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We introduce a new mechanism for second-harmonic generation through geometrically rectifying-funneling-ballistic electrons in THz optical resonators. Our resonant rectifiers inherently act as second-order harmonic generators, rectifying currents without the presence of a potential barrier. Particle-in-cell simulations reveal that femtosecond electron-surface scattering plays a critical role in this process. We differentiate electron funneling from nonlocal plasmonic drag and bulk Dirac anharmonicity, showing that funneling can reduce the required field intensity for second-harmonic generation by 3-4 orders of magnitude. We provide design guidelines for generating funneling-induced second-harmonic generation, including resonance mode matching and materials selection. This approach offers a practical pathway for low-field, geometrically tunable THz upconversion and rectification, operating from sub-10 THz to multiple tens of THz in graphene., Comment: The PDF file includes Main Text and Supplementary Information

Extreme light confinement down to the atomic scale has been theoretically predicted for ultrathin, Ta-based transition metal dichalcogenides (TMDs). In this work, we demonstrate in free-hanging 2H-TaS2 monolayers and bilayers slow light behaviour with a group velocity ~ $10^{-4}c$ and a lateral confinement ratio up to 300 at large wave vectors of $q = 0.15 \, \text{{\r{A}}}^{-1}$. Quantitative momentum-resolved electron energy loss spectroscopy (EELS) with an unprecedented momentum resolution of $0.0036 \, \text{{\r{A}}}^{-1}$ was used as a nanoscale optical platform. With it, momentum-dispersed, two-dimensional (2D) plasmon resonances were experimentally observed, showing a transition from 2D to 3D Coulomb interaction in the high-momentum regime, equivalent to light confinement volumes of $1\text{-}2 \, \text{nm}^3$. Remarkably, the resonant modes do not enter the electron-hole continuum, predicting even more enhanced optical field confinements for this material at cryogenic temperatures., Comment: Main Text and Supplemenary Information

Two-dimensional van der Waals semiconductors are promising for future nanoelectronics. However, integrating high-k gate dielectrics for device applications is challenging as the inert van der Waals material surfaces hinder uniform dielectric growth. Here, we report a liquid metal oxide-assisted approach to integrate ultrathin, high-k HfO2 dielectric on 2D semiconductors with atomically smooth interfaces. Using this approach, we fabricated 2D WS2 top-gated transistors with subthreshold swings down to 74.5 mV/dec, gate leakage current density below 10-6 A/cm2, and negligible hysteresis. We further demonstrate a one-step van der Waals integration of contacts and dielectrics on graphene. This can offer a scalable approach toward integrating entire prefabricated device stack arrays with 2D materials. Our work provides a scalable solution to address the crucial dielectric engineering challenge for 2D semiconductors, paving the way for high-performance 2D electronics.

As a burgeoning technique, out-of-focus electron ptychography offers the potential for rapidly imaging atomic-scale large fields of view (FoV) using a single diffraction dataset. However, achieving robust out-of-focus ptychographic reconstruction poses a significant challenge due to the inherent scan instabilities of electron microscopes, compounded by the presence of unknown aberrations in the probe-forming lens. In this study, we substantially enhance the robustness of out-of-focus ptychographic reconstruction by extending our previous calibration method (the Fourier method), which was originally developed for the in-focus scenario. This extended Fourier method surpasses existing calibration techniques by providing more reliable and accurate initialization of scan positions and electron probes. Additionally, we comprehensively explore and recommend optimized experimental parameters for robust out-of-focus ptychography, includingaperture size and defocus, through extensive simulations. Lastly, we conduct a comprehensive comparison between ptychographic reconstructions obtained with focused and defocused electron probes, particularly in the context of low-dose and precise phase imaging, utilizing our calibration method as the basis for evaluation., Comment: 22 pages, 6 figures

Correcting scan-positional errors is critical in achieving electron ptychography with both high resolution and high precision. This is a demanding and challenging task due to the sheer number of parameters that need to be optimized. For atomic-resolution ptychographic reconstructions, we found classical refining methods for scan positions not satisfactory due to the inherent entanglement between the object and scan positions, which can produce systematic errors in the results. Here, we propose a new protocol consisting of a series of constrained gradient descent (CGD) methods to achieve better recovery of scan positions. The central idea of these CGD methods is to utilize a priori knowledge about the nature of STEM experiments and add necessary constraints to isolate different types of scan positional errors during the iterative reconstruction process. Each constraint will be introduced with the help of simulated 4D-STEM datasets with known positional errors. Then the integrated constrained gradient decent (iCGD) protocol will be demonstrated using an experimental 4D-STEM dataset of the 1H-MoS2 monolayer. We will show that the iCGD protocol can effectively address the errors of scan positions across the spectrum and help to achieve electron ptychography with high accuracy and precision.

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 (EOT), excellent gate control, and low leakage currents. Here, we report liquid metal printed ultrathin and scalable Ga2O3 dielectric for 2D electronics and electro-optical devices. We directly visualize the atomically smooth Ga2O3/WS2 interfaces enabled by the conformal nature of liquid metal printing. We demonstrate atomic layer deposition compatibility with high-k Ga2O3/HfO2 top-gate dielectric stacks on chemical vapour deposition grown monolayer WS2, achieving EOTs of ~1 nm and subthreshold swings down to 84.9 mV/dec. Gate leakage currents are well within requirements for ultra-scaled low-power logic circuits. Our results show that liquid metal printed oxides can bridge a crucial gap in scalable dielectric integration of 2D materials for next-generation nano-electronics.

Phase change memory devices are typically reset by melt-quenching a material to radically lower its electrical conductance. The high power and concomitantly high current density required to reset phase change materials is the major issue that limits the access times of 3D phase change memory architectures. Phase change superlattices were developed to lower the reset energy by confining the phase transition to the interface between two different phase change materials. However, the high thermal conductivity of the superlattices means that heat is poorly confined within the phase change material, and most of the thermal energy is wasted to the surrounding materials. Here, we identified Ti as a useful dopant for substantially lowering the thermal conductivity of Sb2Te3-GeTe superlattices whilst also stabilising the layered structure from unwanted disordering. We demonstrate via laser heating that lowering the thermal conductivity by doping the Sb2Te3 layers with Ti halves the switching energy compared to superlattices that only use interfacial phase change transitions and strain engineering. The thermally optimized superlattice has (0 0 l) crystallographic orientation yet a thermal conductivity of just 0.25 W/m.K in the "on" (set) state. Prototype phase change memory devices that incorporate this Ti-doped superlattice switch faster and and at a substantially lower voltage than the undoped superlattice. During switching the Ti-doped Sb2Te3 layers remain stable within the superlattice and only the Ge atoms are active and undergo interfacial phase transitions. In conclusion, we show the potential of thermally optimised Sb2Te3-GeTe superlattices for a new generation of energy-efficient electrical and optical phase change memory., Comment: 4 Figures, 7 Supplementary Figures, 27 pages including a supplement

Three-dimensional (3D) imaging of thin, extended specimens at nanometer resolution is critical for applications in biology, materials science, advanced synthesis, and manufacturing. One route to 3D imaging is tomography, which requires a tilt series of a local region. Here we describe a coherent imaging alternative that recovers the 3D volume of a thin, homogeneously amorphous specimen with only a single, energy-filtered, bright-field image. We demonstrated this technique with a transmission electron microscope to fill a glaring gap for rapid, accessible, non-destructive 3D nanometrology. This technique is applicable, in general, to any coherent bright field imaging with electrons, photons, or any other wavelike particles., Comment: 28 pages, 12 figures

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 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 interfaces. 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., Comment: 34 pages, 12 figures

Chalcogenide phase change materials (PCMs) have been extensively applied in data storage, and they are now being proposed for high resolution displays, holographic displays, reprogrammable photonics, and all-optical neural networks. These wide-ranging applications all exploit the radical property contrast between the PCMs different structural phases, extremely fast switching speed, long-term stability, and low energy consumption. Designing PCM photonic devices requires an accurate model to predict the response of the device during phase transitions. Here, we describe an approach that accurately predicts the microstructure and optical response of phase change materials during laser induced heating. The framework couples the Gillespie Cellular Automata approach for modelling phase transitions with effective medium theory and Fresnel equations. The accuracy of the approach is verified by comparing the PCM optical response and microstructure evolution with the results of nanosecond laser switching experiments. We anticipate that this approach to simulating the switching response of PCMs will become an important component for designing and simulating programmable photonics devices. The method is particularly important for predicting the multi-level optical response of PCMs, which is important for all-optical neural networks and PCM-programmable perceptrons., Comment: 26 pages, 6 figures

Bound-states-in-the-continuum (BIC)is a wave-mechanical concept that generates resonances with vanishing spectral linewidths. It has many practical applications in Optics, such as narrow-band filters, mirror-less lasing, and nonlinear harmonic generation. As true BIC optical modes non-radiative and confined to the near field of nanostructures, they cannot be excited using propagating light. As a result, their direct experimental observation has been elusive. Rather than using light, we demonstrate probing BIC modes on arrays of silicon nanoantennas using a focused beam of electrons in a tranmission electron microscope. By combining cathodoluminescence (CL) and monochromated electron energy-loss spectroscopy (EELS) with controlled nanofabrication, we provide direct experimental evidence of "true" BIC modes, and demonstrate a BIC mode in the visible spectrum at 720 nm. The ability to observe and quantify these guided resonances with a spatial precision more than two orders of magnitude higher than previous far-field measurements allows the probing of individual elements in the nano-antenna arrays. The high-resolution experimental results are supported by numerical simulations as well as multipolar decomposition analysis, allowing us to demonstrate that the coherent interaction length of the quasi-BIC resonance requires at least 6 neighboring antenna elements, achieving over 60 times higher emissivity than for unpatterned silicon., Comment: 30 pages, 4 figures in the main text, 6 figures in the supplementary information

The accurate determination of the compositional fluctuations is pivotal in understanding their role in the reduction of efficiency in high indium content $In_{x}Ga_{1-x}N$ light-emitting diodes, the origin of which is still poorly understood. Here we have combined electron energy loss spectroscopy (EELS) imaging at sub-nanometer resolution with multiscale computational models to obtain a statistical distribution of the compositional fluctuations in $In_{x}Ga_{1-x}N$ quantum wells (QWs). Employing a multiscale computational model, we show the tendency of intrinsic compositional fluctuation in $In_{x}Ga_{1-x}N$ QWs at different Indium concentration and in the presence of strain. We have developed a systematic formalism based on the autonomous detection of compositional fluctuation in observed and simulated EELS maps. We have shown a direct comparison between the computationally predicted and experimentally observed compositional fluctuations. We have found that although a random alloy model captures the distribution of compositional fluctuations in relatively low In ($\sim$ 18%) content $In_{x}Ga_{1-x}N$ QWs, there exists a striking deviation from the model in higher In content ($\geq$ 24%) QWs. Our results highlight a distinct behavior in carrier localization driven by compositional fluctuations in the low and high In-content InGaN QWs, which would ultimately affect the performance of LEDs. Furthermore, our robust computational and atomic characterization method can be widely applied to study materials in which nanoscale compositional fluctuations play a significant role on the material performance., Comment: 38 pages, 5 Figures