ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Zhenwang Luo,Weisheng Wang,Junhui Wu,Guohua Ma,Yanna Hou,Cheng Yang,Xu Wang,Fei Zheng,Zhenfu Zhao,Ziqi Zhao,Liqiang Zhu,Ziyang Hu
The increasing computational demands of artificial intelligence (AI) algorithms are exceeding the capabilities of conventional computing architectures, creating a strong need for novel materials and paradigms. Memristors that integrate diverse resistive switching (RS) behaviors provide a promising avenue for developing novel computing architectures. In this study, we achieve the coexistence of volatile and nonvolatile RS behaviors in quasi-2D perovskite memristor (Q-2DPM). The Q-2DPM exhibits competitive performance as a nonvolatile memory. Multiple synaptic functions have been successfully simulated on Q-2DPM, such as excitatory postsynaptic currents, paired-pulse facilitation, and long-term potentiation/depression. Furthermore, artificial neural networks using Q-2DPM synapses achieve high accuracy in MNIST image classification tasks. The Q-2DPM’s inherent characteristics suitable for reservoir computing are also demonstrated through its application in a pulse-stream-based digital classification experiment, showcasing its impressive performance. The elucidation of the dual RS mechanisms within Q-2DPM provides fresh insights into memristor RS behavior and underscores the potential of achieving diverse computational units through a single device. This work paves the way for the implementation of physical neuromorphic hardware architectures and the advancement of sophisticated computational primitives, offering a significant step toward the next generation of computing technologies.
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NANO LETTERS
·
2024
·
IF 9.6
Yuan Qie,Hailong Hu,Kuibao Yu,Chao Zhong,Songman Ju,Yanbing Liu,Tailiang Guo,Fushan Li
The photolithographic patterning of fine quantum dot (QD) films is of great significance for the construction of QD optoelectronic device arrays. However, the photolithography methods reported so far either introduce insulating photoresist or manipulate the surface ligands of QDs, each of which has negative effects on device performance. Here, we report a direct photolithography strategy without photoresist and without engineering the QD surface ligands. Through cross-linking of the surrounding semiconductor polymer, QDs are spatially confined to the network frame of the polymer to form high-quality patterns. More importantly, the wrapped polymer incidentally regulates the energy levels of the emitting layer, which is conducive to improving the hole injection capacity while weakening the electron injection level, to achieve balanced injection of carriers. The patterned QD light-emitting diodes (with a pixel size of 1.5 μm) achieve a high external quantum efficiency of 16.25% and a brightness of >1.4 × 105 cd/m2. This work paves the way for efficient high-resolution QD light-emitting devices.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Tao Sun,Meng Qi,Qing-Xiu Li,Hang-Fei Li,Zhi-Peng Feng,Run-Ze Xu,You Zhou,Yu Wen,Gui-Jun Li,Ye Zhou,Su-Ting Han
Gait is among the most dependable, accurate, and secure methods of biometric identification. However, high power consumption and low computing capability are two major obstacles on wearable sensors-based gait recognition system. In this work, an integrated system is reported combining a triboelectric nanogenerator (TENG), a memristor (Ag/HfO x /Pt), and perovskite-based multicolor LEDs (PMCLED) for the visualization and recognition of foot patterns through signal-on-none and multi-wavelength on-device preprocessing. The flexible TENG acts as a sensory receptor, generating voltage based on the duration and intensity of pressure, which in turn promotes voltage-triggered synaptic plasticity in the memristor. The PMCLED, with its threshold switching and multi-wavelength emission characteristics, enables nonlinear filtering and amplification of the synaptic signal from the memristor, resulting in a simplified system design and reduced background noise. Additionally, the effectiveness of on-device preprocessing is validated based on a 5 × 5 array of integrated devices and software-built neural network for foot pattern visualization and recognition. The proposed system is able to recognize the on-device preprocessed images with high accuracy, indicating great potentials in both healthcare monitoring and human-machine interaction.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yongjun Wei,Feiping Lu,Xinqi Ai,Ju Lei,Yong Bai,Ziang Wei,Ziyin Chen
During the solution-based fabrication of perovskite solar cells (PSCs), the rapid and uncontrollable process of crystal nucleation and growth leads to the formation of numerous defects at the surface and grain boundaries, resulting in severe non-radiative recombination, which negatively affects the optoelectronic performance of the device. In this work, two passivation molecules, 2-(3-Pyridyl)-1H-benzimidazole (PBI) and 2-(3-Pyridyl)-1H-benzimidazole-6-carboxylic acid (PBI-CA), were introduced onto the surface of the perovskite film via a post-treatment method. PBI contains two basic functional groups, -C-N and -C N, where the nitrogen atom possesses a lone electron pair. PBI-CA has the same functional groups but also includes a carboxylic acid (-COOH) functional group, which contains both a carbonyl and a hydroxyl group, also having non-bonding electron pairs. The lone electron pairs in these functional groups exhibit Lewis base characteristics, which can coordinate with the uncoordinated Pb 2 + ions in the perovskite film, thereby passivating the ion defects caused by Pb 2+ . Compared to PBI alone, PBI-CA has an additional carboxylic acid group, providing more Lewis base sites, making it more effective in coordinating with Pb 2+ and passivating defects. We investigated the passivation mechanism of these two passivators through first-principles calculations and demonstrated their positive impact on PSCs through experiments and characterizations. The introduction of PBI and PBI-CA increased the size of the perovskite crystals, improved the power conversion efficiency (PCE), and enhanced device stability. The results showed that in a perovskite system with a bandgap of 1.6 eV, the PCE of the PBI-CA-modified device reached 21 %, higher than that of the PBI-modified device (20.3 %) and the baseline device (18.6 %), with significantly improved device stability. These Lewis base-containing molecules can be widely used to fabricate high-performance PSC devices.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Yuhan Deng,Yujie Yuan,Jian Ni,Lei Zheng,Jinlian Bi,Jia Guo,Rufeng Wang,Haoxuan Li,Shuai Zhang,Hongkun Cai,Jianjun Zhang
All-inorganic perovskite quantum dots (PQDs) have sparked a research boom due to their superior optoelectronic properties. However, current synthesis methods are complex and unsuitable for large-scale continuous production because the rapid reaction kinetics of quantum dots (QDs) make regulating their nucleation and growth challenging. Herein, we developed an efficient microfluidic technology using temperature-assisted base-acid ligand modulation to control the nucleation and growth of PQDs for mass fabrication. The obtained CsPbBr3 PQDs exhibited high dispersion, uniform sizes, and high photoluminescence quantum yield. Moreover, CsPbBr3 maintained high photoluminescence intensity for 120 min under UV irradiation, demonstrating good stability. These results provide a promising pathway for large-scale PQD production, which is crucial for advanced optoelectronic applications. Compared with the traditional hot injection (HI) and ligand-assisted reprecipitation (LARP) methods, microfluidic technology significantly saves materials and reagents. The microfluidic technology is also helpful for precisely controlling the nucleation process of QD growth.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Limin Lai,Guiyuan Liu,Yibo Zhou,Xiaoyu He,Ying Ma
Two-dimensional (2D) perovskites have been widely adopted for improving the performance and stability of three-dimensional (3D) metal halide perovskite devices. However, rational manipulation of the phase composition of 2D perovskites for suitable energy level alignment in 2D/3D perovskite photodetectors (PDs) has been rarely explored. Herein, we precisely controlled the dimensionality of the 2D perovskite on CsPbI2Br films by tuning the polarity of the n-butylammonium iodide (BAI)-based solvents. In comparison to the pure n = 1 2D perovskite (ACN-BAI) formed by acetonitrile treatment, a mixture of n = 1 and n = 2 phases (IPA-BAI) generated by isopropanol (IPA) treatment guaranteed more robust defect passivation and favorable energy level alignment at the perovskite/hole transport layer interface. Consequently, the IPA-BAI PD exhibited a responsivity of 0.41 A W–1, a detectivity of 1.01 × 1013 Jones, and a linear dynamic range of 120 dB. Furthermore, the mixed-phase 2D layer effectively shielded the 3D perovskite from moisture. The IPA-BAI device retained 76% of its initial responsivity after 500 h of nonencapsulated storage at 10% relative humidity. This research provides valuable insights into the dimensional modulation of 2D perovskites for further enhancing the performance of 2D/3D perovskite PDs.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Mingze Sun,Ying Chen,Shubing Tian,Mingming Zhang,Haokun Jiang,Kang Liu,Jixiang Xu,Fangxu Dai,Lei Wang,Zhongmin Zhou,Jun Xing
Quasi−2D perovskite films with multiple quantum well structures can provide a large Stokes shift and efficient photoluminescence (PL), which have great potential in the application of luminescent solar concentrators (LSCs). However, its low photoelectric conversion efficiency and poor stability remain obstacles to commercial application. Here, a multifunctional molecule additive octyltriphenylphosphonium bromide is introduced to prepare high-quality perovskite LSCs. The multifunctional molecule can simultaneously passivate perovskite cations and anions, reducing the defect sites and improving the photoluminescence quantum yield (PLQY) of the perovskite nanocrystals. Triphenylphosphine groups with high steric hindrance effect can hinder ion migration; the hydrophobic properties of the long alkyl chain prevent water erosion, which together improves the stability of the perovskite films. The multifunctional molecule passivated perovskite film has a high PLQY of 100% and retains 96% of the initial PL intensity after 30 days of indoor storage. The perovskite LSC device achieves a maximum optical efficiency of 6.5% at a geometric factor of 3.1. The findings open a new way to boost the performance of perovskite-based LSCs.
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Materials Today Communications
·
2024
·
IF 3.7
Xiao Wang,Jinghua Zhou,Cui Zhang,Chaofan Zheng,Qing Zhang,Bei Liu,Zelin Jia,Tao Xue,Kunping Guo,Jin Huang,Fanghui Zhang
Fully inorganic metal halide perovskite solar cells (PSCs) exhibit high efficiency and excellent thermal stability. However, the presence of surface traps caused by oxygen vacancies in the electron transport layer leads to significant non-radiative charge recombination, which limits both the short-circuit current density ( J SC ) and photoelectric conversion efficiency (PCE). In this study, we propose a dual-purpose strategy by incorporating the multifunctional organic salt dopamine hydrochloride (DACl) as an additive into the electron transport layer. Firstly, DACl acts as a Lewis base when added to TiO 2 films, facilitating improvements in electron transport properties and resulting in higher photovoltaic quality of subsequently deposited perovskite layers. This enhancement significantly improves overall photovoltaic performance . Secondly, DACl's electron-rich aromatic structure and -NH 2 functional group can anchor undercoordinated Pb 2+ ions and passivate defects within the perovskite film. Additionally, its -OH functional group and charged ion Cl - play crucial roles in improving perovskite grain size and crystallinity . As a result of these modifications, cell efficiency increased ∼35 %, from 9.37 % to 12.70 %, while short-circuit current density increased from 15.44 mA cm −2 to 17.80 mA cm −2 at an illumination intensity of 100 mW cm −2 . These findings suggest that introducing DACl into the ETL layer is a promising approach for achieving efficient and stable PSCs.
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Nanoscale
·
2024
·Vol. 16
·期 8
·4148-4156
·
IF 5.8
Qing Dai,Zhenwang Luo,Guohua Ma,Yuchen Miao,Xu Wang,Zhenfu Zhao,Feiyu Zhao,Fei Zheng,Liqiang Zhu,Ziyang Hu
The escalating interest in low-dimensional perovskites stems from their tunable optoelectronic traits and robust stability. The pursuit of multifaceted optoelectronic devices holds substantial importance for energy-efficient and space-constrained systems. This investigation showcases the realization of multifunctional two-dimensional perovskite solar cells, incorporating transient light detection and resistive switching functions within a single device, achievable by facile external bias adjustments. Serving as a photodetector, the device exhibits commendable self-powered photodetection attributes, including an exceptionally low dark current density of 1 nA mm−2, a remarkable specific detectivity of 7.67 × 1012 Jones, a swift response time of 0.60 μs, and an expansive linear dynamic range of 72 dB. As a memristor, it showcases enduring performance across 4 × 102 cycles, a substantial on/off ratio of 106, and a rapid operation time of less than 1 μs. This endeavor unveils a pioneering avenue for advancing high-performance, air-stable multifunctional two-dimensional perovskite electronics.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Meng Yan,Liu Yu-Qin,Wang Chao,Si Yang,Wang Yun-Jie,Xia Wen-Qi,Liu Tian,Cao Xu,Guo Zhi-Yan,Chen Jie-Jie,Li Wen-Wei
The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites and the intensive oxidant consumption still severely restrict the decontamination performance. While nanoconfinement of SACs allows drastically enhanced decontamination reaction kinetics, the detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment of reactants, the catalytic pathway shift is also an important cause for the reactivity enhancement of nanoconfined SACs. The surface electronic structure of cobalt site is altered by confining it within the nanopores of mesostructured silica particles, which triggers a fundamental transition from singlet oxygen to electron transfer pathway for 4-chlorophenol oxidation. The changed pathway and accelerated interfacial mass transfer render the nanoconfined system up to 34.7-fold higher pollutant degradation rate and drastically raised peroxymonosulfate utilization efficiency (from 61.8% to 96.6%) relative to the unconfined control. It also demonstrates superior reactivity for the degradation of other electron-rich phenolic compounds, good environment robustness, and high stability for treating real lake water. Our findings deepen the knowledge of nanoconfined catalysis and may inspire innovations in low-carbon water purification technologies and other heterogeneous catalytic applications.
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Advanced Energy Materials
·
2024
·
IF 24.4
Xuchao Guo,Zhiqin Ying,Xin Li,Meili Zhang,Shiqian Su,Jingming Zheng,Haojiang Du,Yihan Sun,Jun Wu,Linhui Liu,Yuheng Zeng,Xi Yang,Jichun Ye
Inverted perovskite solar cells (IPSCs) suffer from significant non-radiative recombination losses at the defective perovskite/C 60 interface, limiting the efficiency and stability of perovskite/silicon tandem solar cells. Despite silicon oxide (SiO X ) being a common passivation material in the silicon industry with higher electron selectivity than conventional atomic layer-deposited alumina, its application in IPSCs is limited by its tendency to damage sensitive perovskite during processing. Here, an oblique angle evaporation method is developed to deposit a conformal, ultra-thin SiO X layer without damaging the underlying perovskite. This SiO X interlayer not only chemically passivates under-coordinated Pb 2+ defects but also forms an n/n+ homojunction that provides effective field-effect passivation, concurrently reducing recombination and enhancing electron selectivity. As a result, extending this strategy to two-terminal monolithic perovskite/tunnel oxide passivating contact silicon tandem solar cells achieves a stabilized power conversion efficiency of 30.2%, representing one of the highest efficiencies reported for such tandems. More importantly, the robust inorganic nature of SiO X enables it to serve as a dense inner encapsulation, enhancing both light (ISOS-L-1) and thermal (ISOS-D-2I) device stabilities.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yuetian Du,Dong Wang
Although considerable progress has been made in developing different types of vitrimers, ongoing challenges remain in tuning their mechanical and rheological properties, self-healing, and adhesion. Here, we demonstrate a one-pot method to produce a novel double-network epoxy vitrimer using an aliphatic amine cross-linker with a siloxane covalent bond and an aromatic amine cross-linker with a disulfide covalent bond. When a controlled two-stage curing process is employed, the markedly different reactivities of aliphatic amine and aromatic amine with epoxy allow for sequential cross-linked network formation, leading to the development of a double network that incorporates two types of dynamic covalent bonds. As a result, the produced vitrimers exhibit controllable mechanical, thermal, and rheological properties, as well as recyclability. This is evidenced by a tensile strength as high as 72 MPa, while maintaining ∼10% elongation at break, a wide glass-transition temperature range from 91 to 171 °C, and an adjustable two-stage stress relaxation. These characteristics suggest opportunities to develop high-performance cross-linked polymers with specific responses to time and temperatures.
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