional UV photolithography systems to endow them with the capability of nanophotolithography, which could provide a cost-effective approach for large scale and rapid nanopatterning.

Damping of the acoustic vibrations of individual gold nanoparticles.

In this letter, the ultrafast vibrational dynamics of individual gold nanorings has been investigated by femtosecond transient absorption spectroscopy. Two acoustic vibration modes have been detected and identified. The influence of the mechanical coupling at the nanoparticle/substrate interface on the acoustic vibrations of the nano-objects is discussed. Moreover, by changing the environment of the nanoring, we provide a clear evidence of the impact of the surrounding medium on the damping of the acoustic vibrations. Such results are reported here for the first time on individual nanoparticles. This work points out a new sensing method based on the sensitivity of the acoustic vibration damping to the surrounding medium.

Plasmonic properties of gold ring-disk nano-resonators: fine shape details matter.

Using numerical simulations, we demonstrate that fine shape details of gold nanoring-disks are responsible for significant modifications of their localized surface plasmon properties. The numerical results are supported by optical transmission measurements and by atomic force microscopy. In particular, we found that, depending on the ring wall sharpness, the spectral shift of the ring-like localized surface plasmon resonance can be as large as few hundred nanometers. These results shed the light on the strong sensitivity of the surface plasmon properties to very small deviations of the ring and disk shapes from the ideally flat surfaces and sharp edges. This effect is particularly important for tailoring the surface plasmon properties of metallic nanostructures presenting edges and wedges for applications in bio- and chemical sensing and for enhancement of light scattering.

Acousto-plasmonic and surface-enhanced Raman scattering properties of coupled gold nanospheres/nanodisk trimers.

This work is devoted to the fundamental understanding of the interaction between acoustic vibrations and surface plasmons in metallic nano-objects. The acoustoplasmonic properties of coupled spherical gold nanoparticles and nanodisk trimers are investigated experimentally by optical transmission measurements and resonant Raman scattering experiments. For excitation close to resonance with the localized surface plasmons of the nanodisk trimers, we are able to detect several intense Raman bands generated by the spherical gold nanoparticles. On the basis of both vibrational dynamics calculations and Raman selection rules, the measured Raman bands are assigned to fundamental and overtones of the quadrupolar and breathing vibration modes of the spherical gold nanoparticles. Simulations of the electric near-field intensity maps performed at the Raman probe wavelengths showed strong localization of the optical energy in the vicinity of the nanodisk trimers, thus corroborating the role of the interaction between the acoustic vibrations of the spherical nanoparticles and the surface plasmons of the nanodisk trimers. Acoustic phonons surface enhanced Raman scattering is here demonstrated for the first time for such coupled plasmonic systems. This work paves the way to surface plasmon engineering for sensing the vibrational properties of nanoparticles.

Gold nanoring trimers: a versatile structure for infrared sensing.

In this work we report on the observation of surface plasmon properties of periodic arrays of gold nanoring trimers fabricated by electron beam lithography. It is shown that the localized surface plasmon resonances of such gold ring trimers occur in the infrared spectral region and are strongly influenced by the nanoring geometry and their relative positions. Based on numerical simulations of the optical extinction spectra and of the electric near-field intensity maps, the resonances are assigned to surface plasmon states arising from the strong intra-trimer electromagnetic interaction. We show that the nanoring trimer configuration allows for generating infrared surface plasmon resonances associated with strongly localized electromagnetic energy, thus providing plasmonic nanoresonators well-suited for sensing and surface enhanced near-infrared Raman spectroscopy.

Dual wavelength sensing based on interacting gold nanodisk trimers.

Fabrication and surface plasmon properties of gold nanostructures consisting of periodic arrays of disk trimers are reported. Using electron beam lithography, disk diameters as small as 96 nm and gaps between disks as narrow as 10 nm have been achieved with an unprecedented degree of control and reproducibility. The disk trimers exhibit intense visible and infrared surface plasmon resonances which are studied as a function of the disk diameter and of the pitch between trimers. Based on simulations of the optical extinction spectra and of the electric near-field intensity maps, the resonances are assigned to a single trimer response and to collective surface plasmon excitations involving electromagnetic interaction between the trimers. The sensing properties of the disk trimers are investigated using various coating media. The reported results demonstrate the possible use of gold disk trimers for dual wavelength chemical sensing.

Formation of interconnects with carbon nanotubes by nano-patterning and acoustics-assisted alignment.

In this work, the feasibility of self-assembling double-walled carbon nanotubes (DWCNTs) to form nano-sized interconnects over pre-fabricated gold electrodes using a combination of nanopatterning, surface functionalization and acoustics-assisted alignment of the DWCNTs was studied. Self-assembly and concurrent alignment of DWCNTs over the gold electrodes on selectively functionalized surfaces within nano-patterns took place in a fluid medium with the potential scalability for wafer-sized mass production. The adverse impacts of curvature and misalignment of DWCNTs on the chance of their attachment to the target zones were analyzed. Microscopic observations and electrical I-V curve measurements verified that DWCNT interconnects were indeed formed. The results indicated that the fabrication of self-assembled interconnects through the combined usage of nano-patterning, surface functionalization and DWCNT alignment is feasible and is in the right direction towards the fabrication of interconnects for future carbon nanotube-based devices and circuits.