Ultrafast Solar‐Blind Ultraviolet Detection by Inorganic Perovskite CsPbX3 Quantum Dots Radial Junction Architecture

Inorganic CsPbX₃ (X = Cl, Br, I, or hybrid among them) perovskite quantum dots (IPQDs) are promising building blocks for exploring high performance optoelectronic applications. In this work, the authors report a new hybrid structure that marries CsPbX₃ IPQDs to silicon nanowires (SiNWs) radial junction structures to achieve ultrafast and highly sensitive ultraviolet (UV) detection in solar‐blind spectrum. A compact and uniform deployment of CsPbX₃ IPQDs upon the sidewall of low‐reflective 3D radial junctions enables a strong light field excitation and efficient down‐conversion of the ultraviolet incidences, which are directly tailored into emission bands optimized for a rapid photodetection in surrounding ultrathin radial p‐i‐n junctions. A fast solar‐blind UV detection has been demonstrated in this hybrid IPQD‐NW detectors, with rise/fall response time scales of 0.48/1.03 ms and a high responsivity of 54 mA W^?1@200 nm (or 32 mA W^?1@270 nm), without the need of any external power supply. These results pave the way toward large area manufacturing of high performance Si‐based perovskite UV detectors in a scalable and low‐cost procedure.     

Synergies of Electrochemical Metallization and Valance Change in All‐Inorganic Perovskite Quantum Dots for Resistive Switching

The in‐depth understanding of ions' generation and movement inside all‐inorganic perovskite quantum dots (CsPbBr₃ QDs), which may lead to a paradigm to break through the conventional von Neumann bottleneck, is strictly limited. Here, it is shown that formation and annihilation of metal conductive filaments and Br^? ion vacancy filaments driven by an external electric field and light irradiation can lead to pronounced resistive‐switching effects. Verified by field‐emission scanning electron microscopy as well as energy‐dispersive X‐ray spectroscopy analysis, the resistive switching behavior of CsPbBr₃ QD‐based photonic resistive random‐access memory (RRAM) is initiated by the electrochemical metallization and valance change. By coupling CsPbBr₃ QD‐based RRAM with a p‐channel transistor, the novel application of an RRAM–gate field‐effect transistor presenting analogous functions of flash memory is further demonstrated. These results may accelerate the technological deployment of all‐inorganic perovskite QD‐based photonic resistive memory for successful logic application.     

3D Nanoprinted Plastic Kinoform X‐Ray Optics

High‐performance focusing of X‐rays requires the realization of very challenging 3D geometries with nanoscale features, sub‐millimeter‐scale apertures, and high aspect ratios. A particularly difficult structure is the profile of an ideal zone plate called a kinoform, which is manufactured in nonideal approximated patterns, nonetheless requires complicated multistep fabrication processes. Here, 3D fabrication of high‐performance kinoforms with unprecedented aspect ratios out of low‐loss plastics using femtosecond two‐photon 3D nanoprinting is presented. A thorough characterization of the 3D‐printed kinoforms using direct soft X‐ray imaging and ptychography demonstrates superior performance with an efficiency reaching up to 20%. An extended concept is proposed for on‐chip integration of various X‐ray optics toward high‐fidelity control of X‐ray wavefronts and ultimate efficiencies even for harder X‐rays. Initial results establish new, advanced focusing optics for both synchrotron and laboratory sources for a large variety of X‐ray techniques and applications ranging from materials science to medicine.     

Photonic Synapses Based on Inorganic Perovskite Quantum Dots for Neuromorphic Computing

Inspired by the biological neuromorphic system, which exhibits a high degree of connectivity to process huge amounts of information, photonic memory is expected to pave a way to overcome the von Neumann bottleneck for nonconventional computing. Here, a photonic flash memory based on all‐inorganic CsPbBr₃ perovskite quantum dots (QDs) is demonstrated. The heterostructure formed between the CsPbBr₃ QDs and semiconductor layer serves as a basis for optically programmable and electrically erasable characteristics of the memory device. Furthermore, synapse functions including short‐term plasticity, long‐term plasticity, and spike‐rate‐dependent plasticity are emulated at the device level. The photonic potentiation and electrical habituation are implemented and the synaptic weight exhibits multiple wavelength response from 365, 450, 520 to 660 nm. These results may locate the stage for further thrilling novel advances in perovskite‐based memories.     

Ultrahigh‐Performance Self‐Powered Flexible Double‐Twisted Fibrous Broadband Perovskite Photodetector

Self‐powered flexible photodetectors without an external power source can meet the demands of next‐generation portable and wearable nanodevices; however, the performance is far from satisfactory becuase of the limited match of flexible substrates and light‐sensitive materials with proper energy levels. Herein, a novel self‐powered flexible fiber‐shaped photodetector based on double‐twisted perovskite–TiO₂–carbon fiber and CuO–Cu₂O–Cu wire is designed and fabricated. The device shows an ultrahigh detectivity of 2.15 × 10¹³ Jones under the illumination of 800 nm light at zero bias. CuO–Cu₂O electron block bilayer extends response range of perovskite from 850 to 1050 nm and suppresses dark current down to 10^?11 A. The fast response speed of less than 200 ms is nearly invariable after dozens of cycles of bending at the extremely 90 bending angle, demonstrating excellent flexibility and bending stability. These parameters are comparable and even better than reported flexible and even rigid photodetectors. The present results suggest a promising strategy to design photodetectors with integrated function of self‐power, flexibility, and broadband response.     

Elucidation of Photoluminescence Blinking Mechanism and Multiexciton Dynamics in Hybrid Organic–Inorganic Perovskite Quantum Dots

Halide perovskites (ABX₃) have emerged as promising materials in the past decade owing to their superior photophysical properties, rendering them potential candidates as solar cells, light‐emitting diode displays, and lasing materials. To optimize their utilization into optoelectronic devices, fundamental understanding of the optical behaviors is necessary. To reveal the comprehensive structure–property relationship, CH₃NH₃PbBr₃ (MAPbBr₃) perovskite quantum dots (PQDs) of three different sizes are prepared by controlling the precipitation temperature. Photoluminescence (PL) blinking, a key process that governs the emission efficiency of the PQD materials, is investigated in detail by the time‐resolved spectroscopic measurements of individual dots. The nature of the generated species in the course of blinking events is identified, and the mechanism governing the PL blinking is studied as a function of PQD sizes. Further, the practical applicability of MAPbBr₃ PQDs is assessed by studying the multiexciton dynamics under high photoexcitation intensity under which most of the display devices work. Ultrafast transient absorption spectroscopy helped in uncovering the volume‐dependent Auger recombination rates, which are further explored by comparing the early‐time transitions related to surface trap states and higher band states.     

Light‐Stimulated Synaptic Transistors Fabricated by a Facile Solution Process Based on Inorganic Perovskite Quantum Dots and Organic Semiconductors

Implementation of artificial intelligent systems with light‐stimulated synaptic emulators may enhance computational speed by providing devices with high bandwidth, low power computation requirements, and low crosstalk. One of the key challenges is to develop light‐stimulated devices that can response to light signals in a neuron‐/synapse‐like fashion. A simple and effective solution process to fabricate light‐stimulated synaptic transistors (LSSTs) based on inorganic halide perovskite quantum dots (IHP QDs) and organic semiconductors (OSCs) is reported. Blending IHP QDs and OSCs not only improves the charge separation efficiency of the photoexcited charges, but also induces delayed decay of the photocurrent in the IHP QDs/OSCs hybrid film. The enhanced charge separation efficiency results in high photoresponsivity, while the induced delayed decay of the photocurrent is critical to achieving light‐stimulating devices with a memory effect, which are important for achieving high synaptic performance. The LSSTs can respond to light signals in a highly neuron‐/synapse‐like fashion. Both short‐term and long‐term synaptic behaviors have been realized, which may lay the foundation for the future implementation of artificial intelligent systems that are enabled by light signals. More significantly, LSSTs are fabricated by a facile solution process which can be easily applied to large‐scale samples.     

High‐Performance Next‐Generation Perovskite Nanocrystal Scintillator for Nondestructive X‐Ray Imaging

Readily commercializable and cost‐effective next‐generation CsPbBr₃ perovskite nanocrystals (PNCs) based X‐ray detectors are demonstrated. The PNCs‐based X‐ray detector exhibits higher spatial resolution (9.8 lp mm^?1 at modulation transfer function (MTF) = 0.2 and 12.5–8.9 lp mm^?1 for a linear line chart), faster response time (≈200 ns), and comparable stability (>40 Gy_air s^?1 of X‐ray exposure) compared with the commercialized terbium‐doped gadolinium oxysulfide (GOS)‐based detectors (spatial resolution = 6.2 lp mm^?1 at MTF = 0.2 and 6.3 lp mm^?1 for a linear line chart, response time = ≈1200 ns) because the PNCs‐based scintillator has ≈5.6‐fold faster average photoluminescence lifetime and stronger emission than the GOS‐based one.     

Perovskite Quantum Dots and Their Application in Light‐Emitting Diodes

Perovskite quantum dots (PQDs) attract significant interest in recent years because of their unique optical properties, such as tunable wavelength, narrow emission, and high photoluminescence quantum efficiency (PLQY). Recent studies report new types of formamidinium (FA) PbBr₃ PQDs, PQDs with organic–inorganic mixed cations, divalent cation doped colloidal CsPb_1?xM_xBr₃ PQDs (M = Sn²⁺, Cd²⁺, Zn²⁺, Mn²⁺) featuring partial cation exchange, and heterovalent cation doped into PQDs (Bi³⁺). These PQD analogs open new possibilities for optoelectronic devices. For commercial applications in lighting and backlight displays, stability of PQDs requires further improvement to prevent their degradation by temperature, oxygen, moisture, and light. Oxygen and moisture‐facilitated ion migration may easily etch unstable PQDs. Easy ion migration may result in crystal growth, which lowers PLQY of PQDs. Surface coating and treatment are important procedures for overcoming such factors. In this study, new types of PQDs and a strategy of improving their stabilities are introduced. Finally, this paper discusses future applications of PQDs in light‐emitting diodes.     

Hierarchical 3D All‐Carbon Composite Structure Modified with N‐Doped Graphene Quantum Dots for High‐Performance Flexible Supercapacitors

Flexible supercapacitors have shown enormous potential for portable electronic devices. Herein, hierarchical 3D all‐carbon electrode materials are prepared by assembling N‐doped graphene quantum dots (N‐GQDs) on carbonized MOF materials (cZIF‐8) interweaved with carbon nanotubes (CNTs) for flexible all‐solid‐state supercapacitors. In this ternary electrode, cZIF‐8 provides a large accessible surface area, CNTs act as the electrical conductive network, and N‐GQDs serve as highly pseudocapactive materials. Due to the synergistic effect and hierarchical assembly of these components, N‐GQD@cZIF‐8/CNT electrodes exhibit a high specific capacitance of 540 F g^?1 at 0.5 A g^?1 in a 1 m H₂SO₄ electrolyte and excellent cycle stability with 90.9% capacity retention over 8000 cycles. The assembled supercapacitor possesses an energy density of 18.75 Wh kg^?1 with a power density of 108.7 W kg^?1. Meanwhile, three supercapacitors connected in series can power light‐emitting diodes for 20 min. All‐solid‐state N‐GQD@cZIF‐8/CNT flexible supercapacitor exhibits an energy density of 14 Wh kg^?1 with a power density of 89.3 W kg^?1, while the capacitance retention after 5000 cycles reaches 82%. This work provides an effective way to construct novel electrode materials with high energy storage density as well as good cycling performance and power density for high‐performance energy storage devices via the rational design.     

Highly Efficient and Ultrasensitive Large‐Area Flexible Photodetector Based on Perovskite Nanowires

Hybrid organic–inorganic perovskites have shown exceptional semiconducting properties and microstructural versatility for inexpensive, solution‐processable photovoltaic and optoelectronic devices. In this work, an all‐solution‐based technique in ambient environment for highly sensitive and high‐speed flexible photodetectors using high crystal quality perovskite nanowires grown on Kapton substrate is presented. At 10 V, the optimized photodetector exhibits a responsivity as high as 0.62 A W^?1, a maximum specific detectivity of 7.3 × 10¹² cm Hz^1/2 W^?1, and a rise time of 227.2 µs. It also shows remarkable photocurrent stability even beyond 5000 bending cycles. Moreover, a deposition of poly(methyl methacrylate) (PMMA) as a protective layer on the perovskite yields significantly better stability under ambient air operation: the PMMA‐protected devices are stable for over 30 days. This work demonstrates a cost‐effective fabrication technique for high‐performance flexible photodetectors and opens opportunities for research advancements in broadband and large‐scale flexible perovskite‐based optoelectronic devices.     

Low‐Voltage Photodetectors with High Responsivity Based on Solution‐Processed Micrometer‐Scale All‐Inorganic Perovskite Nanoplatelets

All‐inorganic photodetectors based on scattered CsPbBr₃ nanoplatelets with lateral dimension as large as 10 µm are fabricated, and the CsPbBr₃ nanoplatelets are solution processed governed by a newly developed ion‐exchange soldering mechanism. Under illumination of a 442 nm laser, the photoresponsivity of photodetectors based on these scattered CsPbBr₃ nanoplatelets is as high as 34 A W^?1, which is the largest value reported from all‐inorganic perovskite photodetectors with an external driven voltage as small as 1.5 V. Moreover, the rise and fall times are 0.6 and 0.9 ms, respectively, which are comparable to most of the state‐of‐the‐art all‐inorganic perovskite‐based photodetectors. All the material synthesis and device characterization are conducted at room temperature in ambient air. This work demonstrates that the solution‐processed large CsPbBr₃ nanoplatelets are attractive candidates to be applied in low‐voltage, low‐cost, ultra highly integrated optoelectronic devices.