Vacuum-assisted growth is promising for scalable halide perovskite solar cells, yet its application to Sn-Pb narrow-band gap systems is hindered by the skin effect, where rapid surface solvent extraction induces buried voids and defective films. Here, we quantitatively elucidate the skin-effect formation through a microscopic solvent-dynamics model, revealing that it emerges when the surface extraction rate exceeds internal diffusion by over 3-fold. A low-temperature vacuum-assisted growth strategy is developed to rebalance surface extraction and internal diffusion, reducing the surface extraction rate by 5.8 times and suppressing the skin effect. This approach lowers film defect density at surface by 2 orders of magnitude. Consequently, Sn-Pb perovskite solar cells achieve efficiencies of 23.44% (0.0768 cm2) and 22.18% (1 cm2), representing the highest reported performance for anti-solvent-free Sn-Pb systems.
All-perovskite tandem solar cells are regarded as the next-generation photovoltaic technique, but their development is hindered by severe surficial recombination loss in Sn-Pb perovskite subcells. Here, we propose a dipole-engineered passivation strategy using methylpyridinium iodide (AMPYI2) molecules, where the methyl substitution position on the pyridinium ring governs the molecular dipole and interfacial interaction. Among the isomers, 2-AMPYI2 exhibits the largest dipole moment and binds most strongly to both the Sn-Pb perovskite surface and C60 electron transport layer. This dipole-driven field-effect passivation reduces the top-interface defect density by two orders of magnitude and suppresses interfacial non-radiative recombination. Consequently, this strategy yields a power conversion efficiency (PCE) of 23.3% in single-junction Sn-Pb perovskite solar cells and a PCE of 28.5% in all-perovskite tandem solar cells. Notably, the encapsulated tandem devices under maximum power point tracking retain 90% of their initial efficiency for 892 h at room temperature or for 228 h at 65 degrees C.
Solution-processed Sn-Pb perovskites have emerged as promising candidates for near-infrared (NIR) photodetectors due to their low-cost, tunable bandgap and scalable fabrication. However, Sn2+ oxidation creates Sn vacancies and undesirable p-type doping, resulting in high dark current and limited detectivity, which hinder the practical deployment of Sn-Pb perovskite photodetectors. Herein, we propose a Sn(SCN)2 inorganic molecular surface passivation strategy to suppress Sn2+ oxidation, significantly reduce surface defect density and enhance the optoelectronic properties (a dark current density of 10 nA cm−2 at a bias of −0.1 V and a high specific detectivity of 1.6 × 1013 Jones). Leveraging this approach, we report the monolithically integrated Sn-Pb perovskite NIR imager with a complementary metal-oxide-semiconductor readout circuit. The imager, featuring a 640 × 512 pixel array with a 15 μm pixel pitch, achieves an external quantum efficiency of 76
SnSe has received significant attention due to its exceptional optoelectronic and thermoelectric properties, making it a promising candidate for energy conversion applications. To exploit its potential for photo-thermoelectric applications, it is essential to prepare high-quality SnSe single-crystal films and investigate their intrinsic properties and local structure. In this work, pure and Na, Cu doped SnSe films were prepared via pulsed laser deposition (PLD). Orthorhombic SnSe films were successfully deposited along the [100] direction on SrTiO3 substrates. Our results show that the growth mode of SnSe films transitions from island-by-layer to 3D island growth as the film thickness increases. Notably, SnSe doped with Na and Cu restores a flatter surface even at larger thicknesses, and the current output of the Na and Cu doped SnSe film under optical and thermal excitations exhibited a significant improvement compared to the individual photo-induced and thermal-induced, as well as the sum of both, highlighting its potential for integrated photoelectric-thermoelectric applications.
A record power conversion efficiency of 27.17% was achieved in the photovoltaic cells under a temperature gradient of 10 °C, enabled by synergistic cooperation between photovoltaic and thermoelectric effects.
The power conversion efficiency of all-perovskite tandem solar cells is predominantly constrained by optical absorption losses, especially reflection losses. In this simulation study, we propose the optimization of a dual-interface serrated microstructure to mitigate these optical reflection losses in all-perovskite tandem solar cells. By adjusting the geometry of the periodic serrated structures at both the front interface and the back electrode, we enhance light absorption in the wide-bandgap perovskite layer and promote light scattering in the narrow-bandgap perovskite layer. The structural modification reduces the reflection-induced photocurrent density loss from 4.47 to 3.65 mA cm -2. It is expected to boost the efficiency of all-perovskite tandem solar cells to approximately 31.13%, representing a 3.41% increase. The dual-interface optimization effectively suppresses reflection losses and improves the overall photocurrent of all-perovskite tandem solar cells. These results offer a promising strategy for minimizing optical losses and enhancing device performance in all-perovskite tandem solar cells.
Paired electrolysis of waste feedstocks holds an energy-efficient alternative for chemical production;however,the sluggish anodic oxidation limited the total efficiency under larger current density.Herein,we constructed ultra low-coordinated Ni species with Ni-O coordination number of ~3 via a hydrothermal synthesis-sulfidation-annealing process and electrochemical activation and demonstrated the vital role in accelerating the proton deintercalation and reactive oxygen intermediate ·OH formation during electro-reforming polyethylene terephthalate hydrolysate(POR).The target catalyst NiCoSx/NF afforded a high formate productivity of 7.4 mmol cm -2 h -1 at~600 mA cm -2 with a formate Faradic efficiency(FE formate ) of 92.4% in POR and maintained a FE formate of ~90% for 100 h at 2 A in a membrane electrode assembly electrolyzer.Coupling POR on NiCoSx/NF with carbon dioxide reduction reaction on oxygen vacancies enriched Vo-BiSnO reached effective concurrent formate production with 172.7% of FE formate at 500 mA cm -2 and long-term stability.Such excellent performance shows the great prospect of electrocatalyst design by regulating the local metal environment.
In various optoelectrical devices, the ability of electrodes to withstand surge currents has a significant impact on the lifespan of the device. Especially when considering the use of ultra-thin metal-based flexible electrodes, which have garnered interest in recent years, it is crucial to address the challenges related to the failure and stability of the silver layer under current conditions within the operating environment. Despite their pivotal importance, these issues often receive inadequate attention in practical applications. In this paper, we report a universal method for the growth of ultra-thin Ag metal films with different metal oxide dispersions (CdO, ZnO and SnO2), emphasizing the evaluation of their stability under surge current. The findings indicated that the introduction of metal oxides significantly enhanced the growth conditions and surge stability of the ultra-thin Ag film. Among them, the Ag-CdO thin film exhibits an impressive average current withstand time of over 1000 min when subjected to a pulse current density of 0.83 MA cm−2. The reasons behind the failure of ultra-thin Ag films under surge current conditions were also examined. These insights provide a robust foundation for realizing the full potential of ultra-thin metal-based flexible electrodes in microelectronic devices.
Bismuth‐based halide perovskite materials have attracted extensive attention for optoelectronic applications due to nontoxicity and ambient stability. However, limited by low‐dimensional structure and isolate octahedron arrangement, the undesirable photophysical properties of bismuth‐based perovskites are still not well modulated. Here, the rational design and synthesis of Cs 3 SbBiI 9 with improved optoelectronic performance via premeditatedly incorporating antimony atoms with a similar electronic structure to bismuth into the host lattice of Cs 3 Bi 2 I 9 is reported. Compared with Cs 3 Bi 2 I 9 , the absorption spectrum of Cs 3 SbBiI 9 is broadened from ≈640 to ≈700 nm, the photoluminescence intensity enhances by two orders of magnitude indicating the extremely suppressed carrier nonradiative recombination, and the charge carrier lifetime is further increased from 1.3 to 207.6 ns. Taking representative applications in perovskite solar cells, the Cs 3 SbBiI 9 exhibits a higher photovoltaic performance benefiting from the improved intrinsic optoelectronic properties. Further structure analysis reveals that the introduced Sb atoms regulate the interlayer spacing between dimers in c ‐axis direction and the micro‐octahedral configuration, which correlate well with the improvement of optoelectronic properties of Cs 3 SbBiI 9 . It is anticipated that this work will benefit the design and fabrication of lead‐free perovskite semiconductors for optoelectronic applications.
The alloyed lead/tin (Pb/Sn) halide perovskites have gained significant attention in the development of tandem solar cells and other optoelectronic devices due to their widely tunable absorption edge. To gain a better understanding of the intriguing properties of Pb/Sn perovskites, such as their anomalous bandgap's dependence on stoichiometry, it is important to deepen the understanding of their chemical behavior and local structure. Herein, we investigate a series of two-dimensional Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) phase alloyed Pb/Sn bromide perovskites using butylammonium (BA) and 3-(aminomethyl)pyridinium (3AMPY) as the spacer cations: (BA)2(MA)n-1PbxSnn-xBr3n+1 (n = 1-3) and (3AMPY)(MA)n-1PbxSnn-xBr3n+1 (n = 1-3) through a solution-based approach. Our results show that the ratio and site preference of Pb/Sn atoms are influenced by the layer thickness (n) and spacer cations (A'), as determined by single-crystal X-ray diffraction. Solid-state 1H, 119Sn, and 207Pb NMR spectroscopy analysis shows that the Pb atoms prefer the outer layers in n = 3 members: (BA)2(MA)PbxSnn-xBr10 and (3AMPY)(MA)PbxSnn-xBr10. Layered 2D DJ alloyed Pb/Sn bromide perovskites (3AMPY)(MA)n-1PbxSnn-xBr3n+1 (n = 1-3) demonstrate much narrower optical band gaps, lower energy PL emission peaks, and longer carrier lifetimes compared to those of RP analogs. Density functional theory calculations suggest that Pb-rich alloys (Pb:Sn ∼4:1) for n = 1 compounds are thermodynamically favored over 50:50 (Pb:Sn ∼1:1) compositions. From grazing-incidence wide-angle X-ray scattering (GIWAXS), we see that films in the RP phase orient parallel to the substrate, whereas for DJ cases, random orientations are observed relative to the substrate.
A schematic of the modification mechanism of chloroformamidine hydrochloride (CFA) at SnO 2 /perovskite (PVK) interface.
Silicon heterojunction(SHJ) solar cells are an important part of the current photovoltaic industry, and they have attracted wide spread attention because of their high open-circuit voltage(V oc ). The optical and electrical properties of transparent conductive oxide(TCO) films in SHJ solar cells affect the short-circuit current(J sc ) and filling factor(FF), respectively, and the variation of J sc and FF will further affect the conversion efficiency of the cells. Therefore, the performance of the TCO film layer limits the long-term development of SHJ solar cells. In recent years, the development of TCO films in SHJ cells has mainly focused on improving the performance of doped In 2 O 3 systems and doped ZnO systems. In this paper, we firstly describe the different structures of SHJ solar cells, followed by the optoelectronic properties, namely, transmittance, band gap, sheet resistance, carrier concentration, mobility, and work function, of transparent conductive oxide films. The effect of contact properties with each layer on the performance of the cell is then summarized, the application and research status of various transparent conductive oxide films in SHJ solar cells are introduced, and the prospects for their future development trends are reviewed.
Inorganic perovskite solar cells (PSCs) have witnessed extraordinary advances owing to their prominent stability against thermal aging. However, they suffer from a phase transition from black phase to yellow phase under ambient conditions and serious energy losses relative to the optical bandgap. Herein, urea (Ur) and methyl‐substituted urea (Me‐Ur) additives are used to modulate the lattice structure and crystallinity of the CsPbI 2 Br, facilitating phase stability and high device performance. The Me‐Ur can attenuate the strong hydrogen bonding networks in the Ur, which leads to stronger coordination of the carbonyl group with undercoordinated Pb 2+ , more efficiently passivating the defect states and suppressing the lattice distortion of the [PbI 6 ] 4− octahedra in the CsPbI 2 Br perovskite. Consequently, a champion power conversion efficiency of 16.5% with an open‐circuit voltage up to 1.33 V is obtained for the CsPbI 2 Br+Me‐Ur‐based PSCs, accompanied by enhanced stability under continuous illumination at a temperature of 45 ± 5 °C. These results emphasize the importance of regulating the lattice distortion by the urea derivative to implement efficient and stable inorganic CsPbI 2 Br PSCs.
Abstract The sufficient utilization of longer-wavelength infrared light is a long-sought goal for efficient perovskite solar cells (PSCs) since they convert into heat easily and destroy the device stability. Establishing thermoelectric effect on the same PSCs is supposed to be an efficient way to convert heat into electricity. However, whether thermoelectric effect exists during the photovoltaic process has never been concerned. Herein, we report that the FAP-based PSCs operated under temperature differences (ΔT=15 oC) afford a champion PCE of 25.74%, higher than 22.84% with ΔT=0 oC, along with an improved Voc from 1.17 V to 1.23 V. It’s demonstrated that integrating photoelectric and thermoelectric effects can magnify the solar-to-electricity conversion. The critical factors to success are utilizing adequately photocarrier in parallel with regulating the intrinsic carrier directional transport and facilitating the charge carriers’ collection. The work shed light on the synergistic contribution of photoelectric and thermoelectric effect to efficient PSCs.
White-light broadband emission in the visible range from the low-dimensional halide perovskites is commonly attributed to structural distortions in lead bromide octahedra. In this paper, we report Dion-Jacobson-phase two-dimensional (2D) lead bromide perovskites based on short aromatic diammonium cations, p-phenylene diammonium (pPDA), m-phenylene dia-mmonium (mPDA), and two 1D compounds templated by o-phenylene diammonium (oPDA). All of the compounds exhibit white-light emission. Single-crystal X-ray diffraction analysis reveals that the distortion of the Pb octahedra is influenced by the stereochemistry of the cations and their interactions with the perovskite layers. Solid-state 1H and 207Pb NMR spectroscopy analysis further confirms this trend, whereby different 1H and 207Pb chemical shifts are observed for the pPDA and mPDA spacer cations, indicating different hydrogen-bonding interactions and octahedral distortions. Owing to the octahedral distortion, 2D (mPDA)PbBr4 compounds exhibit broader white-light emission than 2D (pPDA)PbBr4. Density functional theory calculations suggest that (pPDA)PbBr4 and (mPDA)PbBr4 are direct-band-gap semiconductors, and they exhibit larger electronic band gaps and effective masses than the Ruddlesden-Popper-phase (BA)2PbBr4. Among the films of these compounds, 2D (mPDA)PbBr4 shows the best stability, which is attributed to stronger hydrogen-bonding interactions in the material.
The hole-storage layer (HSL) strategy has been demonstrated as an efficient interfacial modification method to overcome the instability of tantalum nitride (Ta3N5) photoanodes and further boost high performance in photoelectrochemical (PEC) water oxidation reaction. Herein, we report that the CoOx/Ni(OH)(x) bilayer as a typical HSL could effectively extract and store photogenerated holes from Ta3N5, resulting in a decent photocurrent enhancement and stable water oxidation for at least 30 h. Most strikingly, the reversible formation of Co(IV) species inside the ultrathin CoOx layer during PEC water oxidation is found to regulate the hole-storage process, leading to facilitated photogenerated hole extraction capacity and suppressed charge recombination. Furthermore, upon the insertion of the CoOx/Ni(OH)(x) bilayer for the Ta3N5/CoPi photoanode, the photocurrent could be evidently increased, emphasizing the general applicability of the HSL strategy in promoting water oxidation reaction.
Increasing electroluminescene quantum efficiency (EQEEL) of the photoactive layer to reduce non-radiative recombination energy loss (Eloss) has been demonstrated as an effective strategy to improve open-circuit voltage (Voc) of organic solar cells (OSCs). Meanwhile, incorporating a third component into the active-layer film can improve power conversion efficiency (PCE) of resultant ternary OSCs, mostly contributed from increments in short-circuit current density and fill factor but less in the Voc. Herein, we report a highly fluorescent molecule (IT-MCA) as a third component to reduce the Eloss and enhance the Voc for ternary OSCs. Applying the IT-MCA to three binary hosts, a significant increase of Voc (41 mV) is acquired and a best PCE of 16.7% is obtained with outstanding device stability. This work provides a new guideline to design the third-component molecule by enhancing its fluorescence for efficient and stable ternary OSCs with improved Voc.
Non-fullerene organic solar cells (NF–OSCs) have recently attracted enormous attention due to the rapid advance of high-performance photoabsorbers. On the other hand, interfacial materials also play a crucial role in further increasing the device efficiency, but those materials in particular effective hole transporting ones for NF–OSCs are less developed. In this work, three low-temperature solution-processing ferrous oxide films (including CoOx, NiOx, and FeOx) are used as hole transporting layer (HTL) for NF–OSCs. By adding a surfactant and treating with the ultraviolet ozone (UVO), uniform ferrous oxide films with adjustable energy bands are achieved. The NF–OSCs based on PBDB-T-2Cl:IT-4F active layer and using CoOx, NiOx, and FeOx as the HTL afford power conversion efficiencies of 11.4%, 10.2% and 6.4%, respectively. The higher performance of NF–OSCs with the UVO-treated CoOx as the HTL is attributed to its more suitable energy level alignment and better hole transportation property relative to those of the other two counterparts.
Dion-Jacobson (DJ) phase and Ruddlesden-Popper phase 2D perovskites have been, individually, demonstrated to be more stable than 3D counterparts for perovskite solar cells (PSCs). In order to further improve the efficiency and stability of 2D PSCs, we herein report merging them to construct a DJ:RP double-phase perovskite (DPP) structure for the first time. With the DJ 2D perovskite composed of diammonium as the matrix, a monoammonium with a larger size than the diammonium is incorporated to form an independent RP phase 2D perovskite coexisting with the DJ one (DJ:RP DPP structure), which facilitates crystal growth, suppresses charge recombination, and improves charge transport. As a comparison, introduction of a smaller monoammonium than the diammonium leads to its insertion between inorganic slabs, yielding a distorted DJ 2D perovskite structure, which induces lattice relaxation/distortion and thus lowered charge transportation. Consequently, 2D PSCs based on the DJ:RP DPP afford an impressive efficiency of 13.8% with excellent thermal stability at 85 degrees C in damp air. This work demonstrates a new and promising strategy of developing the DJ:RP DPP for highly efficient and robust 2D PSCs.
Ferrihydrite (Fh) has been demonstrated acting as a hole-storage layer (HSL) in photoelectrocatalysis system. However, the intrinsic structure responsible for the hole storage function for Fh remains unclear. Herein, by dehydrating the Fh via a careful calcination, the essential relation between the HSL function and the structure evolution of Fh material is unraveled. The irreversible and gradual loss of crystal water molecules in Fh leads to the weakening of the HSL function, accompanied with the arrangement of inner structure units. A structure evolution of the dehydration process is proposed and the primary active structure of Fh for HSL is identified as the [FeO6] polyhedral units bonding with two or three molecules of crystal water. With the successive loss of chemical crystal water, the coordination symmetry of [FeO6] hydration units undergoes mutation and a more ordered structure is formed, causing the difficulty for accepting photogenerated holes as a consequence.