Efficient Infrared Solar Cells Employing Quantum Dot Solids with Strong Inter-Dot Coupling and Efficient Passivation

Lead chalcogenide quantum dot (QD) infrared (IR) solar cells are promising devices for breaking through the theoretical efficiency limit of single-junction solar cells by harvesting the low-energy IR photons that cannot be utilized by common devices. However, the device performance of QD IR photovoltaic is limited by the restrictive relation between open-circuit voltages (V_OC) and short circuit current densities (J_SC), caused by the contradiction between surface passivation and electronic coupling of QD solids. Here, a strategy is developed to decouple this restriction via epitaxially coating a thin PbS shell over the PbSe QDs (PbSe/PbS QDs) combined with in situ halide passivation. The strong electronic coupling from the PbSe core gives rise to significant carrier delocalization, which guarantees effective carrier transport. Benefited from the protection of PbS shell and in situ halide passivation, excellent trap-state control of QDs is eventually achieved after the ligand exchange. By a fine control of the PbS shell thickness, outstanding IR J_SC of 6.38 mA cm⁻² and IR V_OC of 0.347 V are simultaneously achieved under the 1100 nm-filtered solar illumination, providing a new route to unfreeze the trade-off between V_OC and J_SC limited by the photoactive layer with a given bandgap.     

Core/Shell Quantum Dots Solar Cells

Semiconductor nanocrystals, the so‐called quantum dots (QDs), exhibit versatile optical and electrical properties. However, QDs possess high density of surface defects/traps due to the high surface‐to‐volume ratio, which act as nonradiative carrier recombination centers within the QDs, thereby deteriorating the overall solar cell performance. The surface passivation of QDs through the growth of an outer shell of different materials/compositions called “core/shell QDs” has proven to be an effective approach to reduce the surface defects and confinement potential, which can enable the broadening of the absorption spectrum, accelerate the carrier transfer, and reduce exciton recombination loss. Here, the recent research developments in the tailoring of the structure of core/shell QDs to tune exciton dynamics so as to improve solar cell performance are summarized. The role of band alignment of core and shell materials, core size, shell thickness/compositions, and interface engineering of core/thick shell called “giant” QDs on electron–hole spatial separation, carrier transport, and confinement potential, before and after grafting on the carrier scavengers (semiconductor/electrolyte), is described. Then, the solar cell performance based on core/shell QDs is introduced. Finally, an outlook for the rational design of core/shell QDs is provided, which can further promote the development of high‐efficiency and stable QD sensitized solar cells.     

PbSe/PbS and PbSe/PbSexS1–x Core/Shell Nanocrystals

The synthesis of PbSe/PbS and PbSe/PbSe_xS_1–x core/shell nanocrystals (NCs) with luminescence quantum efficiencies of 45–55 % is reported. PbSe/PbS NCs are prepared via a two‐stage process, while the PbSe/PbSe_xS_1–x NCs are formed in a single‐stage procedure. The core/shell NCs exhibit an energy tuning of the exciton transitions, with respect to that of the core NC, that is dependent on the core diameter, shell thickness, and composition.     

Photoelectrochemically Active and Environmentally Stable CsPbBr3/TiO2 Core/Shell Nanocrystals

Inherent poor stability of perovskite nanocrystals (NCs) is the main impediment preventing broad applications of the materials. Here, TiO₂ shell coated CsPbBr₃ core/shell NCs are synthesized through the encapsulation of colloidal CsPbBr₃ NCs with titanium precursor, followed by calcination at 300 °C. The nearly monodispersed CsPbBr₃/TiO₂ core/shell NCs show excellent water stability for at least three months with the size, structure, morphology, and optical properties remaining identical, which represent the most water‐stable inorganic shell passivated perovskite NCs reported to date. In addition, TiO₂ shell coating can effectively suppress anion exchange and photodegradation, therefore dramatically improving the chemical stability and photostability of the core CsPbBr₃ NCs. More importantly, photoluminescence and (photo)electrochemical characterizations exhibit increased charge separation efficiency due to the electrical conductivity of the TiO₂ shell, hence leading to an improved photoelectric activity in water. This study opens new possibilities for optoelectronic and photocatalytic applications of perovskites‐based NCs in aqueous phase.     

p‐Si/SnO2/Fe2O3 Core/Shell/Shell Nanowire Photocathodes for Neutral pH Water Splitting

Silicon is one of the promising materials for solar water splitting and hydrogen production; however, it suffers from two key factors, including the large external potential required to drive water splitting reactions at its surface and its instability in the electrolyte. In this study, a successful fabrication of novel p‐Si/n‐SnO₂/n‐Fe₂O₃ core/shell/shell nanowire (css‐NW) arrays, consisting of vertical Si NW cores coated with a thin SnO₂ layer and a dense Fe₂O₃ nanocrystals (NCs) shell, and their application for significantly enhanced solar water reduction in a neutral medium is reported. The p‐Si/n‐SnO₂/n‐Fe₂O₃ css‐NW structure is characterized in detail using scanning, transmission, and scanning transmission electron microscopes. The p‐Si/n‐SnO₂/n‐Fe₂O₃ css‐NWs show considerably improved photocathodic performances, including higher photocurrent and lower photocathodic turn‐on potential, compared to the bare p‐Si NWs or p‐Si/n‐SnO₂ core/shell NWs (cs‐NWs), due to increased optical absorption, enhanced charge separation, and improved gas evolution. As a result, photoactivity at 0 V versus reversible hydrogen electrode and a low onset potential in the neutral solution are achieved. Moreover, p‐Si/n‐SnO₂/n‐Fe₂O₃ css‐NWs exhibit long‐term photoelectrochemical stability due to the Fe₂O₃ NCs shell well protection. These results reveal promising css‐NW photoelectrodes from cost‐effective materials by facile fabrication with simultaneously improved photocathodic performance and stability.     

溶剂添加剂对体异质结太阳能电池的影响

体异质结太阳电池因其高效率特点受到了研究者的极大关注.使用添加剂DIO应用于MEH-PPV:PCBM结构中,改善活性层形貌.最终得到了在DIO浓度为20 mg/ml的时候器件短路电流密度最大(Jsc=8.74 mA/cm2),器件效率最高(PCE=2.44％),相比没有使用DIO的情况效率提升了55.4％.     

Polymer selection toward efficient polymer/PbSe planar heterojunction hybrid solar cells

By using a series of polymers in the polymer/PbSe planar heterojunction hybrid solar cells (HSCs), we found that the open circuit voltage of HSCs showed a great improvement compared to that of PbSe Schottky junction solar cells, which might be attributed to the formation of interface dipole, resulting in decreased interfacial resistance, increased built-in electrical field, as well as reduced exciton recombination at interface. Meanwhile, polymers with higher PL quenching have more favorable hole transfer which lead to better device performance. In addition, the energy levels and surface energy of the polymers might largely affect their interaction with PbSe NCs, leading to different interfacial morphologies and influencing the charge transfer efficiency. Furthermore, the optimized HSCs showed a remarkable PCE of 5.31% which was the highest efficiency reported for polymer/PbSe based HSCs. We believe this HSC efficiency can be further improved by selecting polymers with rationally designed structures.     

PbS/Cu2O异质结的制备和性能表征

采用电化学沉积法在酸性电解液中制备n型Cu2O薄膜,并对其进行Cl掺杂,制备Cu2O-Cl结构.然后利用连续离子吸附法在样品薄膜上复合PbS量子点.通过SEM和UV-vis对样品进行表征,并对样品的光电化学性能进行了测试.结果表明,未掺杂的Cu2O对PbS量子点的吸附能力较强一些,经PbS敏化后的样品在太阳光谱的吸收拓展到了近红外区,PbS/Cu2O和PbS/Cu2O-Cl复合结构的光电化学性能均有所增加,尤其是短路电流密度.PbS复合后的样品转换效率最高仅为0.67％,主要原因是两者能级的不匹配,形成异质结时引入界面态,得不到理想的转换效率.     

高效率n-nc-Si∶H/p-c-Si异质结太阳能电池

采用热丝化学气相沉积技术(HWCVD),系统地研究了纳米晶硅层(尤其是本征缓冲层)的晶化度以及晶体硅表面氢处理时间对nc-Si∶H/c-Si异质结太阳能电池性能的影响,通过C-V和C-F测试分析了不同氢处理时间和本征缓冲层氢稀释度对nc-Si∶H/c-Si界面缺陷态的影响,运用高分辨透射电镜观察了不同的本征缓冲层晶化度的nc-Si∶H/c-Si异质结太阳能电池的界面,优化工艺参数,在p型CZ晶体硅衬底上制备出转换效率为17.27%的n-nc-Si∶H/i-nc-Si∶H/p-c-Si异质结电池.     

高效率n-nc-Si:H/p-c-Si异质结太阳能电池

采用热丝化学气相沉积技术(HWCVD),系统地研究了纳米晶硅层(尤其是本征缓冲层)的晶化度以及晶体硅表面氢处理时间对nc-Si∶H/c-Si异质结太阳能电池性能的影响,通过C-V和C-F测试分析了不同氢处理时间和本征缓冲层氢稀释度对nc-Si∶H/c-Si界面缺陷态的影响,运用高分辨透射电镜观察了不同的本征缓冲层晶化度的nc-Si∶H/c-Si异质结太阳能电池的界面,优化工艺参数,在p型CZ晶体硅衬底上制备出转换效率为17.27%的n-nc-Si∶H/i-nc-Si∶H/p-c-Si异质结电池.     

Soft Core/Shell Packages for Stretchable Electronics

This paper presents materials and core/shell architectures that provide optimized mechanical properties in packages for stretchable electronic systems. Detailed experimental and theoretical studies quantitatively connect the geometries and elastic properties of the constituent materials to the overall mechanical responses of the integrated systems, with a focus on interfacial stresses, effective modulus, and maximum extent of elongation. Specific results include core/shell designs that lead to peak values of the shear and normal stresses on the skin that remain less than 10 kPa even for applied strains of up to 20%, thereby inducing minimal somatosensory perception of the device on the human skin. Additional, strain‐limiting mesh structures embedded in the shell improve mechanical robustness by protecting the active components from strains that would otherwise exceed the fracture point. Demonstrations in precommercial stretchable electronic systems illustrate the utility of these concepts.     

Localized Surface Plasmon Enhanced All‐Inorganic Perovskite Quantum Dot Light‐Emitting Diodes Based on Coaxial Core/Shell Heterojunction Architecture

This work presents a strategy of combining the concepts of localized surface plasmons (LSPs) and core/shell nanostructure configuration in a single perovskite light‐emitting diode (PeLED) to addresses simultaneously the emission efficiency and stability issues facing current PeLEDs' challenges. Wide bandgap n‐ZnO nanowires and p‐NiO are employed as the carrier injectors, and also the bottom/upper protection layers to construct coaxial core/shell heterostructured CsPbBr₃ quantum dots LEDs. Through embedding plasmonic Au nanoparticles into the device and thickness optimization of the MgZnO spacer layer, an emission enhancement ratio of 1.55 is achieved. The best‐performing plasmonic PeLED reaches up a luminance of 10 206 cd m^?2, an external quantum efficiency of ≈4.626%, and a current efficiency of 8.736 cd A^?1. The underlying mechanisms for electroluminescence enhancement are associated with the increased spontaneous emission rate and improved internal quantum efficiency induced by exciton–LSP coupling. More importantly, the proposed PeLEDs, even without encapsulation, present a substantially improved operation stability against water and oxygen degradation (30‐day storage in air ambient, 85% humidity) compared with any previous reports. It is believed that the experimental results obtained will provide an effective strategy to enhance the performance of PeLEDs, which may push forward the application of such kind of LEDs.     

Merocyanine/C60 Planar Heterojunction Solar Cells: Effect of Dye Orientation on Exciton Dissociation and Solar Cell Performance

In this study the charge dissociation at the donor/acceptor heterointerface of thermally evaporated planar heterojunction merocyanine/C₆₀ organic solar cells is investigated. Deposition of the donor material on a heated substrate as well as post‐annealing of the complete devices at temperatures above the glass transition temperature of the donor material results in a twofold increase of the fill factor. An analytical model employing an electric‐field‐dependent exciton dissociation mechanism reveals that geminate recombination is limiting the performance of as‐deposited cells. Fourier‐transform infrared ellipsometry shows that, at temperatures above the glass transition temperature of the donor material, the orientation of the dye molecules in the donor films undergoes changes upon annealing. Based on this finding, the influence of the dye molecules’ orientations on the charge‐transfer state energies is calculated by quantum mechanical/molecular mechanics methods. The results of these detailed studies provide new insight into the exciton dissociation process in organic photovoltaic devices, and thus valuable guidelines for designing new donor materials.     

染料敏化纳米晶TiO2太阳能电池

介绍了染料敏化纳米晶TiO2太阳能电池的结构,工作原理,技术指标以及TiO2纳米膜的制备方法.阐述了敏化纳米晶太阳能电池相比于硅太阳电池的低成本及优于其它光电化学电池的关键技术.讨论了影响NPC电池总的光电转换效率的因素,并对有机染料和无机染料光敏化剂的选择及染料的敏化问题进行了论述,在此基础上提出了将其商业化的一些值得深入研究和需要解决的问题.     

Characteristics of Polyaniline/Si Heterojunction Solar Cell By Electrochemical Dye Sensitization

Using the electrochemical polymerization dye sensitization （ECDS） method, polyaniline （PAn）, which is used as top region material in solar cells, is sensitized with direct blue dye（DS）, and sensitized Al grid/DS-PAn/n-Si/Al heterojunction solar cells is prepared by ECDS. Influences of the ECDS on the absorption spectrum and the junction characteristics of the solar cell were discussed, and the output characteristics were measured. The results show that the absorption spectrum of the sensitized PAn films is much wider and stronger in Vis-range; the diode quality factor is about 6.3 and the height of latent barrier potential of p-n junction is 0.89 eV; the short-circuit current and the conversion efficiency of sensitized DS- PAn/Si heterojunction solar cells are greatly improved, which the short-circuit current can increase 6 times, the fill factor is 57% and the efficiency can reach 1.42 % under the illumination of 37.2 W/m^2 , respectively.     

用于四结太阳电池的多对TiO2/SiO2减反膜系的研究

随着GaInP/GaInAs/GaInNAs/Ge四结太阳电池的快速发展,设计并镀制可与四结太阳电池更加匹配的光学减反膜系变得尤为重要.实验中通过TFCale软件理论模拟了3对TiO2/SiO2(6层)减反膜系,其中理论模拟膜系与实际镀制膜系反射率曲线重合性良好.实际制备并讨论了离子源功率、薄膜物理厚度等参数对减反膜系反射率的影响.发现得到优异反射率的关键在于对第二层SiO2薄膜物理厚度的控制,尤其是在400～1 000 nm波段内.实验中制备的3对TiO2/SiO2(6层)减反膜系在280～1 400 nm波段内其反射率均小于10％,特别是在影响四结太阳电池限流结的GaInAs/GaInNAs两结波段(670～900 nm/900～1 100 nm)内,其反射率均在5％以下.     

Ambient Stable and Efficient Monolithic Tandem Perovskite/PbS Quantum Dots Solar Cells via Surface Passivation and Light Management Strategies

Here, highly efficient and stable monolithic (2-terminal (2T)) perovskite/PbS quantum dots (QDs) tandem solar cells are reported, where the perovskite solar cell (PSC) acts as the front cell and the PbS QDs device with a narrow bandgap acts as the back cell. Specifically, ZnO nanowires (NWs) passivated by SnO₂ are employed as an electron transporting layer for PSC front cell, leading to a single cell PSC with maximum power conversion efficiency (PCE) of 22.15%, which is the most efficient NWs-based PSCs in the literature. By surface passivation of PbS QDs by CdCl₂, QD devices with an improved open-circuit voltage and a PCE of 8.46% (bandgap of QDs: 0.92 eV) are achieved. After proper optimization, 2T and 4T tandem devices with stabilized PCEs of 17.1% and 21.1% are achieved, respectively, where the 2T tandem device shows the highest efficiency reported in the literature for this design. Interestingly, the 2T tandem cell shows excellent operational stability over 500 h under continuous illumination with only 6% PCE loss. More importantly, this device without any packaging depicts impressive ambient stability (almost no change) after 70 days in an environment with controlled 65% relative humidity, thanks to the superior air stability of the PbS QDs.     

有机薄膜太阳电池的研究进展

有机薄膜太阳电池作为一种新型光伏电池,近年来得到了迅猛发展。其制备工艺简单、价格低廉、柔性、质轻,为人类解决能源问题提供了一种崭新的途径。文章综述了近年来有机薄膜太阳电池的发展状况,结合有机薄膜太阳电池的发展历史,分析了单异质结、体异质结和叠层三种典型结构器件的工作原理和研究成果,探讨了各种器件结构的优缺点,并对有机薄膜太阳电池的发展趋势作了展望。     

Core/Shell Metal Halide Perovskite Nanocrystals for Optoelectronic Applications

Core/shell structured metal halide perovskite nanocrystals (NCs) are emerging as a type of material with remarkable optical and electronic properties. Research into this field has been developing and expanding rapidly in recent years, with significant advances in the studies of the shell growth mechanism and in understanding of properties of these materials. Significant enhancement of both the stability and the optical performance of core/shell perovskite NCs are of particular importance for their applications in optoelectronic technologies. In this review, the recent advances in core/shell structured perovskite NCs are summarized. The band structures and configurations of core/shell perovskite NCs are elaborated, the shell classification and shell engineering approaches, such as perovskites and their derivative shells, semiconductor shell, oxide shell, polymer shell, etc. are reviewed, and the shell growth mechanisms are discussed. The prospective of these NCs in lighting and displays, solar cells, photodetectors, and other devices is discussed in the light of current knowledge, remaining challenges, and future opportunities.