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.     

Synergistic Passivation and Down-Conversion by Imidazole-Modified Graphene Quantum Dots for High Performance and UV-Resistant Perovskite Solar Cells

Organic–inorganic hybrid perovskite solar cells (PVSCs) have achieved stunning progress during the past decade, which has inspired great potential for future commercialization. However, tin dioxide (SnO₂) as a commonly used electron transport layer with varied defects and energy level mismatch with perovskite contributes to the energy loss and limitation of charge extraction. Herein, imidazole-modified graphene quantum dots (IGQDs) are introduced as the interlayer, which plays a significant role in three aspects: 1) dually passivating the defects of SnO₂ and buried interface of perovskite by first-principles calculations; 2) accelerating the carrier extraction and transfer owing to ideal band alignment; and 3) improving light utilization through down-conversion proved by light intensity measurement. Consequently, the devices based on IGQDs/SnO₂ not only exhibit the champion power conversion efficiency (PCE) of 24.11%, but display a significantly enhanced ultraviolet (UV) stability retaining about 81% of their initial PCEs after continuous UV irradiation (365 nm, 20 mW cm⁻²) for 300 h. Moreover, the unencapsulated modified device remains 82% after storing for 1650 h in air (20–30 °C, RH 45–55%). This work furnishes a novel method for the combination of interfacial passivation and photon management, which holds out for the prospect of employment in other optoelectronic applications.     

Efficiency Enhanced Hybrid Solar Cells Using a Blend of Quantum Dots and Nanorods

The cell performance of organic‐inorganic hybrid photovoltaic devices based on CdSe nanocrystals and the semiconducting polymer poly[2,6‐(4,4‐bis(2‐ethylhexyl)‐4H‐cyclopenta[2,1‐b;3,4‐b′]‐dithiophene)‐alt‐4,7‐(2,1,3‐benzothiadiazole)] (PCPDTBT) is strongly dependent on the applied polymer‐to‐nanocrystal loading ratio and the annealing temperature. It is shown here that higher temperatures for the thermal annealing step have a beneficial impact on the nanocrystal phase by forming extended agglomerates necessary for electron percolation to enhance the short‐circuit current. However, there is a concomitant reduction of the open‐circuit voltage, which arises from energy‐level alterations of the organic and the inorganic component. Based on quantum dots and PCPDTBT, we present an optimized organic–inorganic hybrid system utilizing an annealing temperature of 210 °C, which provides a maximum power conversion efficiency of 2.8%. Further improvement is obtained by blending nanocrystals of two different shapes to compose a favorable n‐type network. The blend of spherical quantum dots and elongated nanorods results in a well‐interconnected pathway for electrons within the p‐type polmer matrix, yielding maximum efficiencies of 3.6% under simulated AM 1.5 illumination.     

InAs/GaAs量子点中间带太阳电池的理论研究与优化

从荧光粉散射机理分析了LED器件色角向分布不均匀的形成原因,提出了一种利用逐点步进光学设计方法,实现了不同入射角度内蓝光光程相等的远荧光粉层结构。应用该方法设计了使用不同折射率载体的LED远荧光粉层光学结构。模拟结果显示,应用所设计的光学形状的远荧光粉层结构,相比传统平面荧光粉层结构,75°方向光斑边缘与中心法线方向色差du′v′从0.05降低到0.01左右,色温偏移降低了43%~98%不等,有效改善了白光LED远程荧光粉封装结构的色度均匀性。该设计不需要增加或改变封装工艺手段,工业生产实现简单,额外成本很少,具有较强的实际应用价值。 更多还原     

InAs/GaAs量子点中间带太阳电池的理论研究与优化

基于InAs/GaAs量子点中间带太阳电池(QD-IBSC)结构和载流子漂移扩散理论建立了计算电流密度与静电势的数学模型,从理论上分析了量子点中间带太阳电池的电压电流特性,定量讨论了量子点层厚度、温度以及n型掺杂对电压电流特性的影响.模拟结果表明:在i层厚度取400 nm时转化效率达到最大值14.01％;温度会对量子点中间带太阳电池的电压电流特性产生影响,温度在300～350 K范围内,开路电压Voc随温度的升高而明显减小,短路电流Jsc几乎不变;对i区进行n型掺杂会抑制量子点层发挥作用.     

Realistic Detailed Balance Study of the Quantum Efficiency of Quantum Dot Solar Cells

An attractive but challenging technology for high efficiency solar energy conversion is the intermediate band solar cell (IBSC), whose theoretical efficiency limit is 63%, yet which has so far failed to yield high efficiencies in practice. The most advanced IBSC technology is that based on quantum dots (QDs): the QD‐IBSC. In this paper, k·p calculations of photon absorption in the QDs are combined with a multi‐level detailed balance model. The model has been used to reproduce the measured quantum efficiency of a real QD‐IBSC and its temperature dependence. This allows the analysis of individual sub‐bandgap transition currents, which has as yet not been possible experimentally, yielding a deeper understanding of the failure of current QD‐IBSCs. Based on the agreement with experimental data, the model is believed to be realistic enough to evaluate future QD‐IBSC proposals.     

Cation‐Exchange Synthesis of Highly Monodisperse PbS Quantum Dots from ZnS Nanorods for Efficient Infrared Solar Cells

Infrared solar cells that utilize low‐bandgap colloidal quantum dots (QDs) are promising devices to enhance the utilization of solar energy by expanding the harvested photons of common photovoltaics into the infrared region. However, the present synthesis of PbS QDs cannot produce highly efficient infrared solar cells. Here, a general synthesis is developed for low‐bandgap PbS QDs (0.65–1 eV) via cation exchange from ZnS nanorods (NRs). First, ZnS NRs are converted to superlattices with segregated PbS domains within each rod. Then, sulfur precursors are released via the dissolution of the ZnS NRs during the cation exchange, which promotes size focusing of PbS QDs. PbS QDs synthesized through this new method have the advantages of high monodispersity, ease‐of‐size control, in situ passivation of chloride, high stability, and a “clean” surface. Infrared solar cells based on these PbS QDs with different bandgaps are fabricated, using conventional ligand exchange and device structure. All of the devices produced in this manner show excellent performance, showcasing the high quality of the PbS QDs. The highest performance of infrared solar cells is achieved using ≈0.95 eV PbS QDs, exhibiting an efficiency of 10.0% under AM 1.5 solar illumination, a perovskite‐filtered efficiency of 4.2%, and a silicon‐filtered efficiency of 1.1%.     

Design and Synthesis of Fluorinated Quantum Dots for Efficient and Stable 0D/3D Perovskite Solar Cells

Dimensionality engineering involving the low-dimensional and 3D perovskites has been demonstrated as an efficient promising strategy to modulate interfacial energy loss as well as instability in perovskite solar cells (PSCs). Herein, the use of fluorinated Cesium Lead Iodide (CsPbI₃) perovskite quantum dot (PQD) is first reported as interface modification layer for PSCs. The binding between the CsPbI₃ PQD surface and native oleic acid (OLA)/oleylamine (OAm) ligands is governed by a dynamic adsorption–desorption equilibrium. Perfluorooctanoic acid (PFA) with stronger binding affinity and more hydrophobic nature is explored to partially replace OLA to prepare the fluorinated ligand capped CsPbI₃ PQDs (F-CsPbI₃). Through optimization of the addition of PFA during hot-injection synthesis, the in situ treated F-CsPbI₃ PQDs display reduced surface defect states, higher photoluminescence quantum yields together with improved stability. Subsequently, both CsPbI₃ and F-CsPbI₃ PQDs are utilized as interface engineering layer in PSCs, delivering the best efficiency values of 21.99% and 23.42%, respectively, which is significantly enhanced compared to the control device (20.37%). More importantly, benefiting from its more hydrophobic properties, the F-CsPbI₃ PQD treated device exhibits excellent ambient storage stability (25 °C, relative humidity: 35–45%), retaining over 80% of its initial efficiency after 1500 h aging.     

量子点合成及其光电功能薄膜研究进展

量子点(quantum dots,QDs),也被称为半导体纳米晶体,得益于其廉价的制造成本和独特的光学物理学特性,已经广泛应用于光电探测器和太阳能电池的设计和开发.而量子点的合成则是制备光电探测器和太阳能电池的重要组成部分之一.本文对几种不同的量子点合成技术进行了概述,对国内外不同的基于量子点的光电探测器和太阳能电池进...     

Quantum Junction Solar Cells: Development and Prospects

Nanocrystals, called semiconductor quantum dots (QDs), contain excitons that are three-dimensionally bound. QDs exhibit a discontinuous electronic energy level structure that is similar to that of atoms and exhibit a distinct quantum confinement effect. As a result, QDs have unique electrical, optical, and physical characteristics that can be used in a variety of optoelectronic device applications, including solar cells. In this review article, the stable and controllable synthesis of QD materials is outlined for upscaling solar cells, including material development and device performance enhancement. It includes a systematic variety of device structures for the fabrication of solar cells, such as QD, hybrid QD/organic, hybrid QD/inorganic, perovskite QD, and hybrid 2D MXene QD/perovskite. The mechanisms for the improvement of stability by QD treatment are examined. For example, the 2D MXene QD and/or Cu_1.8S nanocrystal doping significantly increases the long-term light and ambient stability of perovskite solar cells, resulting from improved perovskite crystallization, reduced hole transport layer (HTL) aggregation and crystallization of films, and reduced UV-induced photocatalytic activity of the electron transport layer (ETL). For the advancement of QD solar cells and their interaction with various materials, the conclusions from this review are crucial. Finally, future prospects for the development of QD solar cells as well as current challenges are discussed.     

Highly Stable Colloidal “Giant” Quantum Dots Sensitized Solar Cells

Colloidal quantum dots (QDs) are widely studied due to their promising optoelectronic properties. This study explores the application of specially designed and synthesized “giant” core/shell CdSe/(CdS)_x QDs with variable CdS shell thickness, while keeping the core size at 1.65 nm, as a highly efficient and stable light harvester for QD sensitized solar cells (QDSCs). The comparative study demonstrates that the photovoltaic performance of QDSCs can be significantly enhanced by optimizing the CdS shell thickness. The highest photoconversion efficiency (PCE) of 3.01% is obtained at optimum CdS shell thickness ≈1.96 nm. To further improve the PCE and fully highlight the effect of core/shell QDs interface engineering, a CdSe_x S_1?x interfacial alloyed layer is introduced between CdSe core and CdS shell. The resulting alloyed CdSe/(CdSe_x S_1?x )₅/(CdS)₁ core/shell QD‐based QDSCs yield a maximum PCE of 6.86%, thanks to favorable stepwise electronic band alignment and improved electron transfer rate with the incorporation of CdSe_x S_1?x interfacial layer with respect to CdSe/(CdS)₆ core/shell. In addition, QDSCs based on “giant” core/CdS‐shell or alloyed core/shell QDs exhibit excellent long‐term stability with respect to bare CdSe‐based QDSCs. The giant core/shell QDs interface engineering methodology offers a new path to improve PCE and the long‐term stability of liquid junction QDSCs.     

Semiconducting Quantum Dots for Energy Conversion and Storage

Semiconducting quantum dots (QDs) have received huge attention for energy conversion and storage due to their unique characteristics, such as quantum size effect, multiple exciton generation effect, large surface-to-volume ratio, high density of active sites, and so on. However, the holistic and systematic understanding of the energy conversion and storage mechanism centering on QDs in specific application is still lacking. Herein, a comprehensive introduction of these extraordinary 0D materials, e.g., metal oxide, metal dichalcogenide, metal halides, multinary oxides, and nonmetal QDs, is presented. It starts with the synthetic strategies and unique properties of QDs. Highlights are focused on the rational design and development of advanced QDs-based materials for the various applications in energy-related fields, including photocatalytic H₂ production, photocatalytic CO₂ reduction, photocatalytic N₂ reduction, electrocatalytic H₂ evolution, electrocatalytic CO₂ reduction, electrocatalytic N₂ fixation, electrocatalytic O₂ evolution, electrocatalytic O₂ reduction, solar cells, metal-ion batteries, lithium–sulfur batteries, metal–air batteries, and supercapacitors. At last, challenges and perspectives of semiconducting QDs for energy conversion and storage are detailedly proposed.     

量子阱太阳能电池的外量子效率

通过实验比较了砷化镓量子阱太阳能电池与不含量子阱结构的普通砷化镓太阳能电池的外量子效率. 结果表明,量子阱太阳能电池吸收光子的波长从870nm 扩展到了1000nm. 当波长小于680nm时,量子阱太阳能电池的外量子效率低于普通太阳能电池;而当波长大于于680nm时,量子阱太阳能电池的外量子效率高于普通太阳能电池. 对这个现象给出了解释,并对用量子阱太阳能电池代替三结电池的中间子电池的可能性进行了讨论.     

Solution-Mediated Hybrid FAPbI3 Perovskite Quantum Dots for Over 15% Efficient Solar Cell

Organic–inorganic formamidinium lead triiodide (FAPbI₃) hybrid perovskite quantum dot (QD) is of great interest to photovoltaic (PV) community due to its narrow band gap, higher ambient stability, and long carrier lifetime. However, the surface ligand management of FAPbI₃ QD is still a key hurdle that impedes the design of high-efficiency solar cells. Herein, this study first develops a solution-mediated ligand exchange (SMLE) for preparing FAPbI₃ QD film with enhanced electronic coupling. By dissolving optimal methylammonium iodide (MAI) into antisolvent to treat the FAPbI₃ QD solution, the SMLE can not only effectively replace the long-chain ligands, but also passivate the A- and X-site vacancies. By combining experimental and theoretical results, this study demonstrates that the SMLE engineered FAPbI₃ QD exhibits lower defect density, which is beneficial for fabricating high-quality QD arrays with desired morphology and carrier transport. Consequently, the SMLE FAPbI₃ QD based solar cell outputs a champion efficiency of 15.10% together with improved long-term ambient storage stability, which is currently the highest reported value for hybrid perovskite QD solar cells. These results would provide new design principle of hybrid perovskite QDs toward high-performance optoelectronic application.     

量子阱太阳能电池的外量子效率

通过实验比较了砷化镓量子阱太阳能电池与不含量子阱结构的普通砷化镓太阳能电池的外量子效率.结果表明,量子阱太阳能电池吸收光子的波长从870nm扩展到了1000nm.当波长小于680nm时,量子阱太阳能电池的外量子效率低于普通太阳能电池;而当波长大于于680nm时,量子阱太阳能电池的外量子效率高于普通太阳能电池.对这个现象给出了解释,并对用量子阱太阳能电池代替三结电池的中间子电池的可能性进行了讨论.     

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.     

Multiple Function Synchronous Optimization by PbS Quantum Dots for Highly Stable Planar Perovskite Solar Cells with Efficiency Exceeding 23%

Colloidal lead sulfide (PbS) quantum dots (QDs), which possess quantum confinement effect and processing compatibility with perovskite, are regarded as an excellent material for optimizing perovskite solar cells (PSCs). However, the existing PSCs optimized by PbS QDs are still facing the challenges of poor performance of the charge transport layers, low utilization in the near-infrared (NIR) region, and unsuitable energy level alignment, which limit the improvement of power conversion efficiency (PCE). Herein, a synchronous optimization strategy is realized via simultaneously introducing PbS QDs into SnO₂ electron transport layer and employing rare-earth-doped PbS QDs (Eu:PbS QDs) film with hydrophobic chain ligands as the NIR light-absorping layer and hole transport layer (HTL) of devices. PbS QDs effectively decrease the density of trap states by passivating defects. Eu:PbS QDs film with adjustable bandgap is employed as an absorption layer to broaden the NIR spectral absorption. The well-matched energy level between Eu:PbS QDs layer and perovskite layer implies efficient hole transfer at the interface. The successful synchronous optimization greatly elevates all photovoltaic parameters, reaching a maximum PCE of 23.27%. This PCE is the highest for PSCs utilizing PbS QDs material in recent years. The optimized PSCs retain long-term moisture and light stability.