Hole Accumulation Research Articles

Achieving pure-fluorescent color-tunable WOLED through long-range coupling of spatially separated electron–hole pairs

Abstract Color-tunable white organic light-emitting diode (CT-WOLED) with a wide correlated color temperature (CCT) offers numerous advantages in meeting human daily needs related to circadian rhythm. The study of CCT variation trends and the rules governing the expansion of the CCT range will help further improve the performance of such devices. This research proposes an effective strategy for achieving high-efficiency fluorescent CT-WOLEDs through long-range radiative coupling of spatially separated electron–hole pairs. After inserting a 5 nm thick DMAC-DPS layer between the donor (TAPC) and the acceptor (PO-T2T), the charge transfer excitons between TAPC and PO-T2T still exist. As the voltage increases, holes selectively undergo different photophysical processes, resulting in a wide CCT range. This demonstrates the extraordinary potential of spatially separated electron–hole pairs in regulating luminescent properties. By further introducing a bulk exciplex and the conventional red fluorescent dye DCJTB, the device’s efficiency, brightness, and CCT range have been further optimized. Additionally, significant highest occupied molecular orbital energy level difference between the hole transport layer TAPC and the spacer layer facilitates hole accumulation at the TAPC/spacer interface, thereby enhancing the long-range coupling effect. In device E, we achieved a wide CCT range of 2774 K along with a high external quantum efficiency of 9.2%. The results indicate that our proposed long-range coupling strategy not only enables a wide CCT range but also ensures broad spectral emission and high electroluminescence efficiency, providing new possibilities for the field of intelligent lighting.

Using the Transversal Admittance to Understand Organic Electrochemical Transistors.

The transient behavior of organic electrochemical transistors (OECTs) is complex due to mixed ionic-electronic properties that play a central role in bioelectronics and neuromorphic applications. Some works applied impedance spectroscopy in OECTs for understanding transport properties and the frequency-dependent response of devices. The transversal admittance (drain current vs gate voltage) is used for sensing applications. However, a general theory of the transversal admittance, until now, has been incomplete. The derive a model that combines electronic motion along the channel and vertical ion diffusion by insertion from the electrolyte, depending on several features as the chemical capacitance, the diffusion coefficient of ions, and the electronic mobility. Based on transport and charge conservation equations, it is shown that the vertical impedance produces a standard result of diffusion in intercalation systems, while the transversal impedance contains the electronic parameters of hole accumulation and transport along the channel. The spectral shapes of drain and gate currents and the complex admittance spectra are established by reference to equivalent circuit models for the vertical and transversal impedances, that describe well the measurements of a PEDOT:PSS OECT. New insights are provided to the determination of mobility by the ratio between drain and gate currents.

Efficient and Stable Quantum‐Dot Light‐Emitting Diodes with Trilayer PIN Architecture

AbstractAlthough the performance of quantum dot light‐emitting diodes (QLEDs) has been greatly improved in recent years, the multilayer device structure has become increasingly complex, limiting the practical application of QLEDs. Here, a novel trilayer PIN QLED with only three functional layers, which are Spiro‐OMeTAD:TFB bulk‐heterojunction (BHJ) hole transport layer (HTL), quantum‐dot emitting layer and ZnMgO electron transport layer is demonstrated. Due to the enhanced hole injection capability and suppressed electron leakage of Spiro‐OMeTAD:TFB BHJ HTL, the trilayer PIN QLED can show an excellent external quantum efficiency (EQE) of 25.1% and an impressive brightness of 299300 cd m−2 at only 8 V, which are significantly higher than those of conventional QLED. Moreover, the device stability is also remarkably improved due to the mitigation of hole accumulation and removal of unstable PEDOT:PSS. By using liquid alloy EGaIn as cathode, a fully solution‐processed vacuum‐free trilayer PIN QLED with a higher EQE of 27.3% can be further realized. The developed trilayer PIN QLEDs, with better performance and fewer functional layers, can promote the commercialization of QLED technology.

N‐ZrS3/p‐ZrOS Photoanodes with NiOOH/FeOOH Oxygen Evolution Catalysts for Photoelectrochemical Water Oxidation

AbstractPhotoelectrochemical water splitting offers a promising approach for carbon neutrality, but its commercial prospects are still hampered by a lack of efficient and stable photoelectrodes with earth‐abundant materials. Here, we report a strategy to construct an efficient photoanode with a coaxial nanobelt structure, comprising a buried‐ZrS3/ZrOS n−p junction, for photoelectrochemical water splitting. The p‐type ZrOS layer, formed on the surface of the n‐type ZrS3 nanobelt through a pulsed‐ozone‐treatment method, acts as a hole collection layer for hole extraction and a protective layer to shield the photoanode from photocorrosion. The resulting ZrS3/ZrOS photoanode exhibits light harvesting with good photo‐to‐current efficiencies across the whole visible region to over 650 nm. By further employing NiOOH/FeOOH as the oxygen evolution reaction cocatalyst, the ZrS3/ZrOS/NiOOH/FeOOH photoanode yields a photocurrent density of ~9.3 mA cm−2 at 1.23 V versus the reversible hydrogen electrode with an applied bias photon‐to‐current efficiency of ~3.2 % under simulated sunlight irradiation in an alkaline solution (pH=13.6). The conformal ZrOS layer enables ZrS3/ZrOS/NiOOH/FeOOH photoanode operation over 1000 hours in an alkaline solution without obvious performance degradation. This study, offering a promising approach to fabricate efficient and durable photoelectrodes with earth‐abundant materials, advances the frontiers of photoelectrochemical water splitting.

Vitalizing Perovskite Oxide-Based Acetone Sensors with Metal-Organic Framework-Derived Heterogeneous Oxide Catalysts.

Perovskite oxides are promising candidates for chemiresistive-type gas sensors owing to their exceptional thermal and chemical stability during solid-gas reactions. However, perovskites suffer from critical issues such as low surface area and poor surface activity, which negatively influence the sensing characteristics. While metal nanoparticles can be incorporated in perovskites to improve their reactivity, the fundamental incompatibility between catalytic metals and perovskite oxides often leads to substantial structural degradation as well as phase instability. Herein, we overcome this challenge through the introduction of an intermediary phase that forms coherent interfaces with both the perovskite phase and catalyst metals. Specifically, we present the case study of p-type La0.8Ca0.2Fe0.98Pt0.02O3 perovskite, whose hole accumulation layer was modulated by the incorporation of metal-organic framework (MOF)-derived n-type α-Fe2O3 nanoparticles decorated with highly dispersed Pt catalysts. The resulting composite exhibited significantly improved surface activity over the nonmodified La0.8Ca0.2FeO3 perovskite, leading to exceptional chemiresistive sensing performance toward acetone gas (Rg/Ra = 39.8 toward 10 ppm of acetone at 250 °C) with high cross-sensitivity against interfering gases. Importantly, our findings reaffirm the critical influence of interfacial engineering in facilitating surface chemical reactions on perovskite oxides and, by doing so, effectively provide a general synthetic guideline to the design of perovskite-based chemiresistors.

Sublimation and Recrystallization of CsPbBr3 Constructing a Perovskite-Carbon Interface to Facilitate Hole Transfer in Printable All-Inorganic Perovskite Solar Cells.

All-inorganic perovskite solar cells (APSCs) are a promising photovoltaic technology due to their unique physical and optical properties. For printable all-inorganic perovskite solar cells, the key factors limiting their photoelectric conversion performance are the crystallization of perovskite and the hole collection capability at the perovskite-carbon interface. In this study, leveraging the high-temperature tolerance of CsPbBr3 perovskite, the sublimation and recrystallization processes were controlled, significantly improving the crystalline quality of the perovskite and suppressing the generation of the nonphotovoltaic CsPb2Br5 phase. Furthermore, a continuous distribution of high-quality CsPbBr3 crystals was achieved at the interface between the carbon electrode and the zirconium oxide layer, ensuring efficient collection of photogenerated holes. The photoelectric conversion efficiency of the printable mesoscopic all-inorganic perovskite solar cell was increased from 5.04 to 8.34% (with a record value of 10.04%) and achieved an ultrahigh open-circuit voltage of 1.54 V due to the significant improvement in the crystal quality of CsPbBr3. This study proposes a novel strategy to enhance the photovoltaic conversion performance of carbon-based all-inorganic perovskite solar cells by suppressing the presence of nonphotovoltaic phases.

Configurational Isomerization‐Induced Orientation Switching: Non‐Fused Ring Dipodal Phosphonic Acids as Hole‐Extraction Layers for Efficient Organic Solar Cells

AbstractPhosphonic acid (PA) self‐assembled molecules have recently emerged as efficient hole‐extraction layers (HELs) for organic solar cells (OSCs). However, the structural effects of PAs on their self‐assembly behaviors on indium tin oxide (ITO) and thus photovoltaic performance remain obscure. Herein, we present a novel class of PAs, namely “non‐fused ring dipodal phosphonic acids” (NFR‐DPAs), featuring simple and malleable non‐fused ring backbones and dipodal phosphonic acid anchoring groups. The efficacy of configurational isomerism in modulating the photoelectronic properties and switching molecular orientation of PAs atop electrodes results in distinct substrate surface energy and electronic characteristics. The NFR‐DPA with linear (C2h symmetry) and brominated backbone exhibits favorable face‐on orientation and enhanced work function modification capability compared to its angular (C2v symmetry) and non‐brominated counterparts. This makes it versatile HELs in mitigating interfacial resistance for energy barrier‐free hole collection, and affording optimal active layer morphology, which results in an impressive efficiency of 19.11 % with a low voltage loss of 0.52 V for binary OSC devices and an excellent efficiency of 19.66 % for ternary OSC devices. This study presents a new dimension to design PA‐based HELs for high‐performance OSCs.

Microscopic analysis of low but stable perovskite solar cell device performance using electron spin resonance

Perovskite solar cells have attracted much attention as next-generation solar cells. However, a typical hole-transport material, spiro-OMeTAD, has associated difficulties including tedious synthesis and high cost. To overcome these shortcomings, an easily synthesized and low-cost hole-transport material has been developed: HND-2NOMe. Although HND-2NOMe has high local charge mobility because of the quasi-planar structure, its lower device performance is a weak point, the cause of which has not yet been clarified. Here, we analyse the source of the lower performance by clarifying the internal states from a microscopic viewpoint using electron spin resonance. We observe hole diffusion from perovskite to HND-2NOMe under dark conditions, indicating hole barrier formation at the perovskite/HND-2NOMe interface, leading to lower performance. Although such a barrier is formed, less hole accumulation for the HND-2NOMe-based cells under solar irradiation occurs, which is related to the stable performance. The sources of the lower but stable performance are crucially important for providing guidelines for improving the device performance.

Configurational Isomerization-Induced Orientation Switching: Non-Fused Ring Dipodal Phosphonic Acids as Hole-Extraction Layers for Efficient Organic Solar Cells.

Phosphonic acid (PA) self-assembled molecules have recently emerged as efficient hole-extraction layers (HELs) for organic solar cells (OSCs). However, the structural effects of PAs on their self-assembly behaviors on indium tin oxide (ITO) and thus photovoltaic performance remain obscure. Herein, we present a novel class of PAs, namely "non-fused ring dipodal phosphonic acids" (NFR-DPAs), featuring simple and malleable non-fused ring backbones and dipodal phosphonic acid anchoring groups. The efficacy of configurational isomerism in modulating the photoelectronic properties and switching molecular orientation of PAs atop electrodes results in distinct substrate surface energy and electronic characteristics. The NFR-DPA with linear (C2h symmetry) and brominated backbone exhibits favorable face-on orientation and enhanced work function modification capability compared to its angular (C2v symmetry) and non-brominated counterparts. This makes it versatile HELs in mitigating interfacial resistance for energy barrier-free hole collection, and affording optimal active layer morphology, which results in an impressive efficiency of 19.11 % with a low voltage loss of 0.52 V for binary OSC devices and an excellent efficiency of 19.66 % for ternary OSC devices. This study presents a new dimension to design PA-based HELs for high-performance OSCs.

A density functional study of type I to type II crossover in g-C3N4/CoN4 heterostructure in presence of external perturbation

Herein, we report the impact of external perturbation on the photocatalytic performance of g-C3N4/CoN4 heterojunction and concomitant transition from type-I to type-II. The state-of-the-art theoretical modeling presented here is the first study on dynamic role of strain and electric field on g-C3N4/CoN4 heterojunction and its potential application as a solar-driven water splitting reaction. Utilizing the density functional theory (DFT) calculation, V. N. et al. recently reported the photocatalytic activity of g-C3N4/MN4 (M = Mn, Fe and Co) heterojunction [J. Comput. Chem. 2024, 45, 2518-2529, https://doi.org/10.1002/jcc.2746412] and subsequently established g-C3N4/CoN4 as a type I heterojunction for photocatalytic water splitting reaction [Phys. Chem. Chem. Phys. 2024, 26, 21117–21133]. In the present study, we applied external perturbation in the form of mechanical strain, electric field and evaluated the electronic structure properties of the system along with the detailed examination of concomitant optical and magnetic properties of g-C3N4/CoN4 heterojunction. The switching of photocatalytic feature from type I to type II originates due to the crossover between valence band maxima (VBM) of g-C3N4 and CoN4 in presence of external perturbation. Notably, the resulting system acts as a type II photocatalyst for water splitting reaction while applying compressive (negative) strain of −2 to −6% and an electric field of −0.5 and +0.5 V/Å, respectively. Accumulation of photogenerated electrons and holes separately in g-C3N4 and CoN4 units confirms the perceptible separation of charge carriers and thereby reduces the recombination compared to un-perturbed system. A red-shifted absorption maximum (689 nm), superior charge transfer (0.9e), and clear separation of photogenerated electrons and holes are the origin of enhanced photocatalytic efficiency of g-C3N4/CoN4 heterojunction in the presence of external perturbation. We believe that our work will provide enough evidence to the experimentalists to achieve such a system in practice leading to human-friendly applications.

Transient Current Analysis of GaN Neutron Detector Based on the SRIM and TCAD Methods

Utilizing Technology Computer Aided Design (TCAD) software, this study determines the optimal thickness and doping concentration for the intrinsic gallium nitride (GaN) layer in a p-i-n GaN diode to improve detection efficiency and reliability. The study examines energy loss and the transient current response induced by alpha and 3H particles within the GaN p-i-n diode. Additionally, TCAD elucidates the transient current behavior arising from electron-hole pair generation, utilizing the Stopping and Range of Ions in Matter SRIM-2013 linear energy transfer distribution as a guide. The simulations disclose that the tailing effect in the transient current response results from radiation-induced hole accumulation. Elevated applied bias results in increased transient current pulse amplitude, attributed to an extended depletion region that boosts carrier collection. These insights are expected to drive advancements in GaN-based neutron detector technology, essential for advancing nuclear and space science applications in the next generation.

Research on the ultra-low temperature tensile deformation mechanism of Al-Mg-Si alloys in different heat treatment states

The susceptibility of Al-Mg-Si alloy to cracking during room temperature large plastic deformation poses a significant obstacle to its widespread application. Cryogenic temperature forming of aluminum alloys has emerged as a prominent research topic. However, the precise mechanisms underlying the enhancement of aluminum alloy plasticity in different states remain elusive. In order to elucidate this matter, a series of uniaxial tensile experiments were conducted on Al-Mg-Si alloy featuring diverse initial states, under varying temperature conditions. The results show that when the deformation temperature is reduced from 25℃ to −196℃, the tensile strength and elongation of the wrought material are increased by 48 MPa and 5.42 %, and the tensile strength and elongation of the annealed material are increased by 118 MPa and 5.65 %. In contrast, while the T4 state sample exhibited a significant improvement in tensile strength (103 MPa), no substantial enhancement in elongation was observed. This disparity can be primarily attributed to the absence of second-phase precipitation in the as-forged and annealed states. As the temperature decreased, the critical shear stress increased, resulting in increased resistance to deformation. Consequently, an increased degree of lattice rotation and activation of dislocations in various slip systems ensued, thereby improving the deformation uniformity. The formation of initial microvoids predominantly occurred close to grain boundaries. Therefore, compared with room temperature deformation, low temperature deformation caused by the accumulation of dislocations and hole sprouting concentrated at a single location was less likely. As a result, the dislocation distribution was more uniform and fracture was less likely to occur. Conversely, in the T4 state, the aging process resulted in the precipitation of a substantial amount of the soluble second phase (Mg5Si6). Consequently, microvoid nucleation transpired at the phase boundaries, leading to an elevated tensile strength. However, because of the increased dislocation hindrance when the deformation temperature was lowered, no significant enhancement in plasticity was observed.

Achieving High Doping Density in pH-neutral Conjugated Polyelectrolyte Toward Effective Hole-Transporting Materials for Organic Solar Cells.

The lack of effective and non-corrosive hole-transporting layer (HTL) materials has remained a long-standing issue that severely restricts the performance of organic solar cells (OSCs). Most pH-neutral conjugated polyelectrolytes (CPEs) exhibit inferior performance to the acid-doped HTL materials due to their low doping density. In this study, a series of pH-neutral CPEs is designed and synthesized with high doping density as HTL materials. Through an elaborate synthetic route, two sulfonate-terminating alkoxyl side chains can be introduced into thiophene, by which the electron-rich, highly soluble, and chemically stable thiophene monomer is synthesized to enable the subsequent polymerization. The CPE PTT-F exhibit a remarkable self-doping property with an enhanced doping density from 2.01 × 1017 to 7.02 × 1018 cm-3. The high work function and the increased doping density of PTT-F-based HTL decrease the depletion region width from 38.4 to 8.1nm at the anode interface, which minimized the energy loss in hole transport. Consequently, a binary OSC modified by PTT-F-based HTL achieve a high PCE of 18.8%. To the best of the knowledge, this is the highest PCE for OSC employing CPE-based HTL. The results from this work demonstrate an encouraging achievement of realizing exceptional hole collection ability in pH-neutral CPEs.

Magnetoelectric Phase Control at Domain‐Wall‐Like Epitaxial Oxide Multilayers

AbstractFerroelectric domain walls are nanoscale objects that can be created, positioned, and erased on demand. They often embody functional properties that are distinct from the surrounding bulk material. Enhanced conductivity, for instance, is observed at charged ferroelectric domain walls. Regrettably, domain walls of this type are scarce because of the energetically unfavorable electrostatics. This hinders the current technological development of domain‐wall nanoelectronics. Here this constraint is overcome by creating robust domain‐wall‐like objects in epitaxial oxide heterostructures. Charged head‐to‐head (HH) and tail‐to‐tail (TT) junctions are designed with two ferroelectric layers (BaTiO3 and BiFeO3) that have opposing out‐of‐plane polarization. To test domain‐wall‐like functionalities, an ultrathin ferromagnetic La0.7Sr0.3MnO3 layer is inserted into the junctions. The interfacial electron or hole accumulation at the interfaces, set by the HH and TT polarization configurations, respectively, controls the LSMO conductivity and magnetization. Thus it is proposed that trilayers reminiscent of artificial domain walls provide magnetoelectric functionality and may constitute an important building block in the design of oxide‐based electronic devices.

N-ZrS3/p-ZrOS Photoanodes with NiOOH/FeOOH Oxygen Evolution Catalysts for Photoelectrochemical Water Oxidation.

Photoelectrochemical water splitting offers a promising approach for carbon neutrality, but its commercial prospects are still hampered by a lack of efficient and stable photoelectrodes with earth-abundant materials. Here, we report a strategy to construct an efficient photoanode with a coaxial nanobelt structure, comprising a buried-ZrS3/ZrOS n-p junction, for photoelectrochemical water splitting. The p-type ZrOS layer, formed on the surface of the n-type ZrS3 nanobelt through a pulsed-ozone-treatment method, acts as a hole collection layer for hole extraction and a protective layer to shield the photoanode from photocorrosion. The resulting ZrS3/ZrOS photoanode exhibits light harvesting with good photo-to-current efficiencies across the whole visible region to over 650 nm. By further employing NiOOH/FeOOH as the oxygen evolution reaction cocatalyst, the ZrS3/ZrOS/NiOOH/FeOOH photoanode yields a photocurrent density of ~9.3 mA cm-2 at 1.23 V versus the reversible hydrogen electrode with an applied bias photon-to-current efficiency of ~3.2 % under simulated sunlight irradiation in an alkaline solution (pH=13.6). The conformal ZrOS layer enables ZrS3/ZrOS/NiOOH/FeOOH photoanode operation over 1000 hours in an alkaline solution without obvious performance degradation. This study, offering a promising approach to fabricate efficient and durable photoelectrodes with earth-abundant materials, advances the frontiers of photoelectrochemical water splitting.

Facet-Engineered BiVO4 Photocatalysts for Water Oxidation: Lifetime Gain Versus Energetic Loss.

A limiting factor to the efficiency of water Oxygen Evolution Reaction (OER) in metal oxide nanoparticle photocatalysts is the rapid recombination of holes and electrons. Facet-engineering can effectively improve charge separation and, consequently, OER efficiency. However, the kinetics behind this improvement remain poorly understood. This study utilizes photoinduced absorption spectroscopy to investigate the charge yield and kinetics in facet-engineered BiVO4 (F-BiVO4) compared to a non-faceted sample (NF-BiVO4) under operando conditions. A significant influence of preillumination on hole accumulation is observed, linked to the saturation and, thus, passivation of deep and inactive hole traps on the BiVO4 surface. In DI-water, F-BiVO4 shows a 10-fold increase in charge accumulation (∼5 mΔOD) compared to NF-BiVO4 (∼0.5 mΔOD), indicating improved charge separation and stabilization. With the addition of Fe(NO3)3, an efficient electron acceptor, F-BiVO4 demonstrates a 30-fold increase in the accumulation of long-lived holes (∼45 mΔOD), compared to NF-BiVO4 (∼1.5 mΔOD) and an increased half-time, from 2 to 10 s. Based on a simple kinetic model, this increase in hole accumulation suggests that facet-engineering causes at least a 50-100 meV increase in band bending in BiVO4 particles, thereby stabilizing surface holes. This energetic stabilization/loss results in a retardation of OER relative to NF-BiVO4. This slower catalysis is, however, offset by the observed increase in density and lifetime of photoaccumulated holes. Overall, this work quantifies how surface faceting can impact the kinetics of long-lived charge accumulation on metal oxide photocatalysts, highlighting the trade-off between lifetime gain and energetic loss critical to optimizing photocatalytic efficiency.

Enhancing Hot Carrier Photoelectric Efficiency through the Boosted Collection of Hot Holes via Au/ZrO2/Si Tunneling Junctions.

Metallic nanoparticles can generate photoexcited hot carriers on the femtosecond scale under light excitation, which holds immense significance for applications such as optical communication and ultrafast imaging. In this study, a tunnelling junction structure with ZrO2 as the dielectric layer is designed and fabricated to achieve efficient hot hole collection between Au nanoparticles and P-type Si. Through characterizations of photoconductive atomic force microscopy, the electrical transition from an ohmic contact to a tunneling junction is confirmed, and the transfer pathway of Au hot holes to P-type Si upon 520 nm excitation is clearly observed. The impact of the tunneling structure on device performance is investigated through the fabrication of Si/ZrO2/Au/TiO2 photodiodes. The performance tests show that hot hole collection by the tunneling effect significantly enhances a range of parameters, e.g., external quantum efficiency by 250%. Noticeably, the external quantum efficiency attributed to photogenerated hot carriers under 520 nm excitation is estimated to exceed 2.5%. Moreover, the transient photoresponse of the photodiodes is examined with a typical rising time of less than 20 ns.

Promoting effect of interfacial hole accumulation on photoelectrochemical water oxidation in BiVO4 and Mo-doped BiVO4

Hole transfer at the semiconductor-electrolyte interface is a key elementary process in (photo)electrochemical (PEC) water oxidation. However, up to now, a detailed understanding of the hole transfer and the influence of surface hole density on PEC water oxidation kinetics is lacking. In this work, we propose a model for the first time in which the surface accumulated hole density in BiVO4 and Mo-doped BiVO4 samples during water oxidation can be acquired via employing illumination-dependent Mott-Schottky measurements. Based on this model, some results are demonstrated as below: (1) Although the surface hole density increases when increasing light intensity and applied potential, the hole transfer rate remains linearly proportional to surface hole density on a log-log scale. (2) Both water oxidation on BiVO4 and Mo-doped BiVO4 follow first-order reaction kinetics at low surface hole densities, which is in good agreement with literature. (3) We find that water oxidation active sites in both BiVO4 and Mo-doped BiVO4 are very likely to be Bi5+, which are produced by photoexcited or/and electro-induced surface holes, rather than VOx species or Mo6+ due to their insufficient redox potential for water oxidation. (4) Introduction of Mo doping brings about higher OER activity of BiVO4, as it suppresses the recombination rate of surface holes and increases formation of Bi5+. This surface hole model offers a general approach for the quantification of surface hole density in the field of semiconductor photoelectrocatalysis.

Enhanced Performance and Stability of Perovskite Solar Cells Through Surface Modification with Benzocaine Hydrochloride.

Current development of inverted p-i-n perovskite solar cells (PSCs), with nickel oxide as the hole transport layer, is progressing toward lower net costs, higher efficiencies, and superior stabilities. Unfortunately, the high density of defect-based traps on the surface of perovskite films significantly limits the photoelectric conversion efficiency and operational stability of perovskite solar cells. Finding cost-effective interface modifiers is crucial for the further commercial development of p-i-n PSCs. In the present work, we report a passivation strategy using a multifunctional molecule, benzocaine hydrochloride (BHC), which is shown to reduce defect density and enhance the photovoltaic performance and stability of the resultant p-i-n PSCs. It has been revealed that BHC strongly interacts with perovskite precursor components and triggers the evolution of the perovskite absorber film morphology and enables improved surface energy level alignment, thus promoting charge carrier transport and extraction. These properties are beneficial for improving open-circuit voltage (VOC) and fill factor (FF). Our results show that the photoelectric conversion efficiency (PCE) of p-i-n PSCs with nickel oxide as the hole transport layer increased from an initial 20.0% to 22.1% after being passivated with BHC, and these passivated devices also exhibited improved stability. DFT calculations reveal the unusual ability of the BHC passivant to improve band alignment while also preventing the accumulation of holes at the interface. In this work, the advantages of BHC passivation are demonstrated by linking theoretical calculations with optical and electrical characterizations.

Bioinspired Flexible and Low-Voltage Organic Synaptic Transistors for UV Light-Driven Vision Systems.

Neuromorphic vision systems, particularly those stimulated by ultraviolet (UV) light, hold great potential applications in portable electronics, wearable technology, biological analysis, military surveillance, etc. Organic artificial synaptic devices hold immense potential in this field due to their ease of processing, flexibility, and biocompatibility. In this work, we have fabricated a flexible organic field-effect transistor (OFET) that utilizes chitosan-silver nanoparticles (AgNPs) composite material as the active dielectric material. During UV light illumination, both silver nanoparticles and the pentacene layer generate a large number of charge carriers. The photogenerated carriers lead to a more significant hole accumulation at the pentacene interface, resulting in a current rise. In the absence of light, the trapped electron in the silver nanoparticles persists for a longer duration, preventing the instant recombination with holes. This extended retention of electrons leads to the observed synaptic performance of the transistor. The use of aluminum oxide (Al2O3) as one of the dielectric layers enables the device to operate effectively at low voltage (<1 V). The device mimics various crucial synaptic properties of the brain, including short-term potentiation and long-term potentiation (STP and LTP), paired-pulse facilitation (PPF), spike-duration dependent plasticity (SDDP), spike-number dependent plasticity (SNDP), and spike-rate dependent plasticity (SRDP), etc. This work introduces an approach to develop flexible organic synaptic transistors that operate efficiently at low voltages, paving the way toward high-performance, UV light-driven neuromorphic vision systems.