Reconfigurable Neuromorphic Computing: Materials, Devices, and Integration.

Neuromorphic computing has been attracting ever-increasing attention due to superior energy efficiency, with great promise to promote the next wave of artificial general intelligence in the post-Moore era. Current approaches are, however, broadly designed for stationary and unitary assignments, thus encountering reluctant interconnections, power consumption, and data-intensive computing in that domain. Reconfigurable neuromorphic computing, an on-demand paradigm inspired by the inherent programmability of brain, can maximally reallocate finite resources to perform the proliferation of reproducibly brain-inspired functions, highlighting a disruptive framework for bridging the gap between different primitives. Although relevant research has flourished in diverse materials and devices with novel mechanisms and architectures, a precise overview remains blank and urgently desirable. Herein, the recent strides along this pursuit are systematically reviewed from material, device, and integration perspectives. At the material and device level, one comprehensively conclude the dominant mechanisms for reconfigurability, categorized into ion migration, carrier migration, phase transition, spintronics, and photonics. Integration-level developments for reconfigurable neuromorphic computing are also exhibited. Finally, a perspective on the future challenges for reconfigurable neuromorphic computing is discussed, definitely expanding its horizon for scientific communities.

Robust Piezoelectricity with Spontaneous Polarization in Monolayer Tellurene and Multilayer Tellurium Film at Room Temperature for Reliable Memory.

Robust neuromorphic computing in the Big Data era calls for long-term stable crossbar-array memory cells; however, the elemental segregation in the switch unit and memory unit that inevitably occurs upon cycling breaks the compositional and structural stability, making the whole memory cell a failure. Searching for a novel material without segregation that can be used for both switch and memory units is the major concern to fabricate robust and reliable nonvolatile cross-array memory cells. Tellurium (Te) is found recently to be the only peculiar material without segregation for switching, but the memory function has not been demonstrated yet. Herein, apparent piezoelectricity is experimentally confirmed with spontaneous polarization behaviors in elementary 2D Te, even in monolayer tellurene (0.4 nm), due to the highly oriented polarization of the molecular structure and the non-centrosymmetric lattice structure. A large memory window of 7000, a low working voltage of 2 V, and high on switching current up to 36.6 µA µm-1 are achieved in the as-fabricated Te-based memory device, revealing the great promise of Te for both switching and memory units in one cell without segregation. The piezoelectric Te with spontaneous polarization provides a platform to build robust, reliable, and high-density logic-in-memory chips in neuromorphic computing.

Coupling enhancement mechanisms, materials, and strategies for surface-enhanced Raman scattering devices.

Surface-enhanced Raman scattering (SERS) has become one of the most sensitive analytical techniques for identifying the chemical components, molecular structures, molecular conformations, and the interactions between molecules. However, great challenges still need to be addressed until it can be widely accepted by the absolute quantification of analytes. Recently, many efforts have been devoted to addressing these issues via various electromagnetic (EM), chemical (CM), and EM-CM hybrid coupling enhancement strategies. In comparison with uncoupled SERS devices, they offer key advantages in terms of sensitivity, reproducibility, uniformity, stability, controllability and reliability. This review provides an in-depth analysis of coupled SERS devices, including coupling enhancement mechanisms, materials and approaches. Finally, we also discuss the remaining bottlenecks and possible strategies for the development of coupling-enhanced SERS devices in the future.

Record-Low Subthreshold-Swing Negative-Capacitance 2D Field-Effect Transistors.

Power consumption is one of the most challenging bottlenecks for complementary metal-oxide-semiconductor integration. Negative-capacitance field-effect transistors (NC-FETs) offer a promising platform to break the thermionic limit defined by the Boltzmann tyranny and architect energy-efficient devices. However, it is a great challenge to achieving ultralow-subthreshold-swing (SS) (10 mV dec-1 ) and small-hysteresis NC-FETs simultaneously at room temperature, which has only been reported using the hafnium zirconium oxide system. Here, based on a ferroelectric LiNbO3 thin film with great spontaneous polarization, an ultralow-SS NC-FET with small hysteresis is designed. The LiNbO3 NC-FET platform exhibits a record-low SS of 4.97 mV dec-1 with great repeatability due to the superior capacitance matching characteristic as evidenced by the negative differential resistance phenomenon. By modulating the structure and operating parameters (such as channel length (Lch ), drain-sourse bias (Vds ), and gate bias (Vg )) of devices, an optimized SS from ≈40 to ≈10 mV dec-1 and hysteresis from ≈900 to ≈60 mV are achieved simultaneously. The results provide a new potential method for future highly integrated electronic and optical integrated energy-efficient devices.

Heterostructured NiS2/ZnIn2S4 Realizing Toroid-like Li2O2 Deposition in Lithium-Oxygen Batteries with Low-Donor-Number Solvents.

The aprotic lithium-oxygen (Li-O2) battery has triggered tremendous efforts for advanced energy storage due to the high energy density. However, realizing toroid-like Li2O2 deposition in low-donor-number (DN) solvents is still the intractable obstruction. Herein, a heterostructured NiS2/ZnIn2S4 is elaborately developed and investigated as a promising catalyst to regulate the Li2O2 deposition in low-DN solvents. The as-developed NiS2/ZnIn2S4 promotes interfacial electron transfer, regulates the adsorption energy of the reaction intermediates, and accelerates O-O bond cleavage, which are convincingly evidenced experimentally and theoretically. As a result, the toroid-like Li2O2 product is achieved in a Li-O2 battery with low-DN solvents via the solvation-mediated pathway, which demonstrates superb cyclability over 490 cycles and a high output capacity of 3682 mA h g-1. The interface engineering of heterostructure catalysts offers more possibilities for the realization of toroid-like Li2O2 in low-DN solvents, holding great promise in achieving practical applications of Li-O2 batteries as well as enlightening the material design in catalytic systems.

Interfacial Capillary-Force-Driven Self-Assembly of Monolayer Colloidal Crystals for Supersensitive Plasmonic Sensors.

Colloidal lithography technology based on monolayer colloidal crystals (MCCs) is considered as an outstanding candidate for fabricating large-area patterned functional nanostructures and devices. Although many efforts have been devoted to achieve various novel applicatons, the quality of MCCs, a key factor for the controllability and reproducibility of the patterned nanostructures, is often overlooked. In this work, an interfacial capillary-force-driven self-assembly strategy (ICFDS) is designed to realize a high-quality and highly-ordered hexagonal monolayer MCCs array by resorting the capillary effect of the interfacial water film at substrate surface as well as controlling the zeta potential of the polystyrene particles. Compared with the conventional self-assembly method, this approach can realize the reself-assembly process on the substrate surface with few colloidal aggregates, vacancy, and crystal boundary defects. Furthermore, various typical large-scale nanostructure arrays are achieved by combining reactive ion etching, metal-assisted chemical etching, and so forth. Specifically, benefiting from the as-fabricated high-quality 2D hexagonal colloidal crystals, the surface plasmon resonance (SPR) sensors achieve an excellent refractive index sensitivity value of 3497 nm RIU-1 , which is competent for detecting bovine serum albumin with an ultralow concentration of 10-8 m. This work opens a window to prepare high-quality MCCs for more potential applications.

Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition.

The growing demand for lithium batteries with higher energy densities requires new electrode chemistries. Lithium metal is a promising candidate as the anode material due to its high theoretical specific capacity, negative electrochemical potential and favorable density. However, during cycling, low and uneven lithium ion concentration on the surface of anode usually results in uncontrolled dendrite growth, especially at high current densities. Here we tackle this issue by using lithiophilic montmorillonite as an additive in the ether-based electrolyte to regulate the lithium ion concentration on the anode surface and thus facilitate the uniform lithium deposition. The lithiophilic montmorillonite demonstrates a pumping feature that improves the self-concentrating kinetics of the lithium ion and thus accelerates the lithium ion transfer at the deposition/electrolyte interface. The signal intensity of TFSI- shows negligible changes via in situ Raman tracking of the ion flux at the electrochemical interface, indicating homogeneous ion distribution, which can lead to a stable and uniform lithium deposition on the anode surface. Our study indicates that the interfacial engineering induced by the lithiophilic montmorillonite could be a promising strategy to optimize the lithium deposition for next-generation lithium metal batteries.

Recent Progress on Surface Reconstruction of Earth-Abundant Electrocatalysts for Water Oxidation.

As one important electrode reaction in electrocatalytic and photoelectrochemical cells for renewable energy circulation, oxygen catalysis has attracted considerable research in developing efficient and cost-effective catalysts. Due to the inevitable formation of oxygenic intermediates on surface sites during the complex reaction steps, the surface structure dynamically evolves toward reaction-preferred active species. To date, transition metal compounds, here defined as TM-Xides, where "X" refers to typical nonmetal elements from group IIIA to VIA, including hydroxide as well, are reported as high-performance oxygen evolution reaction (OER) electrocatalysts. However, more studies observe at least exterior oxidation or amorphization of materials. Thus, whether the TM-Xides can be defined as OER catalysts deserves further discussion. This Review pays attention to recent progress on the surface reconstruction of TM-Xide OER electrocatalysts with an emphasis on the identification of the true active species for OER, and aims at disseminating the real contributors of OER performance, especially under long-duration electrocatalysis.

Modulating Electronic Structures of Inorganic Nanomaterials for Efficient Electrocatalytic Water Splitting.

Electrocatalytic water splitting is one of the most promising sustainable energy conversion technologies, but is limited by the sluggish electrochemical reactions. Inorganic nanomaterials have been widely used as efficient catalysts for promoting the electrochemical kinetics. Several approaches to optimize the activities of these nanocatalysts have been developed. The electronic structures of the catalysts play a pivotal role in governing the activity and thus have been identified as an essential descriptor. However, the underlying working mechanisms related to the refined electronic structures remain elusive. To establish the structure-electronic-behavior-activity relationship, a comprehensive overview of the developed strategies to regulate the electronic structures is presented, emphasizing the surface modification, strain, phase transition, and heterostructure. Current challenges to the fundamental understanding of electron behaviors in the nanocatalysts are fully discussed.

Cytomembrane-Structure-Inspired Active Ni-N-O Interface for Enhanced Oxygen Evolution Reaction.

Surface/interface design is one of the most significant and promising motivations to develop high-performance catalysts for electrolytic water splitting. Here, the nature of cytomembrane having the most effective and functional surface structure is mimicked to fabricate a new configuration of Ni-N-O porous interface nanoparticles (NiNO INPs) with strongly interacting nanointerface between the Ni3 N and NiO domains, for enhancing the electrocatalytic oxygen evolution reaction (OER) performance. The combination of transmission electron microscopy and electrochemical investigations, tracking the correlation between microstructure evolution and catalytic activity, demonstrate the strongly coupled nanointerface for an approximately sixfold improvement of electrolytic efficiency. Density functional theory simulates the electrocatalytic process with a maximum of 85% reduction of the energy barrier. Further investigations find that the real active site for the OER in the NiNO INPs is the strongly coupled Ni-N-O nanointerface, not the derived amorphous hydroxide, during the OER process. The determination of the correlation of constructed nanointerface with catalytic properties suggests a significant strategy toward the rational design of catalysts for efficient water electrocatalysis.

A Facile Molten-Salt Route for Large-Scale Synthesis of NiFe2O4 Nanoplates with Enhanced Lithium Storage Capability.

Binary metal oxides have been deemed as a promising class of electrode materials for high-performance lithium ion batteries owing to their higher conductivity and electrochemical activity than corresponding monometal oxides. Here, NiFe2O4 nanoplates consisting of nanosized building blocks have been successfully fabricated by a facile, large-scale NaCl and KCl molten-salt route, and the changes in the morphology of NiFe2O4 as a function of the molten-salt amount have been systemically investigated. The results indicate that the molten-salt amount mainly influences the diameter and thickness of the NiFe2O4 nanoplates as well as the morphology of the nanosized building blocks. Cyclic voltammetry (CV) and galvanostatic charge-discharge measurements have been conducted to evaluate the lithium storage properties of the NiFe2O4 nanoplates prepared with a Ni(NO3)2/Fe(NO3)3/KCl/NaCl molar ratio of 1:2:20:60. A high reversible capacity of 888 mAh g(-1) is delivered over 100 cycles at a current density of 100 mA g(-1). Even at a current density of 5000 mA g(-1) , the discharge capacity could still reach 173 mAh g(-1). Such excellent electrochemical performances of the NiFe2O4 nanoplates are contributed to the short Li(+) diffusion distance of the nanosized building blocks and the synergetic effect of the Ni(2+) and Fe(3+) ions.

Metal organic frameworks route to in situ insertion of multiwalled carbon nanotubes in Co3O4 polyhedra as anode materials for lithium-ion batteries.

Hybridizing nanostructured metal oxides with multiwalled carbon nanotubes (MWCNTs) is highly desirable for the improvement of electrochemical performance of lithium-ion batteries. Here, a facile and scalable strategy to fabricate hierarchical porous MWCNTs/Co3O4 nanocomposites has been reported, with the help of a morphology-maintained annealing treatment of carbon nanotubes inserted metal organic frameworks (MOFs). The designed MWCNTs/Co3O4 integrates the high theoretical capacity of Co3O4 and excellent conductivity as well as strong mechanical/chemical stability of MWCNTs. When tested as anode materials for lithium-ion batteries, the nanocomposite displays a high reversible capacity of 813 mAh g(-1) at a current density of 100 mA g(-1) after 100 charge-discharge cycles. Even at 1000 mA g(-1), a stable capacity as high as 514 mAh g(-1) could be maintained. The improved reversible capacity, excellent cycling stability, and good rate capability of MWCNTs/Co3O4 can be attributed to the hierarchical porous structure and the synergistic effect between Co3O4 and MWCNTs. Furthermore, owing to this versatile strategy, binary metal oxides MWCNTs/ZnCo2O4 could also be synthesized as promising anode materials for advanced lithium-ion batteries.

Sulfur-impregnated core-shell hierarchical porous carbon for lithium-sulfur batteries.

Core-shell hierarchical porous carbon spheres (HPCs) were synthesized by a facile hydrothermal method and used as host to incorporate sulfur. The microstructure, morphology, and specific surface areas of the resultant samples have been systematically characterized. The results indicate that most of sulfur is well dispersed over the core area of HPCs after the impregnation of sulfur. Meanwhile, the shell of HPCs with void pores is serving as a retard against the dissolution of lithium polysulfides. This structure can enhance the transport of electron and lithium ions as well as alleviate the stress caused by volume change during the charge-discharge process. The as-prepared HPC-sulfur (HPC-S) composite with 65.3 wt % sulfur delivers a high specific capacity of 1397.9 mA h g(-1) at a current density of 335 mA g(-1) (0.2 C) as a cathode material for lithium-sulfur (Li-S) batteries, and the discharge capacity of the electrode could still reach 753.2 mA h g(-1) at 6700 mA g(-1) (4 C). Moreover, the composite electrode exhibited an excellent cycling capacity of 830.5 mA h g(-1) after 200 cycles.

Core-shell NiFe2O4@TiO2 nanorods: an anode material with enhanced electrochemical performance for lithium-ion batteries.

Hierarchical porous core-shell NiFe2O4@TiO2 nanorods have been fabricated with the help of hydrothermal synthesis, chemical bath deposition, and a subsequent calcinating process. The nanorods with an average diameter of 48 nm and length of about 300-600 nm turn out have a highly uniform morphology and are composed of nanosized primary particles. Owing to the synergistic effect of individual constituents as well as the hierarchical porous structure, the novel core-shell NiFe2O4@TiO2 nanorods exhibit superior electrochemical performance when evaluated as anode materials for lithium-ion batteries. At the current density of 100 mA g(-1), the composite exhibits a reversible specific capacity of 1034 mAh g(-1) up to 100 charge-discharge cycles, which is much higher than the uncoated NiFe2O4 nanorods. Even when cycled at 2000 mA g(-1), the discharge capacity could still be maintained at 358 mAh g(-1).