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Abstract Experimentally achieving the first‐ever electric field periodic poling of single crystal barium titanate oxide (BTO, or BaTiO3) thin film on‐insulator is reported. Owing to the outstanding optical nonlinearities of BTO, this result is a key step toward achieving quasi‐phase‐matching (QPM). First, the BTO thin film is grown on a dysprosium scandate substrate using pulsed laser deposition with a thin layer of strontium ruthenate later serving as the bottom electrode for poling. The characterization of the BTO thin film using x‐ray diffraction (XRD) and piezo‐response force microscopy to demonstrate single crystal, single domain growth of the film that enables the desired periodic poling, are presented. To investigate the poling quality, both non‐destructive piezo force response microscopy and destructive etching‐assisted scanning electron microscopy (SEM) are applied, and it is shown that high quality, uniform, and intransient poling with 50% duty cycle and periods ranging from 2 µm to 10 µm is achieved. The successful realization of periodic poling in BTO thin film unlocks the potential for highly efficient nonlinear processes under QPM that seemed far‐fetched with prior polycrystalline BTO thin films which predominantly relied on efficiency‐limited random or non‐phase matching conditions and is a key step toward integration of BTO photonic devices.

Abstract By modulating subwavelength structures and integrating functional materials, 2D artificial microstructures (2D AMs), including heterostructures, superlattices, metasurfaces and microcavities, offer a powerful platform for significant manipulation of light fields and functions. These structures hold great promise in high‐performance and highly integrated optoelectronic devices. However, a comprehensive summary of 2D AMs remains elusive for photonics and optoelectronics. This review focuses on the latest breakthroughs in 2D AM devices, categorized into electronic devices, photonic devices, and optoelectronic devices. The control of electronic and optical properties through tuning twisted angles is discussed. Some typical strategies that enhance light‐matter interactions are introduced, covering the integration of 2D materials with external photonic structures and intrinsic polaritonic resonances. Additionally, the influences of external stimuli, such as vertical electric fields, enhanced optical fields and plasmonic confinements, on optoelectronic properties is analysed. The integrations of these devices are also thoroughly addressed. Challenges and future perspectives are summarized to stimulate research and development of 2D AMs for future photonics and optoelectronics.

Abstract To overcome the intrinsic inefficiency of the von Neumann architecture, neuromorphic devices that perform analog vector–matrix multiplication have been highlighted for achieving power‐ and time‐efficient data processing. In particular, artificial synapses, of which conductance should be programmed to represent the synaptic weights of the artificial neural network, have been intensively researched to realize neuromorphic devices. Here, inspired by excitatory and inhibitory synapses, we develop an artificial optoelectronic synapse that shows both potentiation and depression characteristics triggered only by optical inputs. The design of the artificial optoelectronic synapse, in which excitatory and inhibitory synaptic phototransistors are serially connected, enables these characteristics by spatiotemporally irradiating the phototransistor channels with optical pulses. Furthermore, a negative synaptic weight can be realized without the need for electronic components such as comparators. With such attributes, the artificial optoelectronic synapse is demonstrated to classify three digits with a high recognition rate (98.3%) and perform image preprocessing via analog vector–matrix multiplication.

Abstract Lead halide perovskites have received considerable attention from researchers over the past several years due to their superior optical and optoelectronic properties, because of which they can be a versatile platform for fundamental science research and applications. Patterned structures based on lead halide perovskites have much more novel properties compared with their more commonly seen bulk‐, micro‐, and nano‐crystals, such as improvement in antireflection, light‐scattering effects, and light absorption, as a result of their adjustability of spatial distributions. However, there are many challenges yet to be resolved in this field, such as insufficient patterned resolution, imperfect crystal quality, complicated preparation process, and so on. To pave the way to solve these problems, we provide a systematic presentation of current methods for fabricating lead halide perovskite patterned structures, including thermal imprint, use of etching films, two‐step vapor‐phase growth, template‐confined solution growth, and seed‐assisted growth. Furthermore, the advantages and disadvantages of these methods are elaborated in detail. In addition, thanks to the extraordinary properties of lead halide perovskite patterned structures, a variety of potential applications in optics and optoelectronics of these structures are described. Lastly, we put forward existing challenges and prospects in this exciting field.

Optoelectronic devices based on optically responsive materials have gained significant attention due to their low cross talk and reduced power consumption. These devices rely on light‐induced changes in conductance states, which are used to create synaptic weights for image recognition tasks in neural networks. However, a major drawback of such devices is the rapid decay of conductance states after light stimulus removal, which hinders their long‐term memory and performance without a continuous external stimulus in place. To address this issue, a platform neural network scheme is proposed to counter the natural decay of conductance in optoelectronic devices. The approach restores the memory effect of the devices and significantly enhances their performance by several orders of magnitude without using additional energy‐intensive techniques like training pulses or gate fields. Herein, the model is validated experimentally using optoelectronic devices fabricated with two different materials, BP and doped In2O3, and demonstrates the restoration of memory/image retention ability to any material system being studied for optoelectronic synapses and vision. This approach has important implications for the practical application of neuromorphic visual processing technologies, bringing them closer to real‐world applications.

Abstract Interlayer excitons (IXs) at the interface of heterostructures (HSs) with a staggered band alignment are fascinating quantum quasi‐particles with light‐emitting and long‐lifetime characteristics. In this study, the energy band alignments (EBAs) of the HS of MAPbI3 perovskite thin sheets with CdSe‐ZnS core–shell quantum dot (QD) layers are modulated by using different diameters of the QDs. Far‐red IX emission is observed at 1.42 eV from the HS of MAPbI3/CdSe‐ZnS‐QD (λem = 645 nm) with type‐II EBA owing to charge transfer. The lifetime of the far‐red IXs is estimated to be 5.68 µs, which is considerably longer than that (0.715 ns) of the intralayer excitons from CdSe‐ZnS‐QD. With increasing incident excitation power, the PL peak and its intensity of IXs are blue‐shifted and linearly increased, respectively, indicating a strong dipole alignment of far‐red IXs at the heterojunction. Back focal plane imaging suggests that the directions of dipole moments of the IXs are relatively out‐of‐plane compared to those of the intralayer excitons (MAPbI3 and CdSe‐ZnS‐QD). Notably, the abnormal behavior of the optical characteristics is observed near the phase transition temperature (90 K) of MAPbI3. MAPbI3/CdSe‐ZnS‐QD HS photodetectors show the increase in photocurrent and detectivity compared to MAPbI3 at IX excitation.

Abstract Two‐dimensional (2D) materials show outstanding properties such as dangling bond‐free surfaces, strong in‐plane while weak out‐of‐plane bonding, layer‐dependent electronic structures, and tunable electronic and optoelectronic properties, making them promising for numerous applications. Integrating 2D inorganics with organic materials to make van der Waals heterostructures at the 2D thickness limit has created new platforms for fabricating on‐demand multifunctional devices. To further broaden the limited choices of 2D inorganic‐based heterostructures, a wide range of available 2D organic materials with tunable properties have opened new opportunities for designing large numbers of heterostructures with 2D inorganic materials. This review aims to attract the attention of researchers toward this emerging 2D organic−inorganic field. We first highlight recent progress in organic−inorganic heterostructures and their synthesis and then discuss their potential applications, such as field‐effect transistors, photodetectors, solar cells, and neuromorphic computing devices. In the end, we present a summary of challenges and opportunities in this field.

Abstract This review addresses the latest advancements in the integration of aggregation‐induced emission (AIE) materials with polymer electrospinning, to accomplish fine‐scale electrospun fibers with tunable photophysical and photochemical properties. Micro‐ and nanoscale fibers augmented with AIE dyes (termed AIEgens) are bespoke composite systems that can overcome the limitation posed by aggregation‐caused quenching, a critical deficiency of conventional luminescent materials. This review comprises three parts. First, the reader is exposed to the basic concepts of AIE and the fundamental mechanisms underpinning the restriction of intermolecular motions. This is followed by an introduction to electrospinning techniques pertinent to AIE‐based fibers, and the core parameters for controlling fiber architecture and resultant properties. Second, exemplars are drawn from latest research to demonstrate how electrospun nanofibers and porous films incorporating modified AIEgens (especially tetraphenylethylene and triphenylamine derivatives) can yield enhanced photostability, photothermal properties, photoefficiency (quantum yield), and improved device sensitivity. Advanced applications are drawn from several promising sectors, encompassing optoelectronics, drug delivery and biology, chemosensors and mechanochromic sensors, and innovative photothermal devices, among others. Finally, the outstanding challenges together with potential opportunities in the nascent field of electrospun AIE‐active fibers are presented, for stimulating frontier research and explorations in this exciting field.

Abstract Members of the 2D group VA semiconductors (phosphorene, arsenene, antimonene, and bismuthine) present a new class of 2D materials, which are recently gaining a lot of research interest. These materials possess layered morphology, tunable direct bandgap, high charge carrier mobility, high stability, unique in‐plane anisotropy, and negative Poisson's ratio. They prepare the ground for novel and multifunctional applications in electronics, optoelectronics, and batteries. The most recent analytical and empirical developments in the fundamental characteristics, fabrication techniques, and potential implementation of 2D group VA materials in this review, along with presenting insights and concerns for the field's future are analyzed.

Abstract Atomically thin two‐dimensional (2D) bismuth oxychalcogenides (Bi2O2X, X = S, Se, Te) have recently attracted extensive attention in the material research community due to their unique structure, outstanding long‐term ambient stability, and high carrier mobility, which enable them as promising candidates for high‐performance electronic and optoelectronic applications. Herein, we present a comprehensive review on the recent advances of 2D bismuth oxychalcogenides research. We start with an introduction of their fundamental properties including crystal structure and electronic band structure. Next, we summarize the common techniques for synthesizing these 2D structures with high crystallinity and large lateral size. Furthermore, we elaborate on their device applications including transistors, artificial synapses, optical switch and photodetectors. The last but not the least, we summarize the existing challenges and prospects for this emerging 2D bismuth oxychalcogenides field.

Abstract Electrically conductive thin‐film materials possessing high transparency are essential components for many optoelectronic devices. The advancement in the transparent conductor applications requires a replacement of indium tin oxide (ITO), one of the key materials in electronics. ITO and other transparent conductive metal oxides have several drawbacks, including poor flexibility, high refractive index and haze, limited chemical stability, and depleted raw material supply. Single‐walled carbon nanotubes (SWCNTs) are a promising alternative for transparent conducting films (TCFs) because of their unique and excellent chemical and physical properties. Here, the latest achievements in the optoelectronic performance of TCFs based on SWCNTs are analyzed. Various approaches to evaluate the performance of transparent electrodes are briefly reviewed. A roadmap for further research and development of the transparent conductors using “rational design,” which breaks the deadlock for obtaining the TCFs with a performance close to the theoretical limit, is also described.

Abstract Bottom‐up synthesized graphene nanostructures, including 0D graphene quantum dots and 1D graphene nanoribbons, have recently emerged as promising candidates for efficient, green optoelectronic, and energy storage applications. The versatility in their molecular structures offers a large and novel library of nanographenes with excellent and adjustable optical, electronic, and catalytic properties. In this minireview, recent progress on the fundamental understanding of the properties of different graphene nanostructures, and their state‐of‐the‐art applications in optoelectronics and energy storage are summarized. The properties of pristine nanographenes, including high emissivity and intriguing blinking effect in graphene quantum dots, superior charge transport properties in graphene nanoribbons, and edge‐specific electrochemistry in various graphene nanostructures, are highlighted. Furthermore, it is shown that emerging nanographene‐2D material‐based van der Waals heterostructures provide an exciting opportunity for efficient green optoelectronics with tunable characteristics. Finally, challenges and opportunities of the field are highlighted by offering guidelines for future combined efforts in the synthesis, assembly, spectroscopic, and electrical studies as well as (nano)fabrication to boost the progress toward advanced device applications.

Abstract Structural control of single‐wall carbon nanotubes (SWCNTs) with uniform properties is critical not only for their property modulation and functional design but also for applications in electronics, optics, and optoelectronics. To achieve this goal, various separation techniques have been developed in the past 20 years through which separation of high‐purity semiconducting/metallic SWCNTs, single‐chirality species, and even their enantiomers have been achieved. This progress has promoted the property modulation of SWCNTs and the development of SWCNT‐based optoelectronic devices. Here, the recent advances in the structure separation of SWCNTs are reviewed, from metallic/semiconducting SWCNTs, to single‐chirality species, and to enantiomers by several typical separation techniques and the application of the corresponding sorted SWCNTs. Based on the separation procedure, efficiency, and scalability, as well as, the separable SWCNT species, purity, and quantity, the advantages and disadvantages of various separation techniques are compared. Combined with the requirements of SWCNT application, the challenges, prospects, and development direction of structure separation are further discussed.

Abstract Van der Waals heterojunctions are fast‐emerging quantum structures fabricated by the controlled stacking of two‐dimensional (2D) materials. Owing to the atomically thin thickness, their carrier properties are not only determined by the host material itself, but also defined by the interlayer interactions, including dielectric environment, charge trapping centers, and stacking angles. The abundant constituents without the limitation of lattice constant matching enable fascinating electrical, optical, and magnetic properties in van der Waals heterojunctions toward next‐generation devices in photonics, optoelectronics, and information sciences. This review focuses on the charge and energy transfer processes and their dynamics in transition metal dichalcogenides (TMDCs), a family of quantum materials with strong excitonic effects and unique valley properties, and other related 2D materials such as graphene and hexagonal‐boron nitride. In the first part, we summarize the ultrafast charge transfer processes in van der Waals heterojunctions, including its experimental evidence and theoretical understanding, the interlayer excitons at the TMDC interfaces, and the hot carrier injection at the graphene/TMDCs interface. In the second part, the energy transfer, including both Förster and Dexter types, are reviewed from both experimental and theoretical perspectives. Finally, we highlight the typical charge and energy transfer applications in photodetectors and summarize the challenges and opportunities for future development in this field.

Abstract Semiconductor nanoplatelets (NPLs), with their large exciton binding energy, narrow photoluminescence (PL), and absence of dielectric screening for photons emitted normal to the NPL surface, could be expected to become the fastest luminophores amongst all colloidal nanostructures. However, super‐fast emission is suppressed by a dark (optically passive) exciton ground state, substantially split from a higher‐lying bright (optically active) state. Here, the exciton fine structure in 2–8 monolayer (ML) thick Csn − 1PbnBr3n + 1 NPLs is revealed by merging temperature‐resolved PL spectra and time‐resolved PL decay with an effective mass model taking quantum confinement and dielectric confinement anisotropy into account. This approach exposes a thickness‐dependent bright–dark exciton splitting reaching 32.3 meV for the 2 ML NPLs. The model also reveals a 5–16 meV splitting of the bright exciton states with transition dipoles polarized parallel and perpendicular to the NPL surfaces, the order of which is reversed for the thinnest NPLs, as confirmed by TR‐PL measurements. Accordingly, the individual bright states must be taken into account, while the dark exciton state strongly affects the optical properties of the thinnest NPLs even at room temperature. Significantly, the derived model can be generalized for any isotropically or anisotropically confined nanostructure.

Abstract Research on engineered materials that integrate different 2D crystals has largely focused on two prototypical heterostructures: Vertical van der Waals stacks and lateral heterostructures of covalently stitched monolayers. Extending lateral integration to few layer or even multilayer van der Waals crystals could enable architectures that combine the superior light absorption and photonic properties of thicker crystals with close proximity to interfaces and efficient carrier separation within the layers, potentially benefiting applications such as photovoltaics. Here, the realization of multilayer heterstructures of the van der Waals semiconductors SnS and GeS with lateral interfaces spanning up to several hundred individual layers is demonstrated. Structural and chemical imaging identifies {110} interfaces that are perpendicular to the (001) layer plane and are laterally localized and sharp on a 10 nm scale across the entire thickness. Cathodoluminescence spectroscopy provides evidence for a facile transfer of electron‐hole pairs across the lateral interfaces, indicating covalent stitching with high electronic quality and a low density of recombination centers.

Electrical and optical biointerfaces have contributed considerably to understanding biological systems. Recent advances in biocompatible materials, structure designs, and fabrication techniques have established flexible and minimally invasive electronic/optoelectronic platforms that laminate onto targeted surface regions or implant into precise locations of biosystems to monitor and control various biological processes at cell, tissue, and organ levels. Herein, recent progress in advanced biointegrated electrical and optical platforms is discussed. An overview of materials and device designs to form flexible and even stretchable electrodes is presented. Strategies to reduce tissue damage and foreign‐body response to improve chronic stability are described. State‐of‐the‐art wearable and implantable microsystems with/without wireless capabilities for bioelectrical sensing and stimulation, optical recording and modulation, and multimodal operation are highlighted. In conclusion, a discussion of the remaining obstacles for future research in these areas is provided.

Abstract The remarkable optoelectronic properties and considerable performance of the organo lead‐halide perovskites (PVKs) in various optoelectronic applications grasp tremendous scientific attention. However, the existence of the toxic lead in these compounds is threatening human health and remains a major concern in the way of their commercialization. To address this issue, numerous nontoxic alternatives have been reported. Among these alternatives, bismuth‐based PVKs have emerged as a promising substitute because of similar optoelectronic properties and extended environmental stability. This work communicates briefly about the possible lead‐alternatives and explores bismuth‐based perovskites comprehensively, in terms of their structures, optoelectronic properties, and applications. A brief description of lead‐toxification is provided and the possible Pb‐alternatives from the periodic table are scrutinized. Then, the classification and crystal structures of various Bi‐based perovskites are elaborated on. Detailed optoelectronic properties of Bi‐based perovskites are also described and their optoelectronic applications are abridged. The overall photovoltaic applications along with device characteristics (i.e., VOC, JSC, fill factor, FF, and power conversion efficiency, PCE), fabrication method, device architecture, and operational stability are also summarized. Finally, a conclusion is drawn where a brief outlook highlights the challenges that hamper the future progress of Bi‐based optoelectronic devices and suggestions for future directions are provided.

Abstract Graphene and the following derivative 2D materials have been demonstrated to exhibit rich distinct optoelectronic properties, such as broadband optical response, strong and tunable light–mater interactions, and fast relaxations in the flexible nanoscale. Combining with optical platforms like fibers, waveguides, grating, and resonators, these materials has spurred a variety of active and passive applications recently. Herein, the optical and electrical properties of graphene, transition metal dichalcogenides, black phosphorus, MXene, and their derivative van der Waals heterostructures are comprehensively reviewed, followed by the design and fabrication of these 2D material‐based optical structures in implementation. Next, distinct devices, ranging from lasers to light emitters, frequency convertors, modulators, detectors, plasmonic generators, and sensors, are introduced. Finally, the state‐of‐art investigation progress of 2D material‐based optoelectronics offers a promising way to realize new conceptual and high‐performance applications for information science and nanotechnology. The outlook on the development trends and important research directions are also put forward.

A wearable smart sensing system is capable of continuously monitoring biometric information such as respiration, pulse, and body temperature while attached to an arbitrary surface on the user's body to be utilized freely during activities. Research conducted on new materials, fabrication processes, structure of electrodes, and wireless communication technologies has made constant progress in the development of smart sensing systems that use entirely wearable forms of devices to go beyond conventional devices that are based on intrinsically rigid components, such as silicon. Among various platforms that can be used in the development of smart sensing systems, optoelectronics provides innovative sensing functions (e.g., human–machine interfaces and phototherapy) that can be transferred from traditional healthcare to smart healthcare, such as point of care. Optoelectronics are light‐mediated displays that allow a light source to be controlled and a large light spectrum to be detected. Recently, this platform that uses smart and wearable optoelectronic sensing systems has become increasingly advanced to better help human beings treat their diseases through self‐healthcare. Herein, recent advanced technologies in materials, structures, and wireless platforms for smart sensors using wearable optoelectronics are reviewed.

Abstract Direct 3D printing technologies to produce 3D optoelectronic architectures have been explored extensively over the last several years. Although commercially available 3D printing techniques are useful for many applications, their limits in printable materials, printing resolutions, or processing temperatures are significant challenges for structural optoelectronics in achieving fully 3D‐printed devices on 3D mechanical frames. Herein, the production of active optoelectronic devices with various form factors using a hybrid 3D printing process in ambient air is reported. This hybrid 3D printing system, which combines digital light processing for printing 3D mechanical architectures and a successive electrohydrodynamic jet for directly printing transparent pixels of organic light‐emitting diodes at room temperature, can create high‐resolution, transparent displays embedded inside arbitrarily shaped, 3D architectures in air. Also, the demonstration of a 3D‐printed, eyeglass‐type display for a wireless, augmented reality system is an example of another application. These results represent substantial progress in the development of next‐generation, freeform optoelectronics.