Two-Dimensional Van Der Waals Thin Film and Device.

In the rapidly evolving field of thin-film electronics, the emergence of large-area flexible and wearable devices has been a significant milestone. Although organic semiconductor thin films, which can be manufactured through solution processing, have been identified, their utility is often undermined by their poor stability and low carrier mobility under ambient conditions. However, inorganic nanomaterials can be solution-processed and demonstrate outstanding intrinsic properties and structural stability. In particular, a series of two-dimensional (2D) nanosheet/nanoparticle materials have been shown to form stable colloids in their respective solvents. However, the integration of these 2D nanomaterials into continuous large-area thin with precise control of layer thickness and lattice orientation still remains a significant challenge. This review paper undertakes a detailed analysis of van der Waals thin films, derived from 2D materials, in the advancement of thin-film electronics and optoelectronic devices. The superior intrinsic properties and structural stability of inorganic nanomaterials are highlighted, which can be solution-processed and underscor the importance of solution-based processing, establishing it as a cornerstone strategy for scalable electronic and optoelectronic applications. A comprehensive exploration of the challenges and opportunities associated with the utilization of 2D materials for the next generation of thin-film electronics and optoelectronic devices is presented.

Efficient Tin-Lead Perovskite Solar Cells with a Ultrawide Usage Windows of Precursor Solution Opened by SnF2.

High quality tin-lead perovskite solar cells (Sn─Pb PSCs) can be fabricated via simple solution processing methods. However, the instability of precursor solutions and their narrow usage windows still pose challenges in manufacturing efficient and reproducible Sn─Pb PSCs, hindering the commercialization of PSCs. Fluorine tin (SnF2) is widely used as an antioxidant to improve the crystallinity of perovskite. In this study, another role of SnF2 as a stabilizer is found to restrain the deprotonation of methylammonium iodide (MAI) in the precursor solution, which improves their stability and expands their usage windows. Due to the inhibition of SnF2 on oxidation and deprotonation, stable large-sized colloidal clusters form gradually in perovskite precursor solution during aging, leading to uniform nucleation/crystallization during film growth, significantly reducing the roughness and defect density in the films. Because of the competitive deprotonation and oxidation process of Sn2+, the benefit of larger cluster maximizes after about ten days storage of precursor solution. The champion efficiency of Sn─Pb PSCs prepared with 10 days aged precursor solution is 22.00%. High performance of devices fabricated with precursor solution stored for even ≈40 days discloses the wide usage windows of precursor solution with SnF2 additive.

Interfacial engineering with ultrathin poly (9,9-di-n-octylfluorenyl-2,7-diyl) (PFO) layer for high efficient perovskite light-emitting diodes.

Organic-inorganic hybrid perovskites have attracted great attention in the field of lighting and display due to their very high color purity and low-cost solution-process. Researchers have done a lot of work in realizing high performance electroluminescent devices. However, the current efficiency (CE) of methyl-ammonium lead halide perovskite light-emitting diodes (PeLEDs) still needs to be improved. Herein, we demonstrate the enhanced performance of PeLEDs through introducing an ultrathin poly(9,9-di-n-octylfluorenyl-2,7-diyl) (PFO) buffer layer between poly(3,4-ethylendioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and CH3NH3PbBr3 perovskite. Compared to the reference device without PFO, the optimal device luminous intensity, the maximum CE, and the maximum external quantum efficiency increases from 8139 cd m-2 to 30 150 cd m-2, from 7.20 cd A-1 (at 6.8 V) to 10.05 cd A-1 (at 6.6 V), and from 1.73% to 2.44%, respectively. The ultrathin PFO layer not only reduces the exciton quenching at the interface between the hole-transport layer and emission layer, but also passivates the shallow-trap ensure increasing hole injection, as well as increases the coverage of perovskite film.

High-Efficiency Perovskite Solar Cells Based on New TPE Compounds as Hole Transport Materials: The Role of 2,7- and 3,6-Substituted Carbazole Derivatives.

In this work, four tetraphenylethylene (TPE)-centered hole transport materials (HTMs), with 2,7- or 3,6-substituted carbazole derivatives as periphery groups are deliberately synthesized and characterized. Their photophysical properties, energy levels, and photovoltaic performances are systematically investigated, and their performances as HTMs are discussed with respect to the different substituent positions on the carbazole moiety. It is interesting to find that the TPE-based HTMs with 2,7-carbazole substituents rival the 3,6-carbazole substituents in hole mobility and hole extraction ability. A high power conversion efficiency of up to 16.74 % is achieved for the devices based on the 2,7-carbazole periphery arms, which is even higher than the one of the "star" HTM Spiro-OMeTAD (2,2-7,7-tetrakis(N,N'-diparamethoxy-phenylamine 9,9'-spirobifluorene) under the same conditions. As far as we know, this is the highest efficiency achieved in tetraphenylethylene derivatives.

Hydrogen-peroxide-modified egg albumen for transparent and flexible resistive switching memory.

Egg albumen is modified by hydrogen peroxide with concentrations of 5%, 10%, 15% and 30% at room temperature. Compared with devices without modification, a memory cell of Ag/10% H2O2-egg albumen/indium tin oxide exhibits obviously enhanced resistive switching memory behavior with a resistance ratio of 104, self-healing switching endurance for 900 cycles and a prolonged retention time for a 104 s @ 200 mV reading voltage after being bent 103 times. The breakage of massive protein chains occurs followed by the recombination of new protein chain networks due to the oxidation of amidogen and the synthesis of disulfide during the hydrogen peroxide modifying egg albumen. Ions such as Fe3+, Na+, K+, which are surrounded by protein chains, are exposed to the outside of protein chains to generate a series of traps during the egg albumen degeneration process. According to the fitting results of the double logarithm I-V curves and the current-sensing atomic force microscopy (CS-AFM) images of the ON and OFF states, the charge transfer from one trap center to its neighboring trap center is responsible for the resistive switching memory phenomena. The results of our work indicate that hydrogen- peroxide-modified egg albumen could open up a new avenue of biomaterial application in nanoelectronic systems.

m-Methoxy Substituents in a Tetraphenylethylene-Based Hole-Transport Material for Efficient Perovskite Solar Cells.

Three tetrapheynlethylene derivatives (N,N-di(4-methoxyphenyl)aminophenyl-substituted tetraphenylethylene; TPE-4DPA) with different methoxy positions (pp-, pm-, and po-) have been synthesized and characterized. The methoxy groups can control the oxidation potential of the materials, and the electronic properties of the derivatives were affected by the position of the methoxy substituents. These compounds were synthesized in a facile and cost-effective way, and were applied as hole-transport materials in perovskite solar cells. The corresponding cell performances were compared with respect to their structure modifications, and it was found that the derivative with m-OMe substituents showed the highest power conversion efficiency (PCE) of 15.4 %, with a Jsc value of 20.04 mA cm-2 , a Voc value of 1.07 V, and a fill factor (FF) value of 0.72, which is higher than the p-OMe and o-OMe substituents. Moreover, the PCE of pm-TPE-4DPA is comparable with that of the state-of-the-art 2,2',7,7'-tetrakis(N,N'-di-p-methoxyphenylamine)-9,9'-spirobifluorene under identical conditions.

High-efficiency inverted polymer solar cells controlled by the thickness of polyethylenimine ethoxylated (PEIE) interfacial layers.

In this work, we investigate the effect of the thickness of the polyethylenimine ethoxylated (PEIE) interface layer on the performance of two types of polymer solar cells based on inverted poly(3-hexylthiophene) (P3HT):phenyl C61-butryric acid methyl ester (PCBM) and thieno[3,4-b]thiophene/benzodithiophene (PTB7):[6,6]-phenyl C71-butyric acid methyl ester (PC71BM). Maximum power conversion efficiencies of 4.18% and 7.40% were achieved at a 5.02 nm thick PEIE interface layer, for the above-mentioned solar cell types, respectively. The optimized PEIE layer provides a strong enough dipole for the best charge collection while maintaining charge tunneling ability. Optical transmittance and atomic force microscopy measurements indicate that all PEIE films have the same high transmittance and smooth surface morphology, ruling out the influence of the PEIE layer on these two parameters. The measured external quantum efficiencies for the devices with thick PEIE layers are quite similar to those of the optimized devices, indicating the poor charge collection ability of thick PEIE layers. The relatively low performance of devices with a PEIE layer of thickness less than 5 nm is the result of a weak dipole and partial coverage of the PEIE layer on ITO.

Chelating Dual Interface for Efficient and Stable Crystal Growth and Iodine Defect Management in Sn-Pb Perovskite Solar Cells.

Suppressing Sn2+ oxidation and rationally controlling the crystallization process of tin-lead perovskite (Sn-Pb PVK) films by suitable bonding methods have emerged as key approaches to achieving efficient and stable Sn-Pb perovskite solar cells (PSCs). Herein, the chelating coordination is performed at the top and bottom interfaces of Sn-Pb PVK films. The chelation strength is stronger toward Sn2+ than Pb2+ by introducing oligomeric proanthocyanidins (OPC) at the bottom interface. This difference in chelation strength resulted in a spontaneous gradient distribution of Sn/Pb within the perovskite layer during crystallization, particularly enhancing the enrichment of Sn2+ at the bottom interface and facilitating the extraction and separation of photogenerated charge carriers in PSCs. Simultaneously, this top-down distribution of gradually increasing Sn content slowed down the crystallization rate of Sn-Pb PVK films, forming higher-quality films. On the top interface of the PVK, trifluoroacetamidine (TFA) was used to inhibit the generation of iodine vacancies (VI) through chelating with surface-uncoordinated Pb2+/Sn2+, further passivating defects while suppressing the oxidation of Sn2+. Ultimately, the PSCs with simultaneous chelation at both top and bottom interfaces achieved a power conversion efficiency (PCE) of 23.31% and an open-circuit voltage (VOC) exceeding 0.90 V. The stability of unencapsulated target devices in different environments also improved.

Photocurrent generation through electron-exciton interaction at the organic semiconductor donor/acceptor interface.

In this work, we report our effort to understand the photocurrent generation that is contributed via electron-exciton interaction at the donor/acceptor interface in organic solar cells (OSCs). Donor/acceptor bi-layer heterojunction OSCs, of the indium tin oxide/copper phthalocyanine (CuPc)/fullerene (C60)/molybdenum oxide/Al type, were employed to study the mechanism of photocurrent generation due to the electron-exciton interaction, where CuPc and C60 are the donor and the acceptor, respectively. It is shown that the electron-exciton interaction and the exciton dissociation processes co-exist at the CuPc/C60 interface in OSCs. Compared to conventional donor/acceptor bi-layer OSCs, the cells with the above configuration enable holes to be extracted at the C60 side while electrons can be collected at the CuPc side, resulting in a photocurrent in the reverse direction. The photocurrent thus observed is contributed to primarily by the charge carriers that are generated by the electron-exciton interaction at the CuPc/C60 interface, while charges derived from the exciton dissociation process also exist at the same interface. The mechanism of photocurrent generation due to electron-exciton interaction in the OSCs is further investigated, and it is manifested by the transient photovoltage characteristics and the external quantum efficiency measurements.

Full hardware implementation of neuromorphic visual system based on multimodal optoelectronic resistive memory arrays for versatile image processing.

In-sensor and near-sensor computing are becoming the next-generation computing paradigm for high-density and low-power sensory processing. To fulfil a high-density and efficient neuromorphic visual system with fully hierarchical emulation of the retina and visual cortex, emerging multimodal neuromorphic devices for multi-stage processing and a fully hardware-implemented system with versatile image processing functions are still lacking and highly desirable. Here we demonstrate an emerging multimodal-multifunctional resistive random-access memory (RRAM) device array based on modified silk fibroin protein (MSFP), exhibiting both optoelectronic RRAM (ORRAM) mode featured by unique negative and positive photoconductance memory and electrical RRAM (ERRAM) mode featured by analogue resistive switching. A full hardware implementation of the artificial visual system with versatile image processing functions is realised for the first time, including ORRAM mode array for the in-sensor image pre-processing (contrast enhancement, background denoising, feature extraction) and ERRAM mode array for near-sensor high-level image recognition, which hugely improves the integration density, and simply the circuit design and the fabrication and integration complexity.

An Inverted Perovskite Solar Cell with Good Comprehensive Performance Realized by Reducing the Concentration of Precursors.

Inverted perovskite solar cells (PSCs) exhibit great potential for industrial application thanks to their low complexity and low fabrication temperature. Aiming at commercial applications, it is necessary to comprehensively consider the material consumption and its corresponding electrical performance. Here, a simple strategy has been proposed to obtain inverted PSCs with comprehensive performance, that is, reaching an acceptable electrical performance by reducing the usage of perovskite. More precisely, the inverted PSCs, whose perovskite film is prepared by 1.0 M precursor, yields a power conversion efficiency (PCE) of 15.50%, fulfilling the requirement for real commercial application. In addition, the thickness of the electron transport layer (C60 in this work) in the above inverted PSCs was further optimized by comparing the simulated absorption spectrum, J-V characteristics and impedance with three different thicknesses of C60 layer. More excitingly, the optimized device displays high storage stability which maintains more than 90% of its initial PCE for 28 days. Therefore, our work provides a simple and cost-effective method to reach good comprehensive performance of inverted PSCs for commercial applications.

Dual Function Modification of Cs2CO3 for Efficient Perovskite Solar Cells.

Organic-inorganic hybrid perovskite solar cells (PeSCs) attract much attention in the field of solar cells due to their excellent photovoltaic performance. Many efforts have been devoted to improving their power conversion efficiency (PCE). However, few works focus on simultaneously improving their electrical and optical property. Herein, a simple strategy is proposed to improve the PCE from 19.8% of a reference device to 22.9%, by utilizing cesium carbonate (Cs2CO3) to modify indium tin oxide (ITO) substrate. The insertion of a Cs2CO3-modification layer between ITO substrate and SnO2 electron transport layer simultaneously offers two benefits: improving the electron extraction capability and adjusting the light field distribution in the device. The optical optimization effect of Cs2CO3 revealed in this work has not been reported before. This work provides a new and simple strategy to obtain high performance PeSCs by improving the electrical and optical properties of the devices at the same time.

Multiphotoconductance Levels of the Organic Semiconductor of Polyimide-Based Memristor Induced by Interface Charges.

A memristor with Au/polyimide (PI)/Au structure is prepared by magnetron sputtering to investigate the multiphotoconductance resistive switching (RS) memory behavior. The PI-based memristor presents stable bipolar RS memory and is sensitive to visible light. Four discrete conductance states in both high-resistance state (HRS) and low-resistance state (LRS) are obtained when illuminating by 365, 550, 590, and 780 nm light. Electron trapping and detrapping from the defects distributed at interfaces and the PI switching layer are responsible for the observed RS memory behavior. The enhanced trapping and detrapping process by light illumination is responsible for the multiconductance states. This work provides the possibility for further development of neuromorphic vision sensors using an organic semiconductor-based memristor.

Phase control of quasi-2D perovskite thin films by adding MAPbI3 in the precursor solution.

Quasi two-dimensional (Q-2D) perovskite cells have attracted much attention due to their excellent stability compared to their 3D counterparts. However, the Q-2D perovskite thin films prepared by the solution method have been confirmed to be a mixture of small-n phases and large-n phases instead of a pure phase, where the amount and distribution of these phases have a great significance on the performance of Q-2D perovskite solar cells. Here, commercialized 3D perovskite powder was simply added to an ACI perovskite precursor solution to get a uniform and closely connected heterostructure in which the large-n phases can work as pathways for charge transfer. The characterization results of the films and devices show that the appropriate amount of MAPbI3 in the precursor solution could distribute the 3D phases homogeneously within the final film to promote the photovoltaic performance of the devices. Consequently, the power conversion efficiency of the Q-2D ACI perovskite solar cell has been increased from 10.4% to 13.82% (with a 32.8% performance improvement).

Ag/HfOx/Pt Unipolar Memristor for High-Efficiency Logic Operation.

Unipolar resistive switching (URS) behavior, known as the SET and RESET operating in a single voltage sweep direction, has shown great potential in the simplification of the peripheral circuit. The URS memristor always involves complicated interfacial engineering and structural design. In this work, a reliable URS behavior is realized using a simple Ag/HfOx/Pt memristor structure. The memristor displays a retention time of >104 s, an ON/OFF ratio of >103, and a good operation voltage. Synergy and competition between the Ag conductive filament formed by redox reaction and the migration of an oxygen vacancy are responsible for the observed URS. By comparison, a 35% power consumption is reduced during the logical operation from 0 to 1 to 0. The operation strategy is demonstrated by exhibiting the ACSII code of the capital letter denoted by eight logic states. This work provides a low-power concept for ultrahigh data storage using the URS memristor.

Simultaneous Passivation of Bulk and Interface Defects with Gradient 2D/3D Heterojunction Engineering for Efficient and Stable Perovskite Solar Cells.

Minimizing bulk and interfacial nonradiative recombination losses is key to further improving the photovoltaic performance of perovskite solar cells (PSC) but very challenging. Herein, we report a gradient dimensionality engineering to simultaneously passivate the bulk and interface defects of perovskite films. The 2D/3D heterojunction is skillfully constructed by the diffusion of an amphiphilic spacer cation from the interface to the bulk. The 2D/3D heterojunction engineering strategy has achieved multiple functions, including defect passivation, hole extraction improvement, and moisture stability enhancement. The introduction of tertiary butyl at the spacer cation should be responsible for increased film and device moisture stability. The device with 2D/3D heterojunction engineering delivers a promising efficiency of 22.54% with a high voltage of 1.186 V and high fill factor of 0.841, which benefits from significantly suppressed bulk and interfacial nonradiative recombination losses. Moreover, the modified devices demonstrate excellent light, thermal, and moisture stability over 1000 h. This work paves the way for the commercial application of perovskite photovoltaics.

Second-order associative memory circuit hardware implemented by the evolution from battery-like capacitance to resistive switching memory.

Memristor-based Pavlov associative memory circuit presented today only realizes the simple condition reflex process. The secondary condition reflex endows the simple condition reflex process with more bionic, but it is only demonstrated in design and involves the large number of redundant circuits. A FeO x -based memristor exhibits an evolution process from battery-like capacitance (BLC) state to resistive switching (RS) memory as the I-V sweeping increase. The BLC is triggered by the active metal ion and hydroxide ion originated from water molecule splitting at different interfaces, while the RS memory behavior is dominated by the diffusion and migration of ion in the FeO x switching function layer. The evolution processes share the nearly same biophysical mechanism with the second-order conditioning. It enables a hardware-implemented second-order associative memory circuit to be feasible and simple. This work provides a novel path to realize the associative memory circuit with the second-order conditioning at hardware level.

Multi-functional Strategy: Ammonium Citrate-Modified SnO2 ETL for Efficient and Stable Perovskite Solar Cells.

The tin oxide (SnO2) electron transport layer (ETL) plays a crucial role in perovskite solar cells (PSCs). However, the heterogeneous dispersion of commercial SnO2 colloidal precursors is far from optimized, resulting in dissatisfied device performance with SnO2 ETL. Herein, a multifunctional modification material, ammonium citrate (TAC), is used to modify the SnO2 ETL, bringing four benefits: (1) due to the electrostatic interaction between TAC molecules and SnO2 colloidal particles, more uniformly dispersed colloidal particles are obtained; (2) the TAC molecules distributed on the surface of SnO2 provide nucleation sites for the perovskite film growth, promoting the vertical growth of the perovskite crystal; (3) TAC-doped SnO2 shows higher electron conductivity and better film quality than pristine SnO2 while offering better energy-level alignment with the perovskite layer; and (4) TAC has functional groups of C═O and N-H containing lone pair electrons, which can passivate the defects on the surface of SnO2 and perovskite films through chemical bonding and inhibit the device hysteresis. In the end, the device based on TAC-doped ETL achieved an increased power conversion efficiency (PCE) of 21.58 from 19.75% of the reference without such treatment. Meanwhile, the PSCs using the TAC-doped SnO2 as the ETL maintained 88% of their initial PCE after being stored for about 1000 h under dark conditions and controlled RH of 10-25%.

Influence of Temperature on Exciton Dynamic Processes in CuPc/C60 Based Solar Cells.

Although the effect of high temperature on the performance of organic solar cells has been widely investigated, it is inevitably influenced by the associated annealing effect (which usually leads to film morphology change and variation in electrical properties), which makes the discussion more sophisticated. In this study, we simplified the issue and investigated the influence of low temperatures (from room temperature to 77 K) on the photocurrent and internal/external quantum efficiency of a CuPc/C60 based solar cell. We found that besides the charge dynamic process (charge transport), one or more of the exciton dynamic processes, such as exciton diffusion and exciton dissociation, also play a significant role in affecting the photocurrent of organic solar cells at different temperatures. Additionally, the results showed that the temperature had negligible influence on the absorption of the CuPc film as well as the exciton generation process, but obviously influenced the other two exciton dynamic processes (exciton diffusion and exciton dissociation).

ABO3 multiferroic perovskite materials for memristive memory and neuromorphic computing.

The unique electron spin, transfer, polarization and magnetoelectric coupling characteristics of ABO3 multiferroic perovskite materials make them promising candidates for application in multifunctional nanoelectronic devices. Reversible ferroelectric polarization, controllable defect concentration and domain wall movement originated from the ABO3 multiferroic perovskite materials promotes its memristive effect, which further highlights data storage, information processing and neuromorphic computing in diverse artificial intelligence applications. In particular, ion doping, electrode selection, and interface modulation have been demonstrated in ABO3-based memristive devices for ultrahigh data storage, ultrafast information processing, and efficient neuromorphic computing. These approaches presented today including controlling the dopant in the active layer, altering the oxygen vacancy distribution, modulating the diffusion depth of ions, and constructing the interface-dependent band structure were believed to be efficient methods for obtaining unique resistive switching (RS) behavior for various applications. In this review, internal physical dynamics, preparation technologies, and modulation methods are systemically examined as well as the progress, challenges, and possible solutions are proposed for next generation emerging ABO3-based memristive application in artificial intelligence.