Device Applications Research Articles

Resistive Memristors Using Robust Electropolymerized Porous Organic Polymer Films as Switchable Materials.

Porous organic polymers (POPs) with inherent porosity, tunable pore environment, and semiconductive property are ideally suitable for application in various advanced semiconductor-related devices. However, owing to the lack of processability, POPs are usually prepared in powder forms, which limits their application in advanced devices. Herein, we demonstrate an example of information storage application of POPs with film form prepared by an electrochemical method. The growth process of the electropolymerized films in accordance with the Volmer-Weber model was proposed by observation of atomic force microscopy. Given the mechanism of the electron transfer system, we verified and mainly emphasized the importance of porosity and interfacial properties of porous polymer films for memristor. As expected, the as-fabricated memristors exhibit good performance on low turn-on voltage (0.65 ± 0.10 V), reliable data storage, and high on/off current ratio (104). This work offers inspiration for applying POPs in the form of electropolymerized films in various advanced semiconductor-related devices.

Coupled Electronic and Magnonic Topological States in Two-Dimensional Ferromagnets.

Magnetic materials offer a fertile playground for fundamental physics discovery, with not only electronic but also magnonic topological states intensively explored. However, one natural material with both electronic and magnonic nontrivial topologies is still unknown. Here, we demonstrate the coexistence of first-order topological magnon insulators (TMIs) and electronic second-order topological insulators (SOTIs) in 2D honeycomb ferromagnets, giving rise to the nontrivial corner states being connected by the charge-free magnonic edge states. We show that, with symmetry, the phase factor ± ϕ caused by the next nearest-neighbor Dzyaloshinskii-Moriya interaction breaks the pseudo-spin time-reversal symmetry , which leads to the split of magnon bands, i.e., the emergence of TMIs with a nonzero Chern number of , in experimentally feasible candidates of MoI3, CrSiTe3, and CrGeTe3 monolayers. Moreover, protected by the symmetry, the electronic SOTIs characterized by nontrivial corner states are obtained, bridging the topological aspect of fermions and bosons with a high possibility of innovative applications in spintronics devices.

Boosting Supercapacitor Efficiency with Amorphous Biomass-Derived C@TiO2 Composites.

Carbon materials are readily available and are essential in energy storage. One of the routes used to enhance their surface area and activity is the decoration of carbons with semiconductors, such as amorphous TiO2, for application in energy storage devices. This work reports the preparation of amorphous TiO2 nanopowders, which were obtained through the anodization of titanium in ethaline media. The obtained amorphous TiO2 was used to obtain TiO2-decorated carbon (obtained through the carbonization of glycogen precursor from mussel cooking wastewater, under N2 atmosphere) composites through three different methods: electrochemical in-situ attachment of TiO2 nanopowders to the carbon matrix using ultrasounds and sonication in ethaline. Commercial TiO2 was used as the comparison material. Morphology, composition, and structure analysis were performed, followed by the electrochemical analysis in ethaline electrolyte. The in-situ attachment of amorphous TiO2 to the carbon matrix shows the most promising electrochemical performance of 956 F g-1 at 1 A g-1 for the three-electrode cell setup, with 100% and 98% capacitance retention after 1000 and 10000 cycles. On a two-electrode symmetric solid-state electrolyte cell, the gravimetric capacitance is 1251 F g-1, at 1 A g-1, with 90% and 78% capacitance retention after 1000 and 10000 cycles, respectively.

Design Strategies for Anti‐Freeze Electrolytes in Aqueous Energy Storage Devices at Low Temperatures

AbstractWith the continuous development of electrochemical energy storage technology, especially in the current pursuit of environmental sustainability and safety, aqueous energy storage devices, due to their high safety, environmental friendliness, and cost‐effectiveness, are becoming an important direction of development in the field of energy storage. Diverse application scenarios require that energy storage systems be capable of continuous power supply under low temperature conditions. However, conventional aqueous electrolytes freeze at extremely low temperatures, causing limited ion transport and slow reaction kinetics, degrading the performance of the energy storage system. The design of low‐temperature anti‐freeze aqueous electrolytes has become an effective way to address this issue. In this review, the deep connection between hydrogen bonds (HBs) interactions in aqueous electrolytes and the liquid‐to‐solid conversion process, and the fundamental principles of the anti‐freeze mechanism is first explored. Subsequently, a systematic categorization and discussion of the design strategies for low‐temperature anti‐freeze aqueous electrolytes are conducted. Finally, potential directions are proposed. This review aims to provide comprehensive scientific guidance and technical reference for the development of anti‐freeze aqueous electrolytes with excellent low‐temperature performance, thereby promoting the application and innovation of aqueous energy storage devices in low‐temperature environments.

Manipulating Spin‐Lattice Coupling in Layered Magnetic Topological Insulator Heterostructure via Interface Engineering

AbstractInduced magnetic order in a topological insulator (TI) can be realized either by depositing magnetic adatoms on the surface of a TI or engineering the interface with epitaxial thin film or stacked assembly of 2D van der Waals (vdW) materials. Herein, the observation of spin‐phonon coupling in the otherwise non‐magnetic TI Bi2Te3 is reported, due to the proximity of FePS3 (an antiferromagnet (AFM), TN ≈ 120 K), in a vdW heterostructure framework. Temperature‐dependent Raman spectroscopic studies reveal deviation from the usual phonon anharmonicity originated from spin‐lattice coupling at the Bi2Te3/FePS3 interface at/below 60 K in the peak position (self‐energy) and linewidth (lifetime) of the characteristic phonon modes of Bi2Te3 (106 and 138 cm−1) in the stacked heterostructure. The Ginzburg‐Landau (GL) formalism, where the respective phonon frequencies of Bi2Te3 couple to phonons of similar frequencies of FePS3 in the AFM phase, is adopted to understand the origin of the hybrid magneto‐elastic modes. At the same time, the reduction of characteristic TN of FePS3 from 120 K in isolated flakes to 65 K in the heterostructure, possibly due to the interfacial strain, which leads to smaller Fe‐S‐Fe bond angles as corroborated by computational studies using density functional theory (DFT). Besides, inserting hexagonal boron nitride within Bi2Te3/FePS3 stacking regains the anharmonicity in Bi2Te3. Controlling interfacial spin‐phonon coupling in stacked heterostructure can have potential application in surface code spin logic devices.

Integrating spin-dependent emission and dielectric switching in FeII catenated metal-organic frameworks

Mechanically interlocked molecules (MIMs) including famous catenanes show switchable physical properties and attract continuous research interest due to their potential application in molecular devices. The advantages of using spin crossover (SCO) materials here are enormous, allowing for control through diverse stimuli and highly specific functions, and enabling the transfer of the internal dynamics of MIMs from solution to solid state, leading to macroscopic applications. Herein, we report the efficient self-assembly of catenated metal-organic frameworks (termed catena-MOFs) induced by stacking interactions, through the combination of rationally selected flexible and conjugated naphthalene diimide-based bis-pyridyl ligand (BPND), [MI(CN)2]− (M = Ag or Au) and Fe2+ in a one-step strategy. The obtained bimetallic Hofmann-type SCO-MOFs [FeII(BPND){Ag(CN)2}2]·3CHCl3 (1Ag) and [FeII(BPND{Au(CN)2}2]·2CHCl3·2H2O (1Au) possess a unique three-dimensional (3D) catena-MOF constructed from the polycatenation of two-dimensional (2D) layers with hxl topology. Both complexes undergo thermal- and light-induced SCO. Significantly, abnormal increases in the maximum emission intensity and dielectric constant can be detected simultaneously with the switching of spin states. This research opens up SCO-actuated bistable MIMs that afford dual functionality of coupled fluorescence emission and dielectricity.

Tunable electronic, transport, and optical properties of fluorine- and hydrogen-passivated two-dimensional Ga2O3 by uniaxial strain

Two-dimensional (2D) semiconductors have shown great prospects for future-oriented optoelectronic applications, whereas the applications of conventional 2D materials are significantly impeded by their low electron mobility (⩽200 cm2 V−1 s−1). In this work, strain-mediated fluorine- and hydrogen-passivated 2D Ga2O3 systems (FGa2O3H) have been explored via using first-principles calculations with the Heyd–Scuseria–Ernzerh and Perdew–Burke–Ernzerhof functionals. Our results reveal a considerable high electron mobility of FGa2O3H up to 4863.05 cm2 V−1 s−1 as the uniaxial tensile strain reaches 6%, which can be attributed to the enhanced overlapping of wave functions and bonding features. Overall, when applying uniaxial strain monotonously along the a(b) direction from compressive to tensile cases, the bandgaps of 2D FGa2O3H increase initially and then decrease, which originates from the changes of σ* anti-bonding in the conduction band minimum and π bonding states in the valence band maximum accompanying the lengthening Ga–O bonds. Additionally, when the tensile strain is larger than 8%, the stronger π bonding at the G point leads to an indirect-to-direct transition. Besides the highest electron mobility observed in n-type doped 2D FGa2O3H with 6% tensile strain, the electrical conductivity is enhanced and further elevated as the temperature increases from 300 K to 800 K. The variations of the absorption coefficient in the ultraviolet region are negligible with increasing tensile strain from 0% to 6%, which sheds light on its applications in high-power optoelectronic devices.

Stacking-dependent interlayer magnetic interactions in CrSe2.

Recently, CrSe2, a new ferromagnetic van der Waals two-dimensional material, was discovered to be highly stable under ambient conditions, making it an attractive candidate for fundamental research and potential device applications. Here, we study the interlayer interactions of bilayer CrSe2using first-principles calculations. We demonstrate that the interlayer interaction depends on the stacking structure. The AA and AB stackings exhibit antiferromagnetic (AFM) interlayer interactions, while the AC stacking exhibits ferromagnetic (FM) interlayer interaction. Furthermore, the interlayer interaction can be further tuned by tensile strain and charge doping. Specifically, under large tensile strain, most stacking structures exhibit FM interlayer interactions. Conversely, under heavy electron doping, all stacking structures exhibit AFM interlayer interactions. These findings are useful for designing spintronic devices based on CrSe2.

Metal Halide Perovskite Single Crystals toward Electroluminescent Applications

AbstractMetal halide perovskite single crystals (MHP SCs) have attracted extensive attention due to their superior properties, such as higher carrier mobility, longer carrier diffusion length, and better stability than their polycrystalline counterparts. In particular, the suppression of ion migration and Auger recombination endows MHP SCs with excellent electroluminescence (EL) properties, thus holding great potential for highly efficient and stable light‐emitting devices. In this review, general overview of MHP crystal structures are begin, and highlight the merits of MHP SCs in terms of outstanding optoelectronic properties and high stability. Then, appropriate growth methods of high‐quality, thickness‐controlled MHP SCs for EL device applications are systematically summarized. Subsequently, recent advancements in developing MHP SC‐based perovskite light‐emitting diodes (PeLEDs) are discussed, and the effective strategies to further enhance the device performance are reviewed. Moreover, the potential application of MHP SCs for electrically pumped lasers is highlighted. Finally, the review is concluded with a detailed account of the current challenges and a perspective on the key approaches and opportunities on the optimization of SC growth, the improvement of device performance and the integration of SC‐based optoelectronic devices.

Topological Exciton Polaritons in Compact Perovskite Junction Metasurfaces

AbstractExciton polaritons are hybrid light‐matter quasi‐particles that hold exceptional opportunities for future optoelectronic devices. Taking the synergic advantages of room‐temperature perovskite excitons and topological photonic structures, topological exciton‐polaritons are experimentally demonstrated in organic–inorganic hybrid perovskite thin films. Topological junction structures based on perovskite gratings are realized using a momentum‐space analog of the 1D Dirac system. Desired enhancement phenomena are observed including narrow‐beam polariton emission from a tightly localized junction region, polaritonic nonlinearity boost, and enhanced luminescence. These remarkable features are obtained from highly compact devices with footprint widths on the order of a few micrometers and are efficiently tailorable with simple unit‐cell geometry control. Therefore, the proposed approach can be a powerful platform for room‐temperature topological exciton‐polaritons and concomitant device applications.

Insight into the Physical Properties of the Chalcogenide XZrS3 (X = Ca, Ba) Perovskites: A First-Principles Computation

AbstractThis study investigates the structural, mechanical, optical, thermal, and electronic properties of the ionic semiconducting materials XZrS3 (X = Ca, Ba) within the framework of density functional theory (DFT). Here, the elastic constants, modulus (bulk, shear, Young's), ratios (Pugh, Poisson) and elastic anisotropy for XZrS3 (X = Ca, Ba) are studied. Furthermore, the electronic, optical, and thermal properties for XZrS3 (X = Ca, Ba) are regenerated and designed using the values obtained with Cambridge Serial Total Energy Package (CASTEP) software. The calculated lattice parameters show excellent agreement with theoretical and experimental values. The elastic stiffness constants confirm the mechanical stability of both compounds. Although XZrS3 (X = Ca, Ba) is elastically anisotropic, it has little optical anisotropy. The electronic band structures of the material exhibit direct-bandgap semiconducting behavior, with values of 1.3 eV (CaZrS3) and 1.1 eV (BaZrS3) using the generalized gradient approximation (GGA), respectively, which is ideal for solar cell (0.9–1.56 eV) and optoelectronic device applications. Bandgap values of 1.9 eV and 1.6 eV are found for CaZrS3 and BaZrS3, respectively, using the Heyd–Scuseria–Ernzerhof HSE06 functional, which is consistent with previous theoretical and experimental bandgap results. The optical properties including dielectric function, refractive index, absorption coefficient, reflectivity, and loss function are characterized using the GGA of Perdew–Burke–Ernzerhof (GGA-PBE) and HSE06 methods and are discussed in detail. Because of the relatively low Debye temperature (D), thermal conductivity of the lattice (kph), and minimum thermal conductivity (Kmin), the studied materials can be used as thermal barrier coating (TBC) materials. The capacity of heat, Debye temperature, and thermal coefficient of expansion are all computed.

Rational design of hierarchical porous reduced graphene oxide/9,10-phenanthraquinone/porous carbon nanocomposites for high-performance supercapacitors

The development of advanced electrode material is crucial for promoting the application of new high-performance green energy storage devices and remains a great challenge. Herein, by introducing porous carbon (PC) or carbon nanotubes (CNTs) to further modify the redox-active 9,10-phenanthrenequinone (PQ) molecule non-covalently functionalized reduced graphene oxide (RGO), we have designed and synthesized RGO/PQ/PCs (RPPs) and RGO/PQ/CNTs-10 (RPC-10) nanocomposites using a simple one-step solvothermal method. Benefiting from the optimization of the hierarchical porous nanostructures and each composition further strengthens their respective advantages in the novel synthesized nanocomposites (RPPs and RPC-10), the RPPs and RPC-10 electrodes demonstrated significantly superior electrochemical energy storage performance over the RGO and RGO/PQ (RP) electrodes, especially for the RPP-10 electrode with a high specific capacitance of 343.5 F g−1 at 0.5 A g−1 and good rate capability (69.23 %, 0.5 − 40 A g−1). Furthermore, both the symmetric supercapacitor assembled with the optimal RPP-10 electrode and the hybrid supercapacitor assembled with the RPP-10 negative electrode and the NCSRC-24 positive electrode previously reported show excellent energy densities and ultra-long cycling stabilities. This result demonstrates that the synthesized novel RPP-10 nanocomposite is a highly promising candidate for new light-weight, sustainable, high-flexible and high-performance energy storage devices.

Improved Thermal Stability and Oxygen‐Barrier Performance of SiO2 Thin Films by Modifying Amorphous Network Structure

Due to low‐refractive‐index and grain‐boundary‐free features, amorphous SiO2 thin films possess inherent advantages in serving as antireflective and protective layers against atmosphere. However, under high‐temperature and/or oxidation harsh environment, the thermodynamic instability of SiO bonds and “depolymerization” process among tetrahedral units [SiO4] would result in their insufficient thermal stability and oxygen‐barrier failure. By taking amorphous network former, small element electronegativity, and high oxide dissociation energy into considerations, low‐level Zr dopant is introduced to induce short‐ and medium‐range structural modification in amorphous SiO2 thin films, aiming to shorten SiO bond length and enhance network connectivity, respectively. As expected, the fabricated SiZrO thin films exhibit superior thermal stability and oxygen‐barrier performance without sacrificing their low‐index attribute. The Zr doping significantly elevates the oxygen‐inward‐diffusion activation energy from 0.94 to 1.95 eV in SiO2 network. Further, utilizing as protective layer for W‐SiO2 cermet, the SiZrO can effectively prevent the oxidation of W nanoparticles caused by oxygen inward diffusion. Undoubtedly, the exploration of amorphous SiZrO thin films offers exciting prospects for the application of functional coatings and devices under extreme conditions.

Investigation of structural, electronic, optical and thermoelectric properties of hallide double perovskite Rb2AlAgX6 (X = Cl, I): A first-principles DFT study

In order to meet the demands of the energy consumption, double perovskites (DP) are a dependable green energy source. Consequently, there is a great deal of promise for thermoelectric and optoelectronic device applications when studying these perovskite halides. Our work examined the thermoelectric and optoelectronic properties of Rb2AlAgCl6 and Rb2AlAgI6 halides using Density Functional Theory (DFT). The tolerance factor and energy of formation for the halides that were examined show that they are stable in the cubic phase, structurally and thermodynamically. We calculated the bandgaps for Rb2AlAgCl6 (Eg = 3.82 eV) and Rb2AlAgI6 (Eg = 1.321 eV) using mBJ potentials, and compared them to the reported values. The optical characteristics of the materials under investigation were revealed through the use of a complicated dielectric function. The computed optical findings show that the materials are suitable for optoelectronic applications, with maximal light absorption occurring in the ultraviolet (UV) and infrared (IR) ranges. Optical parameters obtained includes large values of absorption coefficients (∼105cm−1), low reflectivity (∼1–15 %), and high optical conductivity (∼1015 sec−1). Thermoelectric properties revealed enhanced power factor for Rb2AlAgI6 as compared to Rb2AlAgCl6. These results imply that these materials are appropriate for application in optical and thermoelectric devices.

Investigation of Electrical, Dielectric, and Ferroelectric Properties of Complex Compounds BaTiO3 - Bi0.5K0.5TiO3 for some Device Applications

Investigation of Electrical, Dielectric, and Ferroelectric Properties of Complex Compounds BaTiO3 - Bi0.5K0.5TiO3 for some Device Applications

Electronic, magnetic and universality properties of room-temperature antiferromagnet Fe[formula omitted]O[formula omitted] monolayer

The previously reported X2O3 (X=V, Cr, Mn, Ta) monolayers crystallize in a honeycomb–kagome (HK) structure and are found primarily to be ferromagnetic Chern insulators with remarkable quantum anomalous Hall (QAH) properties. However, in this study, it was found that the HK Fe2O3 monolayer exhibits antiferromagnetic semiconducting properties suitable for advanced spintronics applications. Through first-principle calculations based on density functional theory (DFT) calculations, we show that the Fe2O3 monolayer has good energetic, mechanical, and dynamic stability. We further evaluate the magnetic anisotropy energies (MAE) of the Fe2O3 monolayer and find that it prefers the out-of-plane easy axis magnetization direction with a sizeable MAE value of 248.75 μeV per Fe atom. Moreover, by performing Monte Carlo (MC) simulations based on the 2D classical anisotropic Heisenberg model, we predict a Néel temperature of 631.7(5) K for the Fe2O3 monolayer. We demonstrate that the Fe2O3 monolayer belongs to the 2D Ising-like universality class based on the estimated critical exponent ratios of magnetic susceptibility, magnetization, and the exponent of the correlation length. Our findings demonstrate that the Fe2O3 monolayer can be a suitable candidate for future antiferromagnetic spintronic device applications, especially in ultra-high data processing and storage, due to the coexistence of AFM and semiconducting properties.

Balancing Ionic and Electronic Conduction at the LiFePO4 Cathode–Electrolyte Interface and Regulating Solid Electrolyte Interphase in Lithium‐Ion Batteries

AbstractRecently, in electric mobilities and stationary energy storage device applications, the development of long‐lasting, low‐cost, and high‐safety lithium‐ion batteries (LIBs) is widely studied. LiFePO4 (LFP) is a core cathode material for LIBs owing to its cost‐effectiveness and high safety. However, it exhibits low electronic conductivity and sluggish Li+ diffusion, hindering the application of LFP cathodes in high‐power battery industries. Herein, a triazole‐motivated electrolyte additive, 1‐(trimethylsilyl)−1H‐benzotriazole (TMSBTA) is presented, for mitigating iron dissolution via HF scavenging, reinforcing the robustness of the solid electrolyte interphase and constructing a cathode–electrolyte interface (CEI) to balance the ion and electron conduction of the CEI on the LFP cathode. Scanning probe microscopy performed in the conductive atomic force microscopy mode indicates that the electronically conductive CEI created by the oxidative decomposition of TMSBTA enables rapid and homogeneous lithiation and delithiation during cycling without morphological changes in the LFP particles. This study elucidates the design principles of the CEI on the LFP cathode and is expected to guide integrated electrolyte additive engineering for LFP‐containing LIBs.

2D Hybrid Perovskites: From Static and Dynamic Structures to Potential Applications.

2D perovskites have received great attention recently due to their structural tunability and environmental stability, making them highly promising candidates for various applications by breaking property bottlenecks that affect established materials. However, in 2D perovskites, the complicated interplay between organic spacers and inorganic slabs makes structural analysis challenging to interpret. A deeper understanding of the structure-property relationship in these systems is urgently needed to enable high-performance tunable optoelectronic devices. Herein, this study examines how structural changes, from constant lattice distortion and variable structural evolution, modeled with both static and dynamic structural descriptors, affect macroscopic properties and ultimately device performance. The effect of chemical composition, crystallographic inhomogeneity, and mechanical-stress-induced static structural changes and corresponding electronic band variations is reported. In addition, the structure dynamics are described from the viewpoint of anharmonic vibrations, which impact electron-phonon coupling and the carriers' dynamic processes. Correlated carrier-matter interactions, known as polarons and acting on fine electronic structures, are then discussed. Finally, reliable guidelines to facilitate design to exploit structural features and rationally achieve breakthroughs in 2D perovskite applications are proposed. This review provides a global structural landscape of 2D perovskites, expected to promote the prosperity of these materials in emerging device applications.

Cellulose nanofiber-mediated manifold dynamic synergy enabling adhesive and photo-detachable hydrogel for self-powered E-skin

Self-powered skin attachable and detachable electronics are under intense development to enable the internet of everything and everyone in new and useful ways. Existing on-demand separation strategies rely on complicated pretreatments and physical properties of the adherends, achieving detachable-on-demand in a facile, rapid, and universal way remains challenging. To overcome this challenge, an ingenious cellulose nanofiber-mediated manifold dynamic synergy strategy is developed to construct a supramolecular hydrogel with both reversible tough adhesion and easy photodetachment. The cellulose nanofiber-reinforced network and the coordination between Fe ions and polymer chains endow the dynamic reconfiguration of supramolecular networks and the adhesion behavior of the hydrogel. This strategy enables the simple and rapid fabrication of strong yet reversible hydrogels with tunable toughness ((Valuemax-Valuemin)/Valuemax of up to 86%), on-demand adhesion energy ((Valuemax-Valuemin)/Valuemax of up to 93%), and stable conductivity up to 12 mS cm−1. We further extend this strategy to fabricate different cellulose nanofiber/Fe3+-based hydrogels from various biomacromolecules and petroleum polymers, and shed light on exploration of fundamental dynamic supramolecular network reconfiguration. Simultaneously, we prepare an adhesive-detachable triboelectric nanogenerator as a human-machine interface for a self-powered wireless monitoring system based on this strategy, which can acquire the real-time, self-powered monitoring, and wireless whole-body movement signal, opening up possibilities for diversifying potential applications in electronic skins and intelligent devices.

Transient reflectance of silicon carbide during laser-induced phase separation

Laser irradiation can induce local modulations of functional material properties, such as a decreased resistivity or a variation in reflectance. Recent studies investigated the laser-induced phase separation of 4 H-SiC into carbon and silicon on top of regrown SiC to customize its electrical conductivity for the application in electronic devices. To understand the physical processes leading to the laser-induced phase separation, time-resolved pump-probe measurements represent a suitable tool. This study advances the state of the art by characterizing the transient reflectance changes in 4 H-SiC upon irradiation by spatially resolved pump-probe reflectometry. Since the laser heating alters the reflectance of the sample, the spatially resolved measurement enables to observe the heat conduction from the irradiated to the non-irradiated areas, which sustains for several milliseconds. Numerical simulations of the temperature evolution reveal a restricted one-dimensional heat conduction into depth due to the broad lateral extent of the irradiated area. The associated sustained increased temperature within the irradiated area most certainly abets the feasibility of the phase separation. These findings offer practical insights for optimizing the applied laser parameters to tailor the material properties via phase separation.