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Gradient Formation and Charge Carrier Dynamics of CuBiI4 based Perovskite-like Solar Cells
摘要： Designing lead-free inorganic perovskite or perovskite-like structure materials and researching the corresponding photoinduced charge carrier dynamics are always promising due to both the environment and power conversion efficiency considerations. In this work, we intelligently employ bilayer metal Bi/Cu thin film with different atomic ratios as precursor to in-situ fabricate CuBiI4 perovskite-like film with controlled Bi gradient at room temperature. This structure can significantly affect the photoinduced charge carrier dynamic of the resulting products. Next, a series of transient surface photovoltage (TSPV) measurements have been carried out to investigate the photoinduced charge carrier dynamics of such CuBiI4 and CuBiI4: organic hybrid thin films. It reveals that the gradually decreased Bi content from ITO to CuBiI4 can help the photoinduced charge carrier transportation. Finally, a champion PCE of 1.10% has been obtained from an ITO/ CuBiI4: polythieno[3,4-b]-thiophene-co-benzodithiophene (PTB7)/ Au solar cell device. In particular, we find an exact negative correlation of the defined parameter L (the defined value for evaluating the photoinduced charge carrier dynamic in TSPV measurements) with the corresponding PCE of various devices for the first time, which may pave a new way for evaluating the potential photoelectric and photovoltaic performances of new materials without assembly of solar cell devices.
关键词： CuBiI4,solar cell,photoinduced charge carrier dynamics,lead-free inorganic perovskite,transient surface photovoltage
更新于2025-09-23 15:19:57
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Ion Exchange/Insertion Reactions for Fabrication of Efficient Methylammonium Tin Iodide Perovskite Solar Cells
摘要： The low toxicity, narrow bandgaps, and high charge-carrier mobilities make tin perovskites the most promising light absorbers for low-cost perovskite solar cells (PSCs). However, the development of the Sn-based PSCs is seriously hampered by the critical issues of poor stability and low power conversion efficiency (PCE) due to the facile oxidation of Sn2+ to Sn4+ and poor film formability of the perovskite films. Herein, a synthetic strategy is developed for the fabrication of methylammonium tin iodide (MASnI3) film via ion exchange/insertion reactions between solid-state SnF2 and gaseous methylammonium iodide. In this way, the nucleation and crystallization of MASnI3 can be well controlled, and a highly uniform pinhole-free MASnI3 perovskite film is obtained. More importantly, the detrimental oxidation can be effectively suppressed in the resulting MASnI3 film due to the presence of a large amount of remaining SnF2. This high-quality perovskite film enables the realization of a PCE of 7.78%, which is among the highest values reported for the MASnI3-based solar cells. Moreover, the MASnI3 solar cells exhibit high reproducibility and good stability. This method provides new opportunities for the fabrication of low-cost and lead-free tin-based halide perovskite solar cells.
关键词： ion exchange/insertion reaction,solar cells,crystal growth,lead-free perovskites
更新于2025-09-23 15:19:57
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Dimension-controlled Growth of Antimony-based Perovskite-like Halide for Lead-free and Semitransparent Photovoltaics
摘要： Antimony (Sb) has been identified as a promising candidate for replacing toxic lead (Pb) in perovskite materials because Sb-based perovskite-like halides exhibit not only intrinsic thermodynamic stability but also a unique set of intriguing optoelectronic characteristics. However, Sb-based perovskite-like halides still suffer from a poor film morphology and uncontrollable halide constituents, which result from the disorder of the growth process. Herein, we propose a simple strategy to facilitate heterogeneous nucleation and control the dimension transformation by introducing bis(trifluoromethane)sulfonimide lithium (LiTFSI), which produces high-quality two-dimensional (2D) MA3Sb2I9-xClx films. As the spacer molecule among Sb-based pyramidal clusters, LiTFSI plays a role in forming a zero-dimensional (0D) intermediate phase and retarding crystallization. The slower dimension transformation well stabilizes the bandgap of perovskite-like films with a fixed Cl/I ratio (~7:2) and avoids random “x” values in MA3Sb2I9-xClx films prepared from the conventional method. Based on this method, Sb-based perovskite-like solar cells (PLSCs) achieve the highest recorded power conversion efficiency (PCE) of 3.34% and retain 90% of the initial PCE after being stored in ambient conditions for over 1400 h. More importantly, semitransparent Sb-based PLSCs with PCEs from 2.62% to 3.06% and average visible transparencies (AVTs) from 42% to 23% are successfully obtained, which indicates the great potential of the emerging Pb-free halide semiconductor for broad photovoltaic applications.
关键词： Perovskite-like halides,Photovoltaics,Lead-free,Antimony,Semitransparent solar cells
更新于2025-09-23 15:19:57
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with Optimal Band Gap for Photovoltaics and Defect-Insensitive Blue Emission
摘要： Despite rapid progress in the power-conversion efficiency of Pb-based perovskite solar cells, both the long-term instability and Pb toxicity are still the main challenges for their commercial applications. Here, by first-principles GW calculations, we find three kinds of two-dimensional (2D) 111-type Pb-free In-based halide perovskites of the form Cs3In2X9 (X = Cl, Br, I) as promising alternatives to the star material CH3NH3PbI3 (MAPbI3) because of the following excellent electronic, optical, and transport properties: (i) The 2D In-based halide perovskites are environmentally friendly lead-free materials. (ii) Compared with MAPbX3, they have greater structural stability. (iii) As energetic photovoltaic materials, 2D Cs3In2I9 perovskites are direct-band-gap semiconductors with optimal band gaps from 1.25 eV (trilayer) to 1.47 eV (monolayer). (iv) The 2D Cs3In2X9 perovskites have ideal band structures for solid-state lighting with a wide direct-optical-band-gap range (approximately 0.94–3.54 eV), covering the whole visible-light region, and light electron (heavy hole) effective mass, which will directly enhance the defect-insensitive emission efficiency due to the localization of holes. Particularly, Cs3In2BrxCl9?x has a suitable direct optical band gap for highly desired blue emission. (v) The absorption coefficient of Cs3In2X9 is up to 7 × 104 cm?1, which is between that of GaAs (104 cm?1) and that of MAPbI3 (105 cm?1). (vi) The estimated power-conversion efficiency in Cs3In2I9 reaches 28%, which is close to that of MAPbI3 (30%). These findings pave a way for designing nontoxic, stable, and high-performance photovoltaic and light-emitting devices.
关键词： light-emitting devices,photovoltaics,halide perovskites,lead-free,two-dimensional,first-principles calculations
更新于2025-09-23 15:19:57
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Zero-dimensional hybrid iodobismuthate derivatives: from structure study to photovoltaic application
摘要： The quest for lead-free light-absorbing perovskite materials has long been the target of researchers to make the ‘star’ material friendly to the commercial market. After a summary of different lead-free solar absorbers, we demonstrate a zero-dimensional iodobismuthate (MA)3[BiI6] ? 3MACl (MA: CH3NH3) featuring isolated hexaiodobismuthate (III) anions in the crystal analysis. The unexpectedly formed material was made via an orthogonal solvent permeation method and the decomposition of the guest solvent. We compare the BiI6 3- containing compound with a series of more common iodobismuthates, especially the dinuclear Bi2I9 3- in terms of dimensionalities via single-crystal diffraction and DFT calculations, respectively. An undocumented second-order phase transition was found between 190 K and 160 K for the dimeric MA3Bi2I9. The photovoltaic device from a thermally reorganized polycrystalline film of (MA)3[BiI6] ? 3MACl, which resembled the structure of (MA)3[Bi2I9] gave a power conversion efficiency of 1.09%.
关键词： photovoltaic,iodobismuthate,perovskite,zero-dimensional,lead-free
更新于2025-09-23 15:19:57
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Theoretical and experimental investigations on the bulk photovoltaic effect in lead-free perovskites MASnI <sub/>3</sub> and FASnI <sub/>3</sub>
摘要： Perovskite solar cells based on the lead free hybrid organic–inorganic CH3NH3SnI3 (MASnI3) and CH4N2SnI3 (FASnI3) perovskites were fabricated, and the photoelectric conversion e?ciency (PCE) was assessed. FASnI3's PCE was higher than MASnI3's e?ciency. To study the di?erent photovoltaic properties, we calculated their structural, electronic, and optical properties using density functional theory via the Perdew–Burke–Ernzerhof and spin–orbit coupling (PBE-SOC) methods. The results show that FASnI3 exhibits an appropriate band gap, substantial stability, marked optical properties, and signi?cant hole and electron conductive behavior compared with MASnI3. The interaction of organic cations (FA+) with the inorganic framework of FASnI3 was stronger than that with MASnI3, so they a?ected the band length and band angle distribution, causing the structure of the FASnI3 and MASnI3 to change. The calculations also demonstrated that energy splitting was evident in FASnI3 due to the spin–orbit coupling e?ect, however, it was moderate in MASnI3, which was caused by the H bond e?ect. This research not only furthers the understanding of these functional materials, but also can assist the development of highly e?cient and stable non-lead perovskite solar cells.
关键词： MASnI3,Perovskite solar cells,spin–orbit coupling,lead-free,density functional theory,photoelectric conversion efficiency,FASnI3
更新于2025-09-23 15:19:57
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Refractory plasmonics enabling 20% efficient lead-free perovskite solar cells
摘要： Core-shell refractory plasmonic nanoparticles are used as excellent nanoantennas to improve the efficiency of lead-free perovskite solar cells (PSCs). SiO2 is used as the shell coating due to its high refractive index and low extinction coefficient, enabling the control over the sunlight directivity. An optoelectronic model is developed using 3D finite element method (FEM) as implemented in COMSOL Multiphysics to calculate the optical and electrical parameters of plain and ZrN/SiO2-modified PSCs. For a fair comparison, ZrN-decorated PSCs are also simulated. While the decoration with ZrN nanoparticles boosts the power conversion efficiency (PCE) of the PSC from 12.9% to 17%, the use of ZrN/SiO2 core/shell nanoparticles shows an unprecedented enhancement in the PCE to reach 20%. The enhancement in the PCE is discussed in details.
关键词： lead-free perovskite solar cells,refractory plasmonics,ZrN/SiO2 core/shell nanoparticles,power conversion efficiency,optoelectronic modeling
更新于2025-09-23 15:19:57
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High-Performance UVa??Vis Photodetectors Based on a Lead-Free Hybrid Perovskite Crystal (MV)[SbI <sub/>3</sub> Cl <sub/>2</sub> ]
摘要： Low-dimensional lead-free organic?inorganic hybrid perovskites have gained increasing attention as having low toxicity, ease of processing, and good optoelectronic properties. Seeking for lead-free and narrow band gap organic?inorganic hybrid perovskites are of great importance for the development and application of photoelectric materials. Here, we reported a Sb-based organic?inorganic hybrid perovskite (MV)[SbI3Cl2], which has one-dimensional inorganic frameworks of the I-sharing double octahedra. (MV)[SbI3Cl2] shows a narrow direct band gap of 1.5 eV, and displays obvious photoresponse for the 532 nm light with rapid response speed of trise = 0.69 s, tdecay = 0.28 s. With an illumination power of 5 mW and a 50 V bias, the responsivities (R) and external quantum e?ciency (EQE) for (MV)[SbI3Cl2] photodetector under 532 nm laser are 29.75 mA/W and 6.69% respectively. This Sb-based halide double perovskite material will provide an alternative material for photodetector devices.
关键词： organic?inorganic hybrid perovskites,Sb-based,narrow band gap,photodetectors,lead-free
更新于2025-09-23 15:19:57
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Enhanced performance of tin halide perovskite solar cells by addition of hydrazine monohydrobromide
摘要： Although tin-based perovskite has been considered as a kind of potential environmentally-friendly photovoltaic materials, the tin-based perovskite solar cells are limited due to their poor stability and low conversion efficiency mainly tracing to the oxidation from Sn2t state in tin-based perovskite films. Herein, a facile reductive approach is developed to suppress the oxidation, in which tiny amount of hydrazine monohydrobromide is doped into FASnI3-based perovskite precursor solution as a reducing agent. Our results demonstrate that the addition of hydrazine monohydrobromide could reduce the defects and trap states in perovskite by inhibiting formation of tetravalent tin, and increase the open circuit voltage by widening the bandgap of perovskite. As a consequence, the best optimized perovskite solar cell achieves an excellent power conversion efficiency of 7.81%, which represented a 39.5% improvement compared to the best reference device. The optimized devices display stabilized power output near the maximum power point and negligible hysteresis effect.
关键词： Trap states,Defect,Hydrazine monohydrobromide,Lead-free,Tin-based perovskite solar cell
更新于2025-09-23 15:19:57
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Highly Reproducible and Efficient FASnI <sub/>3</sub> Perovskite Solar Cells Fabricated with Volatilizable Reducing Solvent
摘要： Lead-free tin halide perovskite solar cells (PSCs) have attracted great attention because of their low toxicity, ideal band gap, and high carrier mobilities. However, the efficiency and reproducibility of tin halide PSCs has been limited because of the facile oxidation of Sn2+ to Sn4+. Herein, liquid formic acid (LFA) was introduced as a reducing solvent in the FASnI3 (FA: formamidinium) perovskite precursor solution. Unlike solid reducing additives, the LFA solvent is volatile, so no residual LFA remained in the FASnI3 perovskite film. Use of the LFA solvent resulted in production of the FASnI3 perovskite film with high crystallinity, low Sn4+ content, reduced background doping, and low electronic trap density. As a result, an efficiency of over 10% was obtained for lead-free tin halide PSCs with improved reproducibility.
关键词： tin,Lead-free,oxidation,trap density,standard reduction potential
更新于2025-09-23 15:19:57