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Linear resistivity-temperature ( R - T ) at low temperatures, referred to as strange metal (SM), is an unusual characteristic observed in strongly correlated systems. SM is often mingled with superconductivity and magnetism in various materials. Here, we report a linear R - T relation in a hole-doped, degenerate spin-valley (SV) semiconductor, V 0.25 W 0.75 Se 2 , with hole pockets in the valence band. SM emerges over a wide temperature range (1.8-150 K) without any apparent superconductivity down to 110 mK. This SM behavior is suppressed at low temperatures below 20 K in the presence of a magnetic field. The ansatz R ( H , T ) - R ( 0 , 0 ) ∝ ( α k B T ) 2 + ( γ μ B μ 0 H ) 2 yields the γ/α ratio of ∼4, larger than the previous reports. The observed SM over a wide temperature range is explained by a spin-orbit coupling (SOC)-mediated SV pair with strong correlation effects, analogous to a phonon-mediated Cooper pair in superconductivity. This finding opens possible routes for understanding strange metal behavior through the interplay of strong SOC and strong Coulomb interactions.

Rashba states have been actively revisited as a platform for advanced applications such as spintronics and topological quantum computation. Yet, access to the Rashba state is restricted to the specific material sets, and the methodology to control the Rashba state is not established. Here, we report the Rashba states on the (001) surface of KZnBi, a 3D Dirac semimetal. Using angle-resolved photoemission spectroscopy and first-principles calculations, we investigated the evolution of Rashba states under different surface conditions controlled by alkali metal deposition. We observed that restoring surface ordering enables a Rashba state, which is absent in freshly cleaved surfaces. Interestingly, we were able to modify the dispersion of the Rashba state from an ordinary parabolic dispersion to a linearly dispersing Dirac-like state by additional alkali-metal deposition. Our findings provide a methodology for engineering the properties of Rashba states for advanced applications and redefine topological systems as generic hosts of Rashba states.

Prolonging hot carrier cooling, a crucial factor in optoelectronic applications, including hot carrier photovoltaics, presents a significant challenge. High-energy band-nesting excitons within parallel bands offer a promising and underexplored avenue for addressing this issue. Here, we exploit an exceptional D exciton cooling prolongation of 2 to 3 orders of magnitude compared to sub-picosecond in typical transition metal dichalcogenides (TMDs) owing to the complex Coulomb environment and the sequential and mismatch-valley relaxation. Simultaneously, the intervalley scattering upconversion of band-edge excitons with the slow D exciton formation in the metastable Γ valley/hill also reduces the cooling rate. We successfully extract D and C excitons as hot carriers through integrating with various thicknesses of TiO x , achieving the highest efficiency of 98% and 85% at a Ti thickness of 2 nm. Our findings highlight the potential of band-nesting excitons for extending hot carrier cooling time, paving the way for advancements in hot carrier-based optoelectronic devices.

Two-dimensional trigonal tellurium (2D Te), a narrow-bandgap semiconductor with a bandgap of approximately 0.3 eV, hosts Weyl points near the band edge and exhibits a narrow, strong Berry curvature dipole (BCD). By applying a back-gate bias to align the Fermi level with the BCD, a sharp increase in the dissipationless transverse nonlinear Hall response is observed in 2D Te. Gate modulation of the BCD demonstrates an on/off ratio of 10 4 and a responsivity of nearly 10 6 V/W, while the longitudinal current induced by band modulation reaches an on/off ratio of about 10. This current is sustained up to 200 K, exhibiting a change of 3 orders of magnitude. The inclusion of both transistor action and rectification enhances the temperature sensitivity of the dissipationless Hall current, offering potential applications in electrothermal detectors and sensors and highlighting the significance of topological properties in advancing electronic applications.

Recently, 2D semiconductor-based optoelectronic memory has been explored to overcome the limitations of conventional von Neumann architectures by integrating optical sensing and data storage into one device. Persistent photocurrent (PPC), essential for optoelectronic memory, originates from charge carrier trapping according to the Shockley-Read-Hall (SRH) model in 2D semiconductors. The quasi-Fermi level position influences the activation of charge-trapping sites. However, the correlation between quasi-Fermi level modulations and PPC in 2D semiconductors has not been extensively studied. In this study, we demonstrate optoelectronic memory based on a 2D semiconductor-polymer hybrid structure and confirm that the underlying mechanism is charge trapping, as the SRH model explains. Under light illumination, electrons transfer from polyvinylpyrrolidone to p-type tungsten diselenide, resulting in high-level injection and majority carrier-type transitions. The quasi-Fermi level shifts upward with increasing temperature, improving PPC and enabling optoelectronic memory at 433 K. Our findings offer valuable insights into optimizing 2D semiconductor-based optoelectronic memory.

Heterostructures (HSs) formed by the transition-metal dichalcogenide materials have shown great promise in next-generation (opto)electronic applications. An artificially twisted HS allows us to manipulate the optical and electronic properties. In this work, we introduce the understanding of the energy transfer (ET) process governed by the dipolar interaction in a twisted molybdenum diselenide (MoSe 2 ) homobilayer without any charge-blocking interlayer. We fabricated an unconventional homobilayer (i.e., HS) with a large twist angle (∼57°) by combining the chemical vapor deposition (CVD) and mechanical exfoliation (Exf.) techniques to fully exploit the lattice parameter mismatch and indirect/direct (CVD/Exf.) bandgap nature. These effectively weaken the interlayer charge transfer and allow the ET to control the carrier recombination channels. Our experimental and theoretical results explain a massive HS photoluminescence enhancement due to an efficient ET process. This work shows that the electronically decoupled MoSe 2 homobilayer is coupled by the ET process, mimicking a "true" heterobilayer nature.

The rapid increase in data storage worldwide demands a substantial amount of energy consumption annually. Studies looking at low power consumption accompanied by high-performance memory are essential for next-generation memory. Here, Graphdiyne oxide (GDYO), characterized by facile resistive switching behavior, is systematically reported toward a low switching voltage memristor. The intrinsic large, homogeneous pore-size structure in GDYO facilitates ion diffusion processes, effectively suppressing the operating voltage. The theoretical approach highlights the remarkably low diffusion energy of the Ag ion (0.11 eV) and oxygen functional group (0.6 eV) within three layers of GDYO. The Ag/GDYO/Au memristor exhibits an ultralow operating voltage of 0.25 V with a GDYO thickness of 5 nm; meanwhile, the thicker GDYO of 29 nm presents multilevel memory with an ON/OFF ratio of up to 10 4 . The findings shed light on memory resistive switching behavior, facilitating future improvements in GDYO-based devices toward opto-memristors, artificial synapses, and neuromorphic applications.

Magnetic anisotropy in atomically thin correlated heterostructures is essential for exploring quantum magnetic phases for next-generation spintronics. Whereas previous studies have mostly focused on van der Waals systems, here we investigate the impact of dimensionality of epitaxially grown correlated oxides down to the monolayer limit on structural, magnetic, and orbital anisotropies. By designing oxide superlattices with a correlated ferromagnetic SrRuO 3 and nonmagnetic SrTiO 3 layers, we observed modulated ferromagnetic behavior with the change of the SrRuO 3 thickness. Especially, for three-unit-cell-thick layers, we observe a significant 1500% improvement of the coercive field in the anomalous Hall effect, which cannot be solely attributed to the dimensional crossover in ferromagnetism. The atomic-scale heterostructures further reveal the systematic modulation of anisotropy for the lattice structure and orbital hybridization, explaining the enhanced magnetic anisotropy. Our findings provide valuable insights into engineering the anisotropic hybridization of synthetic magnetic crystals, offering a tunable spin order for various applications.

All-solid-state lithium-sulfur batteries (ASSLSBs) are promising next-generation battery technologies with a high energy density and excellent safety. Because of the insulating nature of sulfur/Li 2 S, conventional cathode designs focus on developing porous hosts with high electronic conductivities such as porous carbon. However, carbon hosts boost the decomposition of sulfide electrolytes and suffer from sulfur detachment due to their weak bonding with sulfur/Li 2 S, resulting in capacity decays. Herein, we propose a counterintuitive design concept of host materials in which nonconductive polar mesoporous hosts can enhance the cycling life of ASSLSBs through mitigating the decomposition of adjacent electrolytes and bonding sulfur/Li 2 S steadily to avoid detachment. By using a mesoporous SiO 2 host filled with 70 wt % sulfur as the cathode, we demonstrate steady cycling in ASSLSBs with a capacity reversibility of 95.1% in the initial cycle and a discharge capacity of 1446 mAh/g after 500 cycles at C/5 based on the mass of sulfur.

Quantum dots (QDs) have garnered a significant amount of attention as promising memristive materials owing to their size-dependent tunable bandgap, structural stability, and high level of applicability for neuromorphic computing. Despite these advantageous properties, the development of QD-based memristors has been hindered by challenges in understanding and adjusting the resistive switching (RS) behavior of QDs. Herein, we propose three types of InP/ZnSe/ZnS QD-based memristors to elucidate the RS mechanism, employing a thin poly(methyl methacrylate) layer. This approach not only allows us to identify which carriers (electron or hole) are trapped within the QD layer but also successfully demonstrates QD-based synaptic devices. Furthermore, to utilize the QD memristor as a synapse, long-term potentiation/depression (LTP/LTD) characteristics are measured, resulting in a low nonlinearity of LTP/LTD at 0.1/1. On the basis of the LTP/LTD characteristics, single-layer perceptron simulations were performed using the Extended Modified National Institute of Standards and Technology, verifying a maximum recognition rate of 91.46%.

The demand for high-speed and low-loss interconnects in modern computer architectures is difficult to satisfy by using traditional Si-based electronics. Although optical interconnects offer a promising solution owing to their high bandwidth, low energy dissipation, and high-speed processing, integrating elements such as a light source, detector, and modulator, comprising different materials with optical waveguides, presents many challenges in an integrated platform. Two-dimensional (2D) van der Waals (vdW) semiconductors have attracted considerable attention in vertically stackable optoelectronics and advanced flexible photonics. In this study, optoelectronic components for exciton-based photonic circuits are demonstrated by integrating lithographically patterned poly(methyl methacrylate) (PMMA) waveguides on 2D vdW devices. The excitonic signals generated from the 2D materials by using laser excitation were transmitted through patterned PMMA waveguides. By introducing an external electric field and combining vdW heterostructures, an excitonic switch, phototransistor, and guided-light photovoltaic device on SiO 2 /Si substrates were demonstrated.

Formation of charged trions is detrimental to the luminescence quantum efficiency of colloidal quantum dot (QD) thin films as they predominantly undergo nonradiative recombination. In this regard, control of charged trion formation is of interest for both fundamental characterization of the quasi-particles and performance optimization. Using CdSe/CdS QDs as a prototypical material system, here we demonstrate a metal-oxide-semiconductor capacitor based on QD thin films for studying the background charge effect on the luminescence efficiency and lifetime. The concentration ratio of the charged and neutral quasiparticles in the QDs is reversibly controlled by applying a gate voltage, while simultaneous steady-state and time-resolved photoluminescence measurements are performed. Notably, the photoluminescence intensity is modulated by up to 2 orders of magnitude with a corresponding change in the effective lifetime. In addition, chip-scale modulation of brightness is demonstrated, where the photoluminescence is effectively turned on and off by the gate, highlighting potential applications in voltage-controlled electrochromics.

Transition metal dichalcogenides (TMDs) benefit electrical devices with spin-orbit coupling and valley- and topology-related properties. However, TMD-based devices suffer from traps arising from defect sites inside the channel and the gate oxide interface. Deactivating them requires independent treatments, because the origins are dissimilar. This study introduces a single treatment to passivate defects in a multilayer MoS 2 FET. By applying back-gate bias, protons from an H-TFSI droplet are injected into the MoS 2 , penetrating deeply enough to reach the SiO 2 gate oxide. The characterizations employing low-temperature transport and deep-level transient spectroscopy (DLTS) studies reveal that the trap density of S vacancies in MoS 2 drops to the lowest detection level. The temperature-dependent mobility plot on the SiO 2 substrate resembles that of the h-BN substrate, implying that dangling bonds in SiO 2 are passivated. The carrier mobility on the SiO 2 substrate is enhanced by approximately 2200% after the injection.

The composition of the solid electrolyte interphase (SEI) plays an important role in controlling Li-electrolyte reactions, but the underlying cause of SEI composition differences between electrolytes remains unclear. Many studies correlate SEI composition with the bulk solvation of Li ions in the electrolyte, but this correlation does not fully capture the interfacial phenomenon of SEI formation. Here, we provide a direct connection between SEI composition and Li-ion solvation by forming SEIs using polar substrates that modify interfacial solvation structures. We circumvent the deposition of Li metal by forming the SEI above Li + /Li redox potential. Using theory, we show that an increase in the probability density of anions near a polar substrate increases anion incorporation within the SEI, providing a direct correlation between interfacial solvation and SEI composition. Finally, we use this concept to form stable anion-rich SEIs, resulting in high performance lithium metal batteries.

Lithium-sulfur (Li-S) batteries are promising candidates for next-generation energy storage systems due to their high theoretical energy density and the low cost of sulfur. However, slow conversion kinetics between the insulating S and lithium sulfide (Li 2 S) remains as a technical challenge. In this work, we report a catalyst featuring nickel (Ni) single atoms and clusters anchored to a porous hydrogen-substituted graphdiyne support (termed Ni@HGDY), which is incorporated in Li 2 S cathodes. The rapidly synthesized catalyst was found to enhance ionic and electronic conductivity, decrease the reaction overpotential, and promote more complete conversion between Li 2 S and sulfur. The addition of Ni@HGDY to commercial Li 2 S powder enabled a capacity of over 516 mAh g Li 2 S -1 at 1 C for over 125 cycles, whereas the control Li 2 . These findings highlight the efficacy of Ni as a metal catalyst and demonstrate the promise of HGDY in energy storage devices.Li 2 S -1 . These findings highlight the efficacy of Ni as a metal catalyst and demonstrate the promise of HGDY in energy storage devices.

As the electron mobility of two-dimensional (2D) materials is dependent on an insulating substrate, the nonuniform surface charge and morphology of silicon dioxide (SiO 2 ) layers degrade the electron mobility of 2D materials. Here, we demonstrate that an atomically thin single-crystal insulating layer of silicon oxynitride (SiON) can be grown epitaxially on a SiC wafer at a wafer scale and find that the electron mobility of graphene field-effect transistors on the SiON layer is 1.5 times higher than that of graphene field-effect transistors on typical SiO 2 films. Microscale and nanoscale void defects caused by heterostructure growth were eliminated for the wafer-scale growth of the single-crystal SiON layer. The single-crystal SiON layer can be grown on a SiC wafer with a single thermal process. This simple fabrication process, compatible with commercial semiconductor fabrication processes, makes the layer an excellent replacement for the SiO 2 /Si wafer.

High-quality InP-based quantum dots (QDs) have become very promising, environmentally benign light emitters for display applications, but their synthesis generally entails hazardous hydrofluoric acid. Here, we present a highly facile route to InP/ZnSe/ZnS core/shell/shell QDs with a near-unity photoluminescence quantum yield. As the key additive, the inorganic salt ZnF 2 mildly reacts with carboxylic acid at a high temperature and in situ generates HF, which eliminates surface oxide impurities, thus facilitating epitaxial shell growth. The resulting InP/ZnSe/ZnS QDs exhibit a narrower emission line width and better thermal stability in comparison with QDs synthesized with hydrofluoric acid. Light-emitting diodes using large-sized InP/ZnSe/ZnS QDs without replacing original ligands achieve the highest peak external quantum efficiency of 22.2%, to the best of our knowledge, along with a maximum brightness of >110 000 cd/m 2 and a T lifetime of >32 000 h at 100 cd/m 95 . This safe approach is anticipated to be applied for a wide range of III-V QDs.2 . This safe approach is anticipated to be applied for a wide range of III-V QDs.

Bioinspired yarn/fiber structured hydro-actuators have recently attracted significant attention. However, most water-driven mechanical actuators are unsatisfactory because of the slow recovery process and low full-time power density. A rapidly recoverable high-power hydro-actuator is reported by designing biomimetic carbon nanotube (CNT) yarns. The hydrophilic CNT (HCNT) coiled yarn was prepared by storing pre-twist into CNT sheets and subsequent electrochemical oxidation (ECO) treatment. The resulting yarn demonstrated structural stability even when one end was cut off without the possible loss of pre-stored twists. The HCNT coiled yarn actuators provided maximal contractile work of 863 J/kg at 11.8 MPa stress when driven by water. Moreover, the recovery time of electrically heated yarns at a direct current voltage of 5 V was 95% shorter than that of neat yarns without electric heating. Finally, the electrothermally recoverable hydro-actuators showed a high actuation frequency (0.17 Hz) and full-time power density (143.8 W/kg).

Despite the enormous applications of and fundamental scientific interest in amorphous hollow-silica nanostructures ( h- SiNS s with controllable surface curvatures (concave, convex, or angular), symmetries (spherical, polygonal, or Janus), and interior architectures (open or closed walls) by the addition of a metal salt and implementing kinetic handles of silica precursor (silanes/ammonia) concentrations and reverse-micellar volume. During the silica growth, we identified the key role of transiently h- SiNS s with controllable surface curvatures (concave, convex, or angular), symmetries (spherical, polygonal, or Janus), and interior architectures (open or closed walls) by the addition of a metal salt and implementing kinetic handles of silica precursor (silanes/ammonia) concentrations and reverse-micellar volume. During the silica growth, we identified the key role of transiently in situ crystallized metal coordination complexes as a nanopolyhedral "ghost template", which provides facet-selective interactions with amino-silica monomers and guides the differential silica growth that produces different h- SiNS s. Additionally, crystal-like well-defined polygonal h- SiNS s with flat surfaces, assembled as highly ordered close-packed octahedral mesoscale materials (ca. 3 μm) where h- SiNS s with different nanoarchitectures act as building units (ca. 150 nm) to construct customizable cavities and nanospaces, differ from conventionally assembled materials.

We investigated the role of graphene interfaces in strengthening and toughening of the Cu-graphene nanocomposite by a combination of in situ transmission electron microscopy (TEM) deformation and molecular dynamics (MD) simulations. In situ TEM directly showed that dislocation plasticity is strongly confined within single Cu grains by the graphene interfaces and grain boundaries. The weak Cu-graphene interfacial bonding induces stress decoupling, which results in independent plastic deformation of each Cu layer. As confirmed by the MD simulation, the localized deformation made by such constrained dislocation plasticity results in the nucleation and growth of voids at the graphene interface, which acts as a precursor for crack. The graphene interfaces also effectively block crack propagation promoted by easy delamination of Cu layers dissipating the elastic strain energy. The toughening mechanisms revealed by the present study will provide valuable insights into the optimization of the mechanical properties of metal-graphene nanolayered composites.

Sharks, marine creatures that swim fast and have an antifouling ability, possess dermal denticle structures of micrometer-size. Because the riblet geometries on the denticles reduce the shear stress by inducing the slip of fluid parallel to the stream-wise direction, shark skin has the distinguished features of low drag and antifouling. Although much attention has been given to low-drag surfaces inspired from shark skin, it remains an important challenge to accurately mimic denticle structures in the micrometer scale and to finely control their structural features. This paper presents a novel method to create shark skin-mimetic denticle structures for low drag by exploiting a photoreconfigurable azopolymer. The light-designed denticle structure exhibits superior hydrophobicity and an antifouling effect as sharks do. This work suggests that our novel photoreconfiguration technology, mimicking shark skin and systematically manipulating various structural parameters, can be used in a reliable manner for diverse applications requiring low-drag surfaces.

In heterogeneous catalysts, metal-oxide interactions occur spontaneously but often in an undesired way leading to the oxidation of metal nanoparticles. Manipulating such interactions to produce highly active surface of metal nanoparticles can warrant the optimal catalytic activity but has not been established to date. Here we report that a prior reduced TiO 2 support can reverse the interaction with Pt nanoparticles and augment the metallic state of Pt, exhibiting a 3-fold increase in hydrogen production rate compared to that of conventional Pt/TiO 2 . Spatially resolved electron energy loss spectroscopy of the Ti valence state and the electron density distribution within Pt nanoparticles provide direct evidence supporting that the Pt/TiO 2 /H 2 O triple junctions are the most active catalytic sites for water reduction. Our reverse metal-oxide interaction scheme provides a breakthrough in the stagnated hydrogen production efficiency and can be applied to other heterogeneous catalyst systems composed of metal nanoparticles with reducible oxide supports.

Although van der Waals-layered transition metal dichalcogenides from transient absorption spectroscopy have successfully demonstrated an ideal carrier multiplication (CM) performance with an onset of nearly 2E g , interpretation of the CM effect from the optical approach remains unresolved owing to the complexity of many-body electron-hole pairs. We demonstrate the escalated photocurrent with excitation photon energy by fabricating the dual-gate p-n junction of a MoTe 2 film on a transparent substrate. Electrons and holes were efficiently extracted by eliminating the Schottky barriers in the metal contact and minimizing multiple reflections. The photocurrent was elevated proportionately to the excitation photon energy. The boosted quantum efficiency confirms the multiple electron-hole pair generation of >2E g , consistent with CM results from an optical approach, pushing the solar cell efficiency beyond the Shockley-Queisser limit.

The extreme elastic strain of monolayer transition metal dichalcogenides provides an ideal platform to achieve efficient exciton funneling via local strain modulation; however, studies conducted thus far have focused on the use of substrates with fixed strain profiles. We prepared 1L-WS 2 on a flexible substrate such that the formation of topographic wrinkles could be switched on or off, and the depth or the direction of the wrinkle could be modified by external strain, thereby providing full control of the periodic undulation of the band gap profile of 1L-WS 2 in the range 0-57 meV. Nanoscale photoluminescence (PL) imaging unambiguously evinced that the photoexcited excitons of 1L-WS 2 were accumulated at the top regions of the wrinkles with less band gap than the valley region. Our results of broad tunability of the two-dimensional (2D) exciton funneling suggest a promising route to control exciton drift for enhanced optoelectronic performances and future 2D exciton devices.

Colloidal quantum dots (QDs) exhibit unique characteristics such as facile color tunability, pure color emission with extremely narrow bandwidths, high luminescence efficiency, and high photostability. In addition, quantum dot light-emitting diodes (QLEDs) feature bright electroluminescence, low turn-on voltage, and ultrathin form factor, making them a promising candidate for next-generation displays. To achieve the overarching goal of the full-color display based on the electroluminescence of QDs, however it is essential to enhance the performance of QLEDs further for each color (e.g., red, green, and blue; RGB) and develop novel techniques for patterning RGB QD pixels without cross-contamination. Here, we present state-of-the-art material, process, and device technologies for full-color QLED-based displays. First, we highlight recent advances in the development of efficient red-, green-, and blue-monochromatic QLEDs. In particular, we focus on the progress of heavy-metal-free QLEDs. Then, we describe patterning techniques for individual RGB QDs to fabricate pixelated displays. Finally, we briefly summarize applications of such QLEDs, presenting the possibility of full-color QLED-based displays.

Visualizing the oxygen vacancy distributions is highly desirable for understanding the atomistic oxygen diffusion mechanisms in perovskites. In particular, the direct observation of the one-dimensional oxygen vacancy channels has not yet been achieved in perovskites with dual ion (i.e., cation and anion) ordering. Here, we perform atomic-resolution imaging of the one-dimensional oxygen vacancy channels and their structural dynamics in a NdBaCo 2 O 5.5 double perovskite oxide. An in situ heating transmission electron microscopy investigation reveals the disordering of oxygen vacancy channels by local rearrangement of oxygen vacancies at the specific temperature. A density functional theory calculation suggests that the possible pathway of oxygen vacancy migration is a multistep route via Co-O and Nd-O v (oxygen vacancy) sites. These findings could provide robust guidance for understanding the static and dynamic behaviors of oxygen vacancies in perovskite oxides.

Grain boundaries (GBs) are ubiquitous in solids and have been of central importance in understanding the nature of polycrystals. In addition to their classical roles, topological insulators (TIs) offer a chance to realize GBs hosting distinct topological states that can be controlled by their crystal symmetries. However, such roles of crystalline symmetry in two-dimensional (2D) TIs have not been definitively measured yet. Here, we present the first direct evidence of a symmetry-enforced metallic state along a GB in 1T'-MoTe 2 , a prototypical 2D TI. Using scanning tunneling microscopy, we show a metallic state along a GB with nonsymmorphic lattice symmetry and its absence along another boundary with symmorphic symmetry. Our atomistic simulations demonstrate in-gap Weyl semimetallic states for the former, whereas they demonstrate gapped states for the latter, explaining our observation well. The observed metallic state, tightly linked to its crystal symmetry, can be used to create a stable conducting nanowire inside TIs.

We study the electronic and optoelectronic properties of a broken-gap heterojunction composed of SnSe 2 and MoTe 2 with gate-controlled junction modes. Owing to the interband tunneling current, our device can act as an Esaki diode and a backward diode with a peak-to-valley current ratio approaching 5.7 at room temperature. Furthermore, under an 811 nm laser irradiation the heterostructure exhibits a photodetectivity of up to 7.5 × 10 12 Jones. In addition, to harness the electrostatic gate bias, V can be tuned from negative to positive by switching from the accumulation mode to the depletion mode of the heterojunction. Additionally, a photovoltaic effect with a fill factor exceeding 41% was observed, which highlights the significant potential for optoelectronic applications. This study not only demonstrates high-performance multifunctional optoelectronics based on the SnSe oc can be tuned from negative to positive by switching from the accumulation mode to the depletion mode of the heterojunction. Additionally, a photovoltaic effect with a fill factor exceeding 41% was observed, which highlights the significant potential for optoelectronic applications. This study not only demonstrates high-performance multifunctional optoelectronics based on the SnSe 2 heterostructure but also provides a comprehensive understanding of broken-band alignment and its applications.2 heterostructure but also provides a comprehensive understanding of broken-band alignment and its applications.

Although organic-inorganic halide perovskite (OIHP)-based photovoltaics have high photoconversion efficiency (PCE), their poor humidity stability prevents commercialization. To overcome this critical hurdle, focusing on the grain boundary (GB) of OIHPs, which is the main humidity penetration channel, is crucial. Herein, pressure-induced crystallization of OIHP films prepared with controlled mold geometries is demonstrated as a GB-healing technique to obtain high moisture stability. When exposed to 85% RH at 30 °C, OIHP films fabricated by pressure-induced crystallization have enhanced moisture stability due to the enlarged OIHP grain size and low-angle GBs. The crystallographic and optical properties indicate the effect of applying pressure onto OIHP films in terms of moisture stability. The photovoltaic devices with pressure-induced crystallization exhibited dramatically stabilized performance and sustained over 0.95 normalized PCE after 200 h at 40% RH and 30 °C.

A fundamental understanding of hot electron transport is critical for developing efficient hot-carrier-based solar cells. There have been significant efforts to enhance hot electron flux, and it has been found that a key factor affecting the hot electron flux is the lifetime of the hot electrons. Here, we report a combined study of hot electron flux and the lifetime of hot carriers using a perovskite-modified plasmonic nanodiode. We found that perovskite deposition on a plasmonic nanodiode can considerably improve hot electron generation induced by photon absorption. The perovskite plasmonic nanodiode consists of MAPbI 3 layers covering a plasmonic-Au/TiO 2 Schottky junction that is composed of randomly connected Au nanoislands deposited on a TiO 2 layer. The measured incident photon-to-electron conversion efficiency and the short-circuit photocurrent show a significantly improved solar-to-electrical conversion performance of this nanodiode. Such an improvement is ascribed to the improved hot electron flux in MAPbI 3 caused by effective light absorption from near-field enhancement of plasmonic Au and the efficient capture of hot electrons from Au nanoislands via the formation of a three-dimensional Schottky interface. The relation between the lifetime and flux of hot electrons was confirmed by femtosecond transient absorption spectroscopy that showed considerably longer hot electron lifetimes in MAPbI 3 combined with the plasmonic Au structure. These findings can provide a fundamental understanding of hot electron generation and transport in perovskite, which can provide helpful guidance to designing efficient hot carrier photovoltaics.

The real-time selective detection of disease-related markers in blood using biosensors has great potential for use in the early diagnosis of diseases and infections. However, this potential has not been realized thus far due to difficulties in interfacing the sensor with blood and achieving transparent circuits that are essential for detecting of target markers (e.g., protein, ions, etc.) in a complex blood environment. Herein, we demonstrate the real-time detection of a specific protein and ion in blood without a skin incision. Complementary metal-oxide-semiconductor technology was used to fabricate silicon micropillar array (SiMPA) electrodes with a height greater than 600 μm, and the surface of the SiMPA electrodes was functionalized with a self-assembling artificial peptide (SAP) as a receptor for target markers in blood, i.e., cholera toxin (CTX) and mercury(II) ions (Hg). The detection of CTX was investigated in both in vitro (phosphate-buffered saline and human blood serum, HBO model) and in vivo (mouse model) modes via impedance analysis. In the in vivo mode, the SiMPA pierces the skin, comes into contact with the blood system, and creates comprehensive circuits that include all the elements such as electrodes, blood, and receptors. The SiMPA achieves electrically transparent circuits and, thus, can selectively detect CTX in the blood in real time with a high sensitivity of 50 pM and 5 nM in the in vitro and in vivo modes, respectively. Mercury(II) ions can also be detected in both the in vitro and the in vivo modes by changing the SAP. The results illustrate that a robust sensor that can detect a variety of molecular species in the blood system in real time that will be helpful for the early diagnosis of disease and infections.

The quantum confinement of charge carriers has been a promising approach to enhance the efficiency of thermoelectric devices, by lowering the dimension of materials and raising the boundary phonon scattering rate. The role of quantum confinement in thermoelectric efficiency has been investigated by using macroscopic device-scale measurements based on diffusive electron transport with the thermal de Broglie wavelength of the electrons. Here, we report a new class of thermoelectric operation originating from quasi-bound state electrons in low-dimensional materials. Coherent thermoelectric power from confined charges was observed at room temperature in graphene quantum dots with diameters of several nanometers. The graphene quantum dots, electrostatically defined as circular n-p-n junctions to isolate charges in the p-type graphene quantum dots, enabled thermoelectric microscopy at the atomic scale, revealing weakly localized and coherent thermoelectric power generation. The conceptual thermoelectric operation provides new insights, selectively enhancing coherent thermoelectric power via resonant states of charge carriers in low-dimensional materials.

Chemical treatment using bis(trifluoromethane) sulfonimide (TFSI) was shown to be particularly effective for increasing the photoluminescence (PL) of monolayer (1L) MoS 2 , suggesting a convenient method for overcoming the intrinsically low quantum yield of this material. However, the underlying atomic mechanism of the PL enhancement has remained elusive. Here, we report the microscopic origin of the defect healing observed in TFSI-treated 1L-MoS 2 through a correlative combination of optical characterization and atomic-scale scanning transmission electron microscopy, which showed that most of the sulfur vacancies were directly repaired by the extrinsic sulfur atoms produced from the dissociation of TFSI, concurrently resulting in a significant PL enhancement. Density functional theory calculations confirmed that the reactive sulfur dioxide molecules that dissociated from TFSI can be reduced to sulfur and oxygen gas at the vacancy site to form strongly bound S-Mo. Our results reveal how defect-mediated nonradiative recombination can be effectively eliminated by a simple chemical treatment method, thereby advancing the practical applications of monolayer semiconductors.

Molecular conformation, intermolecular interaction, and electrode-molecule contacts greatly affect charge transport in molecular junctions and interfacial properties of organic devices by controlling the molecular orbital alignment. Here, we statistically investigated the charge transport in molecular junctions containing self-assembled oligophenylene molecules sandwiched between an Au probe tip and graphene according to various tip-loading forces ( F L ) that can control the molecular-tilt configuration and the van der Waals (vdW) interactions. In particular, the molecular junctions exhibited two distinct transport regimes according to the F L dependence (i.e., F L -dependent and F L -independent tunneling regimes). In addition, the charge-injection tunneling barriers at the junction interfaces are differently changed when the F L ≤ 20 nN. These features are associated to the correlation effects between the asymmetry-coupling factor (η), the molecular-tilt angle (θ), and the repulsive intermolecular vdW force ( F vdW ) on the molecular-tunneling barriers. A more-comprehensive understanding of these charge transport properties was thoroughly developed based on the density functional theory calculations in consideration of the molecular-tilt configuration and the repulsive vdW force between molecules.

Despite a longstanding controversy surrounding TiO 2 materials, TiO 2 polymorphs with heterojunctions composed of anatase and rutile outperform individual polymorphs because of the type-II energetic band alignment at the heterojunction interface. Improvement in photocatalysis has also been achieved via black TiO 2 with a thin disorder layer surrounding ordered TiO 2 . However, localization of this disorder layer in a conventional single TiO 2 nanoparticle with the heterojunction composed of anatase and rutile has remained a big challenge. Here, we report the selective positioning of a disorder layer of controlled thicknesses between the anatase and rutile phases by a conceptually different synthetic route to access highly efficient novel metal-free photocatalysis for H 2 production. The presence of a localized disorder layer within a single TiO 2 nanoparticle was confirmed for the first time by high-resolution transmission electron microscopy with electron energy-loss spectroscopy and inline electron holography. Multiple heterojunctions in single TiO 2 nanoparticles composed of crystalline anatase/disordered rutile/ordered rutile layers give the nanoparticles superior electron/hole separation efficiency and novel metal-free surface reactivity, which concomitantly yields an H 2 production rate that is ∼11-times higher than that of Pt-decorated conventional anatase and rutile single heterojunction TiO 2 systems.

Synaptic computation, which is vital for information processing and decision making in neural networks, has remained technically challenging to be demonstrated without using numerous transistors and capacitors, though significant efforts have been made to emulate the biological synaptic transmission such as short-term and long-term plasticity and memory. Here, we report synaptic computation based on Joule heating and versatile doping induced metal-insulator transition in a scalable monolayer-molybdenum disulfide (MoS 2 ) device with a biologically comparable energy consumption (∼10 fJ). A circuit with our tunable excitatory and inhibitory synaptic devices demonstrates a key function for realizing the most precise temporal computation in the human brain, sound localization: detecting an interaural time difference by suppressing sound intensity- or frequency-dependent synaptic connectivity. This Letter opens a way to implement synaptic computing in neuromorphic applications, overcoming the limitation of scalability and power consumption in conventional CMOS-based neuromorphic devices.

Monolayer (1L) transition metal dichalcogenides (TMDCs) are promising materials for nanoscale optoelectronic devices because of their direct band gap and wide absorption range (ultraviolet to infrared). However, 1L-TMDCs cannot be easily utilized for practical optoelectronic device applications (e.g., photodetectors, solar cells, and light-emitting diodes) because of their extremely low optical quantum yields (QYs). In this investigation, a high-gain 1L-MoS 2 photodetector was successfully realized, based on the surface plasmon (SP) of the Ag nanowire (NW) network. Through systematic optical characterization of the hybrid structure consisting of a 1L-MoS 2 and the Ag NW network, it was determined that a strong SP and strain relaxation effect influenced a greatly enhanced optical QY. The photoluminescence (PL) emission was drastically increased by a factor of 560, and the main peak was shifted to the neutral exciton of 1L-MoS 2 . Consequently, the overall photocurrent of the hybrid 1L-MoS 2 photodetector was observed to be 250 times better than that of the pristine 1L-MoS 2 photodetector. In addition, the photoresponsivity and photodetectivity of the hybrid photodetector were effectively improved by a factor of ∼1000. This study provides a new approach for realizing highly efficient optoelectronic devices based on TMDCs.

We observe that carriers in graphene can be accelerated to the Fermi velocity without heating the lattice. At large Fermi energy | E F | > 110 meV, electrons excited by a high-power terahertz pulse E THz relax by emitting optical phonons, resulting in heating of the graphene lattice and optical-phonon generation. This is owing to enhanced electron-phonon scattering at large Fermi energy, at which the large phase space is available for hot electrons. The emitted optical phonons cause carrier scattering, reducing the drift velocity or carrier mobility. However, for | E F | ≤ 110 meV, electron-phonon scattering rate is suppressed owing to the diminishing density of states near the Dirac point. Therefore, E THz continues to accelerate carriers without them losing energy to optical phonons, allowing the carriers to travel at the Fermi velocity. The exotic carrier dynamics does not result from the massless nature, but the electron-optical-phonon scattering rate depends on Fermi level in the graphene. Our observations provide insight into the application of graphene for high-speed electronics without degrading carrier mobility.

Epitaxial growth suffers from the mismatches in lattice and dangling bonds arising from different crystal structures or unit cell parameters. Here, we demonstrate the epitaxial growth of 2D MoS 2 ribbon on 1D CdS nanowires (NWs) via surface and subsurface defects. The interstitial Cd 0 in the (12̅10) crystal plane of the [0001]-oriented CdS NWs are found to serve as nucleation sites for interatomically bonded [001]-oriented MoS 2 , where the perfect lattice match (∼99.7%) between the (101̅1) plane of CdS and the (002)-faceted in-plane MoS 2 result in coaxial MoS 2 ribbon/CdS NWs heterojunction. The coaxial but heterotropic epitaxial MoS 2 ribbon on the surface of CdS NWs induces delocalized interface states that facilitate charge transport and the reduced surface state. A less than 5-fold ribbon width of MoS 2 as hydrogen evolution cocatalyst exhibits a ∼10-fold H 2 evolution enhancement than state of the art Pt in an acidic electrolyte, and apparent quantum yields of 79.7% at 420 nm, 53.1% at 450 nm, and 9.67% at 520 nm, respectively.

Demands on high-quality layer structured two-dimensional (2D) thin films such as pnictogen chalcogenides and transition metal dichalcogenides are growing due to the findings of exotic physical properties and potentials for device applications. However, the difficulties in controlling epitaxial growth and the unclear understanding of van der Waals epitaxy (vdWE) for a 2D chalcogenide film on a three-dimensional (3D) substrate have been major obstacles for the further advances of 2D materials. Here, we exploit the spontaneous vdWE of a high-quality 2D chalcogenide (Bi 0.5 Sb 1.5 Te 3 ) film by the chalcogen-driven surface reconstruction of a conventional 3D sapphire substrate. It is verified that the in situ formation of a pseudomorphic Te atomic monolayer on the surface of sapphire, which results in a dangling bond-free surface, allows the spontaneous vdWE of 2D chalcogenide film. Since this route uses the natural surface reconstruction of sapphire with chalcogen under vacuum condition, it can be scalable and easily utilized for the developments of various 2D chalcogenide vdWE films through conventional thin-film fabrication technologies.

Phase transitions in correlated materials can be manipulated at the nanoscale to yield emergent functional properties, promising new paradigms for nanoelectronics and nanophotonics. Vanadium dioxide (VO 2 ), an archetypal correlated material, exhibits a metal-insulator transition (MIT) above room temperature. At the thicknesses required for heterostructure applications, such as an optical modulator discussed here, the strain state of VO 2 largely determines the MIT dynamics critical to the device performance. We develop an approach to control the MIT dynamics in epitaxial VO 2 films by employing an intermediate template layer with large lattice mismatch to relieve the interfacial lattice constraints, contrary to conventional thin film epitaxy that favors lattice match between the substrate and the growing film. A combination of phase-field simulation, in situ real-time nanoscale imaging, and electrical measurements reveals robust undisturbed MIT dynamics even at preexisting structural domain boundaries and significantly sharpened MIT in the templated VO 2 films. Utilizing the sharp MIT, we demonstrate a fast, electrically switchable optical waveguide. This study offers unconventional design principles for heteroepitaxial correlated materials, as well as novel insight into their nanoscale phase transitions.

Nanoscale metal/graphene nanolayered composite is known to have ultrahigh strength as the graphene effectively blocks dislocations from penetrating through the metal/graphene interface. The same graphene interface, which has a strong sp2 bonding, can simultaneously serve as an effective interface for deflecting the fatigue cracks that are generated under cyclic bendings. In this study, Cu/Gr composite with repeat layer spacing of 100 nm was tested for bending fatigue at 1.6% and 3.1% strain up to 1,000,000 cycles that showed for the first time a 5-6 times enhancement in fatigue resistance compared to the conventional Cu thin film. Fatigue cracks that are generated within the Cu layer were stopped by the graphene interface, which are evidenced by cross-sectional scanning electron microscopy and transmission electron microscopy images. Molecular dynamics simulations for uniaxial tension of Cu/Gr showed limited accumulation of dislocations at the film/substrate interface, which makes the fatigue crack formation and propagation through thickness of the film difficult in this materials system.

Monolayer MoS 2 , among many other transition metal dichalcogenides, holds great promise for future applications in nanoelectronics and optoelectronics due to its ultrathin nature, flexibility, sizable band gap, and unique spin-valley coupled physics. However, careful study of these properties at low temperature has been hindered by an inability to achieve low-temperature Ohmic contacts to monolayer MoS 2 , particularly at low carrier densities. In this work, we report a new contact scheme that utilizes cobalt (Co) with a monolayer of hexagonal boron nitride (h-BN) that has the following two functions: modifies the work function of Co and acts as a tunneling barrier. We measure a flat-band Schottky barrier of 16 meV, which makes thin tunnel barriers upon doping the channels, and thus achieve low-T contact resistance of 3 kΩ.μm at a carrier density of 5.3 × 10 12 /cm 2 . This further allows us to observe Shubnikov-de Haas oscillations in monolayer MoS 2 at much lower carrier densities compared to previous work.

Doping two-dimensional (2D) semiconductors beyond their degenerate levels provides the opportunity to investigate extreme carrier density-driven superconductivity and phase transition in 2D systems. Chemical functionalization and the ionic gating have achieved the high doping density, but their effective ranges have been limited to ∼1 nm, which restricts the use of highly doped 2D semiconductors. Here, we report on electron diffusion from the 2D electride [Ca 2 N] + ·e - to MoTe 2 over a distance of 100 nm from the contact interface, generating an electron doping density higher than 1.6 × 10 14 cm -2 and a lattice symmetry change of MoTe 2 as a consequence of the extreme doping. The long-range lattice symmetry change, suggesting a length scale surpassing the depletion width of conventional metal-semiconductor junctions, was a consequence of the low work function (2.6 eV) with highly mobile anionic electron layers of [Ca 2 N] + ·e - . The combination of 2D electrides and layered materials yields a novel material design in terms of doping and lattice engineering.

Dislocations are one-dimensional line defects in three-dimensional crystals or periodic structures. It is common that the dislocation networks made of interactive dislocations be generated during plastic deformation. In van der Waals layered materials, the highly anisotropic nature facilitates the formation of such dislocation networks, which is critical for the friction or exfoliation behavior for these materials. By transmission electron microscopy analysis, we found the topological defects in such dislocation networks can be perfectly rationalized in the framework of traditional dislocation theory, which we applied the name "hyperdislocations". Due to the strong pinning effect of hyperdislocations, the state of exfoliation can be easily triggered by 1° twisting between two layers, which also explains the origin of disregistry and frictionlessness for all of the superlubricants that are widely used for friction reduction and wear protection.

Aside from unusual properties of monolayer graphene, bilayer has been shown to have even more interesting physics, in particular allowing bandgap opening with dual gating for proper interlayer symmetry. Such properties, promising for device applications, ignited significant interest in understanding and controlling the growth of bilayer graphene. Here we systematically investigate a broad set of flow rates and relative gas ratio of CH 4 to H 2 in atmospheric pressure chemical vapor deposition of multilayered graphene. Two very different growth windows are identified. For relatively high CH 4 to H 2 ratios, graphene growth is relatively rapid with an initial first full layer forming in seconds upon which new graphene flakes nucleate then grow on top of the first layer. The stacking of these flakes versus the initial graphene layer is mostly turbostratic. This growth mode can be likened to Stranski-Krastanov growth. With relatively low CH 4 to H 2 ratios, growth rates are reduced due to a lower carbon supply rate. In addition bi-, tri-, and few-layer flakes form directly over the Cu substrate as individual islands. Etching studies show that in this growth mode subsequent layers form beneath the first layer presumably through carbon radical intercalation. This growth mode is similar to that found with Volmer-Weber growth and was shown to produce highly oriented AB-stacked materials. These systematic studies provide new insight into bilayer graphene formation and define the synthetic range where gapped bilayer graphene can be reliably produced.

Layered hexagonal boron nitride (h-BN) thin film is a dielectric that surpasses carrier mobility by reducing charge scattering with silicon oxide in diverse electronics formed with graphene and transition metal dichalcogenides. However, the h-BN effect on electron doping concentration and Schottky barrier is little known. Here, we report that use of h-BN thin film as a substrate for monolayer MoS 2 can induce ∼6.5 × 10 11 cm -2 electron doping at room temperature which was determined using theoretical flat band model and interface trap density. The saturated excess electron concentration of MoS 2 on h-BN was found to be ∼5 × 10 13 cm -2 at high temperature and was significantly reduced at low temperature. Further, the inserted h-BN enables us to reduce the Coulombic charge scattering in MoS 2 /h-BN and lower the effective Schottky barrier height by a factor of 3, which gives rise to four times enhanced the field-effect carrier mobility and an emergence of metal-insulator transition at a much lower charge density of ∼1.0 × 10 12 cm -2 (T = 25 K). The reduced effective Schottky barrier height in MoS 2 /h-BN is attributed to the decreased effective work function of MoS 2 arisen from h-BN induced n-doping and the reduced effective metal work function due to dipole moments originated from fixed charges in SiO 2 .

Enhancing hole extraction inside the perovskite layer is the key factor for boosting photovoltaic performance. Realization of halide concentration gradient perovskite materials has been expected to exhibit rapid hole extraction due to the precise bandgap tuning. Moreover, a formation of Br-rich region on the tri-iodide perovskite layer is expected to enhance moisture stability without a loss of current density. However, conventional synthetic techniques of perovskite materials such as the solution process have not achieved the realization of halide concentration gradient perovskite materials. In this report, we demonstrate the fabrication of Br concentration gradient mixed halide perovskite materials using a novel and facile halide conversion method based on vaporized hydrobromic acid. Accelerated hole extraction and enhanced lifetime due to Br gradient was verified by observing photoluminescence properties. Through the combination of secondary ion mass spectroscopy and transmission electron microscopy with energy-dispersive X-ray spectroscopy analysis, the diffusion behavior of Br ions in perovskite materials was investigated. The Br-gradient was found to be eventually converted into a homogeneous mixed halide layer after undergoing an intermixing process. Br-substituted perovskite solar cells exhibited a power conversion efficiency of 18.94% due to an increase in open circuit voltage from 1.08 to 1.11 V and an advance in fill-factor from 0.71 to 0.74. Long-term stability was also dramatically enhanced after the conversion process, i.e., the power conversion efficiency of the post-treated device has remained over 97% of the initial value under high humid conditions (40-90%) without any encapsulation for 4 weeks.

Electrical transport in monolayer graphene on SrTiO3 (STO) thin film is examined in order to promote gate-voltage scaling using a high-k dielectric material. The atomically flat surface of thin STO layer epitaxially grown on Nb-doped STO single-crystal substrate offers good adhesion between the high-k film and graphene, resulting in nonhysteretic conductance as a function of gate voltage at all temperatures down to 2 K. The two-terminal conductance quantization under magnetic fields corresponding to quantum Hall states survives up to 200 K at a magnetic field of 14 T. In addition, the substantial shift of charge neutrality point in graphene seems to correlate with the temperature-dependent dielectric constant of the STO thin film, and its effective dielectric properties could be deduced from the universality of quantum phenomena in graphene. Our experimental data prove that the operating voltage reduction can be successfully realized due to the underlying high-k STO thin film, without any noticeable degradation of graphene device performance.