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Salt Effect in Ion-Pair Dynamics after Bimolecular Photoinduced Electron Transfer in a Room-Temperature Ionic Liquid
摘要： Bimolecular photoinduced electron transfer between perylene and two quenchers was investigated in an imidazolium room-temperature ionic liquid (RTIL) and in a dipolar solvent mixture of the same viscosity using transient absorption on the subpicosecond to submicrosecond timescales. Whereas charge separation dynamics were similar in both solvents, significant differences were observed in the temporal evolution of the ensuing radical ions: although small, the free ion yield is significantly larger in the RTIL, and recombination of the ion pair to the triplet state of perylene is more efficient in the dipolar solvent. The temporal evolution of reactant, ion and triplet state populations could be well reproduced using Unified Encounter Theory. This analysis reveals that the observed differences can be explained by the strong screening of the Coulomb potential in the ion pair by the ionic solvent. In essence, RTILs favor free ions compared to highly dipolar solvents of the same viscosity.
关键词： unified encounter theory,free ions,spin conversion,charge recombination,transient absorption,charge separation
更新于2025-09-23 15:21:21
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Effects of Anisotropy Field and Easy Axis Dispersions on Squareness Ratio for HDDR-Processed Nd-Fe-B Powders
摘要： Nd-Fe-B magnetic powders produced by the hydrogenation-decomposition-desorption-recombination process have a lower squareness ratio than sintered magnets. In this paper, the anisotropy ?eld (Hk) distribution was assumed to be a horizontally ?ipped lognormal distribution and the effect of the Hk dispersion on the squareness ratio was investigated by using a micromagnetic simulator. As a result, the squareness ratio was very similar to the experimental demagnetization loop, when (cid:2)Hk(cid:3) was 5500 kA/m and σ Hk/(cid:2)Hk(cid:3) was 30%. Moreover, we investigated the easy axis dispersion of grains on squareness ratio in consideration of soft magnetic or nonmagnetic grain boundaries. As a result, the squareness ratio for the nonmagnetic grain boundary was closer to the experimental value; however, it is dif?cult to describe the experimental demagnetization loop by only considering the easy axis dispersion.
关键词： hydrogenation-decomposition-desorption-recombination (HDDR)-processed Nd-Fe-B,horizontally ?ipped lognormal distribution,Anisotropy ?eld and easy axis dispersions,squareness ratio
更新于2025-09-23 15:21:21
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Electron–hole correlations govern Auger recombination in nanostructures
摘要： The fast nonradiative decay of multiexcitonic states via Auger recombination is a fundamental process affecting a variety of applications based on semiconductor nanostructures. From a theoretical perspective, the description of Auger recombination in confined semiconductor nanostructures is a challenging task due to the large number of valance electrons and exponentially growing number of excited excitonic and biexcitonic states that are coupled by the Coulomb interaction. These challenges have restricted the treatment of Auger recombination to simple, noninteracting electron–hole models. Herein we present a novel approach for calculating Auger recombination lifetimes in confined nanostructures having thousands to tens of thousands of electrons, explicitly including electron–hole interactions. We demonstrate that the inclusion of electron–hole correlations are imperative to capture the correct scaling of the Auger recombination lifetime with the size and shape of the nanostructure. In addition, correlation effects are required to obtain quantitatively accurate lifetimes even for systems smaller than the exciton Bohr radius. Neglecting such correlations can result in lifetimes that are 2 orders of magnitude too long. We establish the utility of the new approach for CdSe quantum dots of varying sizes and for CdSe nanorods of varying diameters and lengths. Our new approach is the first theoretical method to postdict the experimentally known “universal volume scaling law” for quantum dots and makes novel predictions for the scaling of the Auger recombination lifetimes in nanorods.
关键词： semiconductor nanocrystals,quantum dots,excitons,auger recombination,biexcitons,nanorods
更新于2025-09-23 15:21:21
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Effective Photocatalytic Hydrogen Evolution by Cascadal Carrier Transfer in the Reverse Direction
摘要： Visible-light-responsive photocatalysts used in the highly efficient hydrogen production exhibit several disadvantages such as photocorrosion and fast recombination. Because of the potential important applications of such catalysts, it is crucial that a simple, effective solution is developed. In this respect, in this study, we combined SiC (β modification) and TiO2 with CdS to overcome the challenges of photocorrosion and fast recombination of CdS. Notably, we found that when irradiated with visible light, CdS was excited, and the excited electrons moved to the conduction band of TiO2, thereby increasing the efficiency of charge separation. In addition, by moving the holes generated on CdS to the valence band of SiC, in the opposite direction of TiO2, photocorrosion and fast recombination were prevented. As a result, in the sulfide solution, the CdS/SiC composite catalyst exhibited 4.3 times higher hydrogen generation ability than pure CdS. Moreover, this effect was enhanced with the addition of TiO2, giving 10.8 times higher hydrogen generation ability for the CdS/SiC/TiO2 catalyst. Notably, the most efficient catalyst, which was obtained by depositing Pt as a cocatalyst, exhibited 1.09 mmol g?1 h?1 hydrogen generation ability and an apparent quantum yield of 24.8%. Because water reduction proceeded on the TiO2 surface and oxidative sulfide decomposition proceeded on the SiC surface, the exposure of CdS to the solution was unnecessary, and X-ray photoelectron spectroscopy confirmed that photocorrosion was successfully suppressed. Thus, we believe that the effective composite photocatalyst construction method presented herein can also be applied to other visible-light-responsive powder photocatalysts having the same disadvantages as CdS, thereby improving the efficiency of such catalysts.
关键词： CdS,photocorrosion,hydrogen production,TiO2,photocatalysts,SiC,fast recombination
更新于2025-09-23 15:21:21
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Degradation of InGaN-based LEDs: Demonstration of a recombination-dependent defect-generation process
摘要： This paper provides insights into the degradation of InGaN-based LEDs by presenting a comprehensive analysis carried out on devices having two quantum wells (QWs) with different emission wavelengths (495 nm and 405 nm). Two different configurations are considered: one with the 495 nm QW closer to the p-side and one with the 495 nm QW closer to the n-side. The original results collected within this work indicate that (i) during stress, the devices show an increase in defect-related leakage both in reverse and low-forward voltage ranges: current increases with the square-root of stress time, indicating the presence of a diffusion process; (ii) stress induces a decrease in the luminescence signal emitted by both quantum wells: the drop in luminescence is stronger when measurements are carried out at low current levels, indicating that degradation is due to the generation of Shockley–Read–Hall recombination centers; (iii) remarkably, the degradation rate is linearly dependent on the luminescence signal emitted before stress by the well, indicating that carrier density impacts on degradation; and (iv) the optical degradation rate has a linear dependence on the stress current density. The results strongly suggest the existence of a recombination-driven degradation process: the possible role of Shockley–Read–Hall and Auger recombination is discussed. The properties of the defects involved in the degradation process are described through steady-state photocapacitance measurements.
关键词： quantum wells,Shockley–Read–Hall recombination,Auger recombination,degradation,steady-state photocapacitance,InGaN-based LEDs
更新于2025-09-23 15:21:01
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[IEEE 2019 IEEE 46th Photovoltaic Specialists Conference (PVSC) - Chicago, IL, USA (2019.6.16-2019.6.21)] 2019 IEEE 46th Photovoltaic Specialists Conference (PVSC) - Aqueous Solution Processed Copper Iodide as Hole Transport Material For Planar Inverted Perovskite Solar Cells
摘要： The inorganic carrier transport layers are robust and stable to the environment compared to the organic hole transport layer (HTL). Here, we report on the fabrication of the halide perovskite devices employing CuI as HTL and explored material properties and optoelectronic characterizations. The CuI device demonstrated the device efficiency of 14.1%. The film morphology of CuI is found to have the influence on the perovskite film growth and hence affected on the device parameters. The interface activation energy (EA) ~Eg suggests the recombination activities in the perovskite bulk is dominant. The capacitance analysis revealed the two trap centers of 0.527 eV and 0.332 eV in the perovskite bulk.
关键词： capacitance spectra,interface recombination,defect,copper iodide,halide perovskite
更新于2025-09-23 15:21:01
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Reducing Anomalous Hysteresis in Perovskite Solar Cells by Suppressing Interfacial Ferroelectric Order
摘要： Despite booming researches in organometal halide perovskite solar cells (PSCs) of recent years, considerable roadblocks remain for their large-scale deployment, ranging from undesirable current-voltage hysteresis to inferior device stability. Among various plausible origins of the hysteresis, interfacial ferroelectricity is particularly intriguing and warrants a close scrutiny. Here, we examine interfacial ferroelectricity in MAPbI3 (FAPbI3)/TiO2 and MAPbI3/PCBM heterostructures, and explore the correlations between the interfacial ferroelectricity and the hysteresis from the perspective of nonadiabatic electronic dynamics. It is found that ferroelectric order develops at the MAPbI3/TiO2 interface owing to the interaction between the polar MA ions and TiO2. The polarization switching of the MA ions under an applied gate field would result in drastically different rates in interfacial photoelectron injection and electron-hole recombination, contributing to the undesirable hysteresis. In a sharp contrast, ferroelectricity is suppressed at the FAPbI3/TiO2 and MAPbI3/PCBM interfaces, thanks to elimination of the interfacial electric field between perovskite and TiO2 via substitution of strong polar MA (dipole moment: 2.29 Debye) by weak polar FA ions (dipole moment: 0.29 Debye) and interface passivation, leading to consistent interfacial electronic dynamics and the absence of the hysteresis. The present work sheds light to the physical cause for hysteresis and points to the direction to which the hysteresis could be mitigated in PSCs.
关键词： Ferroelectricity,Hysteresis,Perovskite Solar Cells,Excited-state Electronic Dynamics,Electron-Hole Recombination,Orientation Selectivity
更新于2025-09-23 15:21:01
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Trap State and Charge Recombination in Nanocrystalline Passivized Conductive and Photoelectrode Interface of Dye-Sensitized Solar Cell
摘要： The dynamic competition between electron generation and recombination was found to be a bottleneck restricting the development of high-performance dye-sensitized solar cells (DSSCs). Introducing a passivation layer on the surface of the TiO2 photoelectrode material plays a crucial role in separating the charge by preventing the recombination of photogenerated electrons with the oxidized species. This study aims to understand in detail the kinetics of the electron recombination process of a DSSC fabricated with a conductive substrate and photoelectrode film, both passivized with a layer of nanocrystalline TiO2. Interestingly, the coating, which acted as a passivation layer, suppressed the back-electron transfer and improved the overall performance of the integrated DSSC. The passivation layer reduced the exposed site of the fluorine-doped tin oxide (FTO)–electrolyte interface, thereby reducing the dark current phenomenon. In addition, the presence of the passivation layer reduced the rate of electron recombination related to the surface state recombination, as well as the trapping/de-trapping phenomenon. The photovoltaic properties of the nanocrystalline-coated DSSC, such as short-circuit current, open-circuit voltage, and fill factor, showed significant improvement compared to the un-coated photoelectrode film. The overall performance efficiency improved by about 22% compared to the un-coated photoelectrode-based DSSC.
关键词： Electron recombination,electrochemical analysis,nanocrystalline coating,Dye-sensitized solar cell,passivation layer
更新于2025-09-23 15:21:01
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Performance analysis of c-Si heterojunction solar cell with passivated transition metal oxides carrier-selective contacts
摘要： Transition metal oxides (TMOs) as passivating carrier-selective contact layers are investigated for silicon heterojunction solar cells. MoOx as hole-selective layer and TiOx as an electron-selective layer are explored in detail to design a high-efficiency silicon heterojunction solar cell without any specified surface passivation layer. The thickness and optical transparency of the MoOx hole-selective layer have been evaluated through optical simulation. The impact of TMOs’ work function and their passivation quality has been examined in detail to extract the maximum conversion efficiency from silicon heterojunction solar cells. To increase the optical absorption in c-Si, the micro–nanopillar structure has also been implemented. It has been found that the barrier height at the TMO/silicon heterocontact plays a significant role in the overall performance improvement of the solar cell. The optimized cell design without doping and separate passivating layer can achieve a power conversion efficiency of ~ 22%. Our findings open the potential pathways and opportunities to obtain simplified heterojunction solar cells at lower temperatures and without impurity doping.
关键词： Surface recombination velocity,Carrier-selective contact layers,Transition metal oxides,c-Si heterojunction solar cells
更新于2025-09-23 15:21:01
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Surface Modification on Nanoripple-like ZnO Nanorod Arrays Using Two-dimensional (2D) Bi2OS2 to Fabricate High-Performance Inverted Polymer Solar Cells
摘要： In this paper, three-dimensional (3D) nanoripple-like ZnO nanorod arrays (R-ZnO NRAs) are successfully fabricated and modified by two-dimensional (2D) Bi2OS2 material, and inverted polymer solar cells (IPSCs) with R-ZnO modified by Bi2OS2 as electron transmission layer (ETL) are fabricated for the first time. The results show that the surface morphologies of R-ZnO NRAs can be controlled by adjusting the concentration of the modified 2D Bi2OS2 solution. Bi2OS2 modification can not only suppress the surface defects of R-ZnO NRAs, reduce the recombination of photogenerated charges, but also increase crystallinity of the active layer, resulting in effective electron collection. And thus, the performance of IPSCs is obviously improved. The power conversion efficiency (PCE) of PTB7: PCBM based PSCs with R-ZnO NRAs modified by 2% Bi2O2S as ETL is considerably raised to 7.31% from 5.51%. More interestingly, Bi2OS2 modification enhances IPSCs stability to remain 80.9% of their initial PCE after 80 days, yet IPSCs with pristine R-ZnO NRAs remain only 47.4% of their initial PCE. Moreover, this approach can also successfully improve the performance of another IPSC composed of PBDB-T: ITIC blends. The PCE of the device based on 2% Bi2OS2-modified R-ZnO NRAs is improved to 9.94% from 8.03% of the reference device without Bi2OS2 modification. This work not only provides an effective mean of surface modification of R-ZnO NRAs, but also shows the Bi2OS2 material has potential application in PSCs.
关键词： Recombination,Bi2OS2 nanosheets,Inverted polymer solar cells,Nanoripple-like ZnO nanorod arrays
更新于2025-09-23 15:21:01