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Thin-film optical diodes are important elements for miniaturizing photonic systems. However, the design of optical diodes relies on empirical and heuristic approaches. This poses a significant challenge for identifying optimal structural models of optical diodes at given wavelengths. Here, we leverage a quantum annealing-enhanced active learning scheme to automatically identify optimal designs of 130 nm-thick optical diodes. An optical diode is a stratified volume diffractive film discretized into rectangular pixels, where each pixel is assigned to either a metal or dielectric. The proposed scheme identifies the optimal material states of each pixel, maximizing the quality of optical isolation at given wavelengths. Consequently, we successfully identify optimal structures at three specific wavelengths (600, 800, and 1000 nm). In the best-case scenario, when the forward transmissivity is 85%, the backward transmissivity is 0.1%. Electromagnetic field profiles reveal that the designed diode strongly supports surface plasmons coupled across counterintuitive metal-dielectric pixel arrays. Thereby, it yields the transmission of first-order diffracted light with a high amplitude. In contrast, backward transmission has decoupled surface plasmons that redirect Poynting vectors back to the incident medium, resulting in near attenuation of its transmission. In addition, we experimentally verify the optical isolation function of the optical diode.
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Heat dissipation plays a crucial role in the performance and reliability of high-power GaN-based electronics. While AlN transition layers are commonly employed in the heteroepitaxial growth of GaN-on-SiC substrates, concerns have been raised about their impact on thermal transport across GaN/SiC interfaces. In this study, we present experimental measurements of the thermal boundary conductance (TBC) across GaN/SiC interfaces with varying thicknesses of the AlN transition layer (ranging from 0 to 73 nm) at different temperatures. Our findings reveal that the addition of an AlN transition layer leads to a notable increase in the TBC of the GaN/SiC interface, particularly at elevated temperatures. Structural characterization techniques are employed to understand the influence of the AlN transition layer on the crystalline quality of the GaN layer and its potential effects on interfacial thermal transport. To gain further insights into the trend of TBC, we conduct molecular dynamics simulations using high-fidelity deep learning-based interatomic potentials, which reproduce the experimentally observed enhancement in TBC even for atomically perfect interfaces. These results suggest that the enhanced TBC facilitated by the AlN intermediate layer could result from a combination of improved crystalline quality at the interface and the "phonon bridge" effect provided by AlN that enhances the overlap between the vibrational spectra of GaN and SiC.
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Electrolyte-gated transistors (EGTs) are promising candidates as artificial synapses owing to their precise conductance controllability, quick response times, and especially their low operating voltages resulting from ion-assisted signal transmission. However, it is still vague how ion-related physiochemical elements and working mechanisms impact synaptic performance. Here, to address the unclear correlations, we suggest a methodical approach based on electrochemical analysis using poly(ethylene oxide) EGTs with three alkali ions: Li+, Na+, and K+. Cyclic voltammetry is employed to identify the kind of electrochemical reactions taking place at the channel/electrolyte interface, which determines the nonvolatile memory functionality of the EGTs. Additionally, using electrochemical impedance spectroscopy and qualitative analysis of electrolytes, we confirm that the intrinsic properties of electrolytes (such as crystallinity, solubility, and ion conductivity) and ion dynamics ultimately define the linearity/symmetricity of conductance modulation. Through simple but systematic electrochemical analysis, these results offer useful insights for the selection of components for high-performing artificial synapses.
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Understanding the dynamics of surface bubble formation and growth on heated surfaces holds significant implications for diverse modern technologies. While such investigations are traditionally confined to terrestrial conditions, the expansion of space exploration and economy necessitates insights into thermal bubble phenomena in microgravity. In this work, we conduct experiments in the International Space Station to study surface bubble nucleation and growth in a microgravity environment and compare the results to those on Earth. Our findings reveal significantly accelerated bubble nucleation and growth rates, outpacing the terrestrial rates by up to ~30 times. Our thermofluidic simulations confirm the role of gravity-induced thermal convective flow, which dissipates heat from the substrate surface and thus influences bubble nucleation. In microgravity, the influence of thermal convective flow diminishes, resulting in localized heat at the substrate surface, which leads to faster temperature rise. This unique condition enables quicker bubble nucleation and growth. Moreover, we highlight the influence of surface microstructure geometries on bubble nucleation. Acting as heat-transfer fins, the geometries of the microstructures influence heat transfer from the substrate to the water. Finer microstructures, which have larger specific surface areas, enhance surface-to-liquid heat transfer and thus reduce the rate of surface temperature rise, leading to slower bubble nucleation. Our experimental and simulation results provide insights into thermal bubble dynamics in microgravity, which may help design thermal management solutions and develop bubble-based sensing technologies.
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Machine learning (ML) provides temporal advantage and performance improvement in practical electronic device design by adaptive learning. Herein, Bayesian optimization (BO) is successfully applied to the design of optimal dual-layer oxide semiconductor thin film transistors (OS TFTs). This approach effectively manages the complex correlation and interdependency between two oxide semiconductor layers, resulting in the efficient design of experiment (DoE) and reducing the trial-and-error. Considering field effect mobility (ð) and threshold voltage (Vth ) simultaneously, the dual-layer structure designed by the BO model allows to produce OS TFTs with remarkable electrical performance while significantly saving an amount of experimental trial (only 15 data sets are required). The optimized dual-layer OS TFTs achieve the enhanced field effect mobility of 36.1 cm2 V-1 s-1 and show good stability under bias stress with negligible difference in its threshold voltage compared to conventional IGZO TFTs. Moreover, the BO algorithm is successfully customized to the individual preferences by applying the weight factors assigned to both field effect mobility (ð) and threshold voltage (Vth ).
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Optical manipulation of nanoparticles (NPs) in liquid has garnered increasing interest for various applications, ranging from biological systems to nanofabrication. A plane wave as an optical source has recently been shown to be capable of pushing or pulling an NP when the NP is encapsulated by a nanobubble (NB) in water. However, the lack of an accurate model to describe the optical force on NP-in-NB systems hinders a comprehensive understanding of NP motion mechanisms. In this study, we present an analytical model using vector spherical harmonics to accurately capture the optical force and the resultant trajectory of an NP in an NB. We test the developed model using a solid Au NP as an example. By visualizing the vector field line of the optical force, we reveal the possible moving paths of the NP in the NB. This study can provide valuable insights for designing experiments to manipulate supercaviting NPs using plane waves.
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The advent of nanophotonics enables the regulation of thermal emission in the momentum domain as well as in the frequency domain. However, earlier attempts to steer thermal emission in a certain direction were restricted to a narrow spectrum or specific polarization, and thus their average (8-14 µm) emissivity (εav) and angular selectivity were nominal. Therefore, the practical uses of directional thermal emitters have remained unclarified. Here, we report broadband, polarization-irrelevant, amplified directional thermal emission from hollow microcavities covered with deep-subwavelength-thickness oxide shells. A hexagonal array of SiO2/AlOX (100/100 nm) hollow microcavities designed by Bayesian optimization exhibited εav values of 0.51-0.62 at 60°-75° and 0.29-0.32 at 5°-20°, yielding a parabolic antenna-shaped distribution. The angular selectivity peaked at 8, 9.1, 10.9, and 12 µm, which were identified as the epsilon-near-zero (via Berreman modes) and maximum-negative-permittivity (via photon-tunneling modes) wavelengths of SiO2 and AlOX, respectively, thus supporting phonon-polariton resonance mediated broadband side emission. As proof-of-concept experiments, we demonstrated that these exceptional epsilon-based microcavities could provide thermal comfort to users and practical cooling performance to optoelectronic devices.
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Interfaces impede heat flow in micro/nanostructured systems. Conventional theories for interfacial thermal transport were derived based on bulk phonon properties of the materials making up the interface without explicitly considering the atomistic interfacial details, which are found critical to correctly describing thermal boundary conductance. Recent theoretical studies predicted the existence of localized phonon modes at the interface which can play an important role in understanding interfacial thermal transport. However, experimental validation is still lacking. Through a combination of Raman spectroscopy and high-energy-resolution electron energy-loss spectroscopy in a scanning transmission electron microscope, we report the experimental observation of localized interfacial phonon modes at ~12 THz at a high-quality epitaxial Si-Ge interface. These modes are further confirmed using molecular dynamics simulations with a high-fidelity neural network interatomic potential, which also yield thermal boundary conductance agreeing well with that measured in time-domain thermoreflectance experiments. Simulations find that the interfacial phonon modes have an obvious contribution to the total thermal boundary conductance. Our findings significantly contribute to the understanding of interfacial thermal transport physics and have impact on engineering thermal boundary conductance at interfaces in applications such as electronics thermal management and thermoelectric energy conversion.
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We show that the Brownian motion of a nanoparticle (NP) can reach a ballistic limit when intensely heated to form supercavitation. As the NP temperature increases, its Brownian motion displays a sharp transition from normal to ballistic diffusion upon the formation of a vapor bubble to encapsulate the NP. Intense heating allows the NP to instantaneously extend the bubble boundary via evaporation, so the NP moves in a low-friction gaseous environment. We find the dynamics of the supercavitating NP is largely determined by the near field effect, i.e., highly localized vapor phase property in the vicinity of the NP.
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Photothermal surface bubbles play important roles in applications like microfluidics and biosensing, but their formation on transparent substrates immersed in a plasmonic nanoparticle (NP) suspension has an unknown origin. Here, we reveal NPs deposited on the transparent substrate by optical forces are responsible for the nucleation of such photothermal surface bubbles. We show the surface bubble formation is always preceded by the optically driven NPs moving toward and deposited to the surface. Interestingly, such optically driven motion can happen both along and against the photon stream. The laser power density thresholds to form a surface bubble drastically differ depending on if the surface is forward- or backward-facing the light propagation direction. We attributed this to different optical power densities needed to enable optical pulling and pushing of NPs in the suspension, as optical pulling requires higher light intensity to excite supercavitation around NPs to enable proper optical configuration.
Asunto(s)
Oro , Nanopartículas del Metal , Rayos Láser , LuzRESUMEN
Aluminum nitride (AlN) has garnered much attention due to its intrinsically high thermal conductivity. However, engineering thin films of AlN with these high thermal conductivities can be challenging due to vacancies and defects that can form during the synthesis. In this work, we report on the cross-plane thermal conductivity of ultra-high-purity single-crystal AlN films with different thicknesses (â¼3-22 µm) via time-domain thermoreflectance (TDTR) and steady-state thermoreflectance (SSTR) from 80 to 500 K. At room temperature, we report a thermal conductivity of â¼320 ± 42 W m-1 K-1, surpassing the values of prior measurements on AlN thin films and one of the highest cross-plane thermal conductivities of any material for films with equivalent thicknesses, surpassed only by diamond. By conducting first-principles calculations, we show that the thermal conductivity measurements on our thin films in the 250-500 K temperature range agree well with the predicted values for the bulk thermal conductivity of pure single-crystal AlN. Thus, our results demonstrate the viability of high-quality AlN films as promising candidates for the high-thermal-conductivity layers in high-power microelectronic devices. Our results also provide insight into the intrinsic thermal conductivity of thin films and the nature of phonon-boundary scattering in single-crystal epitaxially grown AlN thin films. The measured thermal conductivities in high-quality AlN thin films are found to be constant and similar to bulk AlN, regardless of the thermal penetration depth, film thickness, or laser spot size, even when these characteristic length scales are less than the mean free paths of a considerable portion of thermal phonons. Collectively, our data suggest that the intrinsic thermal conductivity of thin films with thicknesses less than the thermal phonon mean free paths is the same as bulk so long as the thermal conductivity of the film is sampled independent of the film/substrate interface.
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Understanding the growth dynamics of the microbubbles produced by plasmonic heating can benefit a wide range of applications like microfluidics, catalysis, micropatterning, and photothermal energy conversion. Usually, surface plasmonic bubbles are generated on plasmonic structures predeposited on the surface subject to laser heating. In this work, we investigate the growth dynamics of surface microbubbles generated in plasmonic nanoparticle (NP) suspension. We observe much faster bubble growth rates compared to those in pure water with surface plasmonic structures. Our analyses show that the volumetric heating effect around the surface bubble due to the existence of NPs in the suspension is the key to explaining this difference. Such volumetric heating increases the temperature around the surface bubble more efficiently compared to surface heating which enhances the expelling of dissolved gas. We also find that the bubble growth rates can be tuned in a very wide range by changing the concentration of NPs, besides laser power and dissolved gas concentration.
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Directed high-speed motion of nanoscale objects in fluids can have a wide range of applications like molecular machinery, nano robotics, and material assembly. Here, we report ballistic plasmonic Au nanoparticle (NP) swimmers with unprecedented speeds (~336,000 µm s-1) realized by not only optical pushing but also pulling forces from a single Gaussian laser beam. Both the optical pulling and high speeds are made possible by a unique NP-laser interaction. The Au NP excited by the laser at the surface plasmon resonance peak can generate a nanoscale bubble, which can encapsulate the NP (i.e., supercavitation) to create a virtually frictionless environment for it to move, like the Leidenfrost effect. Certain NP-in-bubble configurations can lead to the optical pulling of NP against the photon stream. The demonstrated ultra-fast, light-driven NP movement may benefit a wide range of nano- and bio-applications and provide new insights to the field of optical pulling force.
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Precise spatiotemporal control of surface bubble movement can benefit a wide range of applications like high-throughput drug screening, combinatorial material development, microfluidic logic, colloidal and molecular assembly, and so forth. In this work, we demonstrate that surface bubbles on a solid surface are directed by a laser to move at high speeds (>1.8 mm/s), and we elucidate the mechanism to be the depinning of the three-phase contact line (TPCL) by rapid plasmonic heating of nanoparticles (NPs) deposited in situ during bubble movement. On the basis of our observations, we deduce a stick-slip mechanism based on asymmetric fore-aft plasmonic heating: local evaporation at the front TPCL due to plasmonic heating depins and extends the front TPCL, followed by the advancement of the trailing TPCL to resume a spherical bubble shape to minimize surface energy. The continuous TPCL drying during bubble movement also enables well-defined contact line deposition of NP clusters along the moving path. Our finding is beneficial to various microfluidics and pattern writing applications.
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Water slip at solid surfaces is important for a wide range of micro-/nanofluidic applications. While it is known that water slip behavior depends on surface functionalization, how it impacts the molecular level dynamics and mass transport at the interface is still not thoroughly understood. In this paper, we use nonequilibrium molecular dynamics simulations to investigate the slip behavior of water confined between gold surfaces functionalized by self-assembled monolayer (SAM) molecules with different polar functional groups. We observe a positive-to-negative slip transition from hydrophobic to hydrophilic SAM functionalizations, which is found to be related to the stronger interfacial interaction between water molecules and more hydrophilic SAM molecules. The stronger interaction increases the surface friction and local viscosity, making water slip more difficult. More hydrophilic functionalization also slows down the interfacial water relaxation and leads to more pronounced water trapping inside the SAM layer, both of which impede water slip. The results from this work will provide useful insights into the understanding of the water slip at functionalized surfaces and design guidelines for various applications.
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Thermal transport across solid interfaces is of great importance for applications like power electronics. In this work, we perform non-equilibrium molecular dynamics simulations to study the effect of light atoms on the thermal transport across SiC/GaN interfaces, where light atoms refer to substitutional or interstitial defect atoms lighter than those in the pristine lattice. Various light atom doping features, such as the light atom concentration, mass of the light atom, and skin depth of the doped region, have been investigated. It is found that substituting Ga atoms in the GaN lattice with lighter atoms (e.g. boron atoms) with 50% concentration near the interface can increase the thermal boundary conductance (TBC) by up to 50%. If light atoms are introduced interstitially, a similar increase in TBC is observed. Spectral analysis of interfacial heat transfer reveals that the enhanced TBC can be attributed to the stronger coupling of mid- and high-frequency phonons after introducing light atoms. We have also further included quantum correction, which reduces the amount of enhancement, but it still exists. These results may provide a route to improve TBC across solid interfaces as light atoms can be introduced during material growth.
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Polymers with superior mechanical properties are desirable in many applications. In this work, polyethylene (PE) films reinforced with exfoliated thermally reduced graphene oxide (TrGO) fabricated using a roll-to-roll hot-drawing process are shown to have outstanding mechanical properties. The specific ultimate tensile strength and Young's modulus of PE/TrGO films increased monotonically with the drawing ratio and TrGO filler fraction, reaching up to 3.2 ± 0.5 and 109.3 ± 12.7 GPa, respectively, with a drawing ratio of 60× and a very low TrGO weight fraction of 1%. These values represent by far the highest reported to date for a polymer/graphene composite. Experimental characterizations indicate that as the polymer films are drawn, TrGO fillers are exfoliated, which is further confirmed by molecular dynamics (MD) simulations. Exfoliation increases the specific area of the TrGO fillers in contact with the PE matrix molecules. Molecular dynamics simulations show that the PE-TrGO interaction is stronger than the PE-PE intermolecular van der Waals interaction, which enhances load transfer from PE to TrGO and leverages the ultrahigh mechanical properties of TrGO.
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Enhancing thermal energy transport across solid interfaces is of critical importance to a wide variety of applications ranging from energy systems and lighting devices to electronics. Nanoscale surface roughness is usually considered detrimental to interfacial thermal transport because of its role in phonon scattering. In this study, however, we demonstrate significant thermal conductance enhancements across metal-semiconductor interfaces by as much as 90% higher than that of the planar interfaces using engineered nanostructures fabricated by Au nanoparticle (NP)-assisted lithography, where self-assembled Au NPs are used as an efficient etching mask to pattern solid substrates over large surface areas. The enlarged interfacial contact area due to the presence of nanostructures is the main reason for the significantly enhanced thermal transport. It is further demonstrated that the conductance can be systematically tuned over a wide range through the use of the Au NP self-assembly process that is regulated by a sacrificial Sb layer whose thickness determines the size and density of the nanostructures produced. This strategy is tested on two technologically important semiconductors, Si and GaN, and their interfacial thermal conductance with Al being measured using the time-domain thermoreflectance technique. Moreover, the nanostructured interfaces can maintain the enhanced conductance for a temperature range of 30-110 °C-the operating temperatures commonly experienced by energy, lighting, and electronic devices. Our results could provide a wafer-scale and low-cost strategy for improving the thermal management of these devices.
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Thermal transport across solid interfaces plays important roles in many applications, especially in the thermal management of modern power electronics. In this study, we use non-equilibrium MD (NEMD) simulations to systematically study a model SiC/GaN interface, which is an important interface in GaN-based power electronics, mated by different intermediate layers (ILs) with the focus on how the atomic masses of the ILs influence the overall thermal conductance. To isolate the mass effect, the Tersoff potential with the same parameters is used to approximate the interatomic interactions between all atoms, with the only differences between materials being their atomic masses. The NEMD results show that the thermal boundary conductance (TBC) of IL-mated interfaces depends not only on the total primitive cell mass of the IL but also on the relative masses of the atoms within the unit cell. By analyzing the vibrational power spectra (VPS) of SiC, IL, and GaN, it is found that the optical phonons play important roles in thermal transport across the solid/solid interfaces. There is an optimal mass ratio of the atoms in the unit cell of the IL that can maximize the overlap of IL optical phonon VPS with those of SiC and GaN. Furthermore, the atomic masses of a number of III-V semiconductor compounds are studied for the ILs. It is shown that when only considering the mass effect, in the classical limit, AlN will be the best IL to enhance thermal transport across SiC/GaN interfaces with an improvement of as much as 27% over that of a pristine SiC/GaN interface. Despite the known limitation of the model (e.g., absence of strain and quantum effects), the results from this work may still provide some useful information for the design of ILs to improve thermal transport across solid/solid interfaces.
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Oxide semiconductors thin film transistors (OS TFTs) with good transparency and electrical performance have great potential for future display technology. In particular, solution-processed OS TFTs have been attracted much attention due to many advantages such as continuous, large scale, and low cost processability. Recently, OS TFTs fabricated with a metal aqua complex have been focused because they have low temperature processability for deposition on flexible substrate as well as high field-effect mobility for application of advanced display. However, despite some remarkable results, important factors to optimize their electrical performance with reproducibility and uniformity have not yet been achieved. Here, we newly introduce the strong effects of humidity to enhance the electrical performance of OS TFTs fabricated with the metal aqua complex. Through humidity control during the spin-coating process and annealing process, we successfully demonstrate solution-processed InOx/SiO2 TFTs with a good electrical uniformity of â¼5% standard deviation, showing high average field-effect mobility of 2.76 cm2V-1s-1 and 15.28 cm2V-1s-1 fabricated at 200 and 250 °C, respectively. Also, on the basis of the systematic analyses, we demonstrate the mechanism for the change in electrical properties of InOx TFTs depending on the humidity control. Finally, on the basis of the mechanism, we extended the humidity control to the fabrication of the AlOx insulator. Subsequently, we successfully achieved humidity-controlled InOx/AlOx TFTs fabricated at 200 °C showing high average field-effect mobility of 9.5 cm2V-1s-1.