Wide-bandgap Perovskite Research Articles

Role of NiO in wide-bandgap perovskite solar cells based on self-assembled monolayers

NiO/self-assembled monolayer (SAM) double hole transport layers (HTLs) has become the mainstream choice in high-efficiency single-junction and tandem perovskite solar cells (PSCs). However, the underlying role of NiO in double HTLs from the microscale is not systematically revealed currently. Herein, we reveal that NiO plays an important role in inducing a more uniform and thinner SAM from three aspects. Firstly, compared with indium tin oxide (ITO), the NiO surface exposes less crystal facet orientations and a higher metal atom density, suggesting that sufficient chemical binding sites for SAMs are provided to facilitate the close-packed assembly of SAMs. Secondly, NiO modified ITO exhibits smaller surficial roughness and strongly bonded −OH, which is beneficial to the uniform distribution of SAMs and strong adhesion to the NiO surface. Utilizing the well-constructed SAM, we fabricate wide-bandgap (>1.75 eV) PSCs using vacuum-assisted technology and achieve an impressive photoelectric conversion efficiency of 19.55 %. These findings not only deepen the understanding of SAM assembly on substrates but also provide essential guidance for the future industrialization of PSCs.

Solvent engineering for scalable fabrication of perovskite/silicon tandem solar cells in air

Perovskite/silicon tandem solar cells hold great promise for realizing high power conversion efficiency at low cost. However, achieving scalable fabrication of wide-bandgap perovskite (~1.68 eV) in air, without the protective environment of an inert atmosphere, remains challenging due to moisture-induced degradation of perovskite films. Herein, this study reveals that the extent of moisture interference is significantly influenced by the properties of solvent. We further demonstrate that n-Butanol (nBA), with its low polarity and moderate volatilization rate, not only mitigates the detrimental effects of moisture in air during scalable fabrication but also enhances the uniformity of perovskite films. This approach enables us to achieve an impressive efficiency of 29.4% (certified 28.7%) for double-sided textured perovskite/silicon tandem cells featuring large-size pyramids (2–3 μm) and 26.3% over an aperture area of 16 cm2. This advance provides a route for large-scale production of perovskite/silicon tandem solar cells, marking a significant stride toward their commercial viability.

Ligand Homogenized Br-I Wide-Bandgap Perovskites for Efficient NiOx-Based Inverted Semitransparent and Tandem Solar Cells.

Phase heterogeneity of bromine-iodine (Br-I) mixed wide-bandgap (WBG) perovskites has detrimental effects on solar cell performance and stability. Here, we report a heterointerface anchoring strategy to homogenize the Br-I distribution and mitigate the segregation of Br-rich WBG-perovskite phases. We find that methoxy-substituted phenyl ethylammonium (x-MeOPEA+) ligands not only contribute to the crystal growth with vertical orientation but also promote halide homogenization and defect passivation near the buried perovskite/hole transport layer (HTL) interface as well as reduce trap-mediated recombination. Based on improvements in WBG-perovskite homogeneity and heterointerface contacts, NiOx-based opaque WBG-perovskite solar cells (WBG-PSCs) achieved impressive open-circuit voltage (Voc) and fill factor (FF) values of 1.22 V and 83%, respectively. Moreover, semitransparent WBG-PSCs exhibit a PCE of 18.5% (15.4% for the IZO front side) and a high FF of 80.7% (79.4% for the IZO front side) for a designated illumination area (da) of 0.12 cm2. Such a strategy further enables 24.3%-efficient two-terminal perovskite/silicon (double-polished) tandem solar cells (da of 1.159 cm2) with a high Voc of over 1.90 V. The tandem devices also show high operational stability over 1000 h during T90 lifetime measurements.

4F-Phenethylammonium chloride as a key component for interfacial engineering of wide-bandgap perovskite absorber

The development of high-efficiency and stabilized tandem solar cells and solar cells for indoor light harvesting relies heavily on the fabrication of wide-bandgap (WBG) perovskite solar cells (PSCs) that exhibit exceptional efficiency and stability. In this study, we introduce an effective method for enhancing the optoelectronic properties of a 1.74 eV WBG perovskite absorber by interfacial engineering. Specifically, we utilize 4F-Phenethylammonium Chloride (4F-PEACL) as a key component for the surface treatment of perovskite layer. The treatment of perovskite with 4F-PEACL alters the surface stoichiometry, promoting self-doping and surface passivation, reducing surface recombination, and improving the optoelectronic properties of perovskite. Consequently, PCSs with perovskite treated with 4F-PEACL exhibit a notable power conversion efficiency of 20.27 %. Furthermore, the devices subjected to 4F-PEACL treatment demonstrate enhanced stability compared to the control devices across a range of testing settings. The findings of our study indicate that the utilization of organic salt perovskite passivation holds great potential in the development of efficient and stable WBG PSCs.

Monolithic all-perovskite tandem solar cells: advancing sustainable energy options

This paper discusses the results of a simulation-based study on lead-free perovskite tandem devices. Wide bandgap (1.8 eV) perovskite materials Cs2AgBi0.75Sb0.25Br6 as the top cell and narrow bandgap (1.3 eV) perovskite materials CsSnI3 as the bottom cell make up the simulated tandem cell device, respectively. The optimisation process involves individually fine-tuning both cells under standard solar radiation conditions of 100 W/m2. The tandem cells necessitate precise current matching between the two sub-cells. The current matching condition manifests at Jsc of 16 mA cm−2 when the top and bottom cells reach an optimised thickness of 700 nm and 65 nm, respectively. The optimised tandem cell achieves a 24.47% power conversion efficiency (PCE), a high Voc of 1.7278 V, and a high fill factor of 83.72%. Furthermore, tandem solar cells’ temperature dependence is examined in the 300 K to 400 K range, revealing that efficiency decreases with temperature due to a reduction in Jsc (short-circuit current). Notably, the current matching condition is primarily influenced by the top cell, which exhibits less variation than the bottom cell. This study paves the way for developing tandem solar cells made entirely of lead-free perovskites and presents a new approach for the experimental realisation of high-power conversion efficiency.

Influence of Hole Transport Layers on Buried Interface in Wide-Bandgap Perovskite Phase Segregation.

Light-induced phase segregation, particularly when incorporating bromine to widen the bandgap, presents significant challenges to the stability and commercialization of perovskite solar cells. This study explores the influence of hole transport layers, specifically poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine (PTAA) and [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz), on the dynamics of phase segregation. Through detailed characterization of the buried interface, we demonstrate that Me-4PACz enhances perovskite photostability, surpassing the performance of PTAA. Nanoscale analyses using in situ Kelvin probe force microscopy and quantitative nanomechanical mapping techniques elucidate defect distribution at the buried interface during phase segregation, highlighting the critical role of substrate wettability in perovskite growth and interface integrity. The integration of these characterization techniques provides a thorough understanding of the impact of the buried bottom interface on perovskite growth and phase segregation.

Enhancement of Efficiency of Perovskite Solar Cells with Hole-Selective Layers of Rationally Designed Thiazolo[5,4-d]thiazole Derivatives.

We introduce thiazolo[5,4-d]thiazole (TT)-based derivatives featuring carbazole, phenothiazine, or triphenylamine donor units as hole-selective materials to enhance the performance of wide-bandgap perovskite solar cells (PSCs). The optoelectronic properties of the materials underwent thorough evaluation and were substantially fine-tuned through deliberate molecular design. Time-of-flight hole mobility TTs ranged from 4.33 × 10-5 to 1.63 × 10-3 cm2 V-1 s-1 (at an electric field of 1.6 × 105 V cm-1). Their ionization potentials ranged from -4.93 to -5.59 eV. Using density functional theory (DFT) calculations, it has been demonstrated that S0 → S1 transitions in TTs with carbazolyl or ditert-butyl-phenothiazinyl substituents are characterized by local excitation (LE). Mixed intramolecular charge transfer (ICT) and LE occurred for compounds containing ditert-butyl carbazolyl-, dimethoxy carbazolyl-, or alkoxy-substituted triphenylamino donor moieties. The selected derivatives of TT were used for the preparation of hole-selective layers (HSL) in PSC with the structure of glass/ITO/HSLs/Cs0.18FA0.82Pb(I0.8Br0.2)3/PEAI/PC61BM/BCP/Ag. The alkoxy-substituted triphenylamino containing TT (TTP-DPA) has been demonstrated to be an effective material for HSL. Its layer also functioned well as an interlayer, improving the surface of control HSL_2PACz (i.e., reducing the surface energy of 2PACz from 66.9 to 52.4 mN m-1), thus enabling precise control over perovskite growth energy level alignment and carrier extraction/transportation at the hole-selecting contact of PSCs. 2PACz/TTP-DPA-based devices showed an optimized performance of 19.1 and 37.0% under 1-sun and 3000 K LED (1000 lx) illuminations, respectively. These values represent improvements over those achieved by bare 2PACz-based devices, which attained efficiencies of 17.4 and 32.2%, respectively. These findings highlight the promising potential of TTs for the enhancement of the efficiencies of PSCs.

Visualizing the Structure-Property Nexus of Wide-Bandgap Perovskite Solar Cells under Thermal Stress.

Wide-bandgap perovskite solar cells (PSCs) toward tandem photovoltaic applications are confronted with the challenge of device thermal stability, which motivates to figure out a thorough cognition of wide-bandgap PSCs under thermal stress, using in situ atomic-resolved transmission electron microscopy (TEM) tools combing with photovoltaic performance characterizations of these devices. The in situ dynamic process of morphology-dependent defects formation at initial thermal stage and their proliferations in perovskites as the temperature increased are captured. Meanwhile, considerable iodine enables to diffuse into the hole-transport-layer along the damaged perovskite surface, which significantly degrade device performance and stability. With more intense thermal treatment, atomistic phase transition reveals the perovskite transform to PbI2 along the topo-coherent interface of PbI2/perovskite. In conjunction with density functional theory calculations, a mutual inducement mechanism of perovskite surface damage and iodide diffusion is proposed to account for the structure-property nexus of wide-bandgap PSCs under thermal stress. The entire interpretation also guided to develop a thermal-stable monolithic perovskite/silicon tandem solar cell.

Low temperature method-based evaporation/spray-coating technology for wide bandgap perovskite solar cells

Years of working on perovskite solar cells (PSCs)-based tandem devices and single-junction devices have approved that low annealing temperatures can be beneficial for improving device performances. In this study, pseudo-halogen ion engineering works well in the evaporation/spray-coating method. According to our research, it is has been proven that the addition of formamidine acetate (FAAc) can effectively reduce the annealing temperature from 170 °C to 150 °C, accelerate the maturation process of the perovskite films, and broaden the annealing window. As a result, a perovskite film with homogeneous crystallization and low residual stress is achieved, leading to extended charge carrier lifetimes, elevated photoluminescence quantum yields (PLQY), reduced Urbach energies. The corresponding PSCs were prepared through evaporation/spray-coating method achieves an impressive power conversion efficiency (PCE) of 19.46%, which is the highest efficiency among wide-bandgap (WBG) PSCs fabricated by this method. And the unencapsulated devices exhibit satisfactory stability, retaining 80% of the initial PCE after 600 h of thermal aging at 60 °C and retaining 90% of the initial PCE after 1500 h of 50% humidity aging at 25 °C, respectively.

Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

23.6 % Efficient perovskite-organic tandem photovoltaics enabled by recombination layer engineering

Recombination layers are crucial in achieving high power conversion efficiency (PCE) in tandem solar cells. Here, we report the development and optimization of recombination junctions for high PCE perovskite-organic tandem solar cells (PO-TSCs). We choose a wide bandgap perovskite (1.79 eV) for the front subcell and a narrow bandgap (1.36 eV) organic bulk heterojunction (BHJ) for the rear subcell. The optimal thicknesses of the perovskite and organic layers were determined to be 260 and 100 nm, respectively, based on the analysis of Transfer-Matrix optical simulations. Our results demonstrate that the optimal recombination layer consists of an ultrathin layer of indium zinc oxide IZO (∼ 2 nm) deposited on MoOx/2PACz, which delivers a PCE of 23.6 %. This high PCE is attributed to the high transparency of the recombination layer in the NIR spectra region and the low sheet resistance of IZO. Furthermore, we provide a theoretical analysis of the potential efficiency of PO-TSCs as a function of front and rear subcells and predict a maximum theoretical PCE value of more than 36 %. Our work highlights the importance of selecting the proper recombination layer design for achieving high-performance PO-TSCs.

Enhanced chemical interaction between ionic liquid and halide perovskite to improve performance of perovskite solar cells

Perovskite solar cells (PSCs) with wide bandgap (Eg > 1.67 eV) metal halides combined with silicon solar cells for tandem photovoltaics are one of the most promising technologies for achieving efficiencies over 33%. However, the low long-term stability of PSCs due to deep trap states and halide segregation in the perovskites impedes commercialization. Ionic liquids have been widely used to overcome this drawback, with anions primarily interacting with the perovskite and cations playing a more limited role. Here, by giving cations functional groups that bind to the perovskite and passivate defects, both cations and anions in the ionic liquid are designed to improve the quality of the perovskite thin film. The incorporation of a methoxy group within the cation fosters interaction with lead cations in the perovskite structure. This interaction enhances passivation at the interfaces, thereby suppressing ion migration and leading to improved optoelectronic properties. PSCs fabricated with the wide-bandgap perovskite containing 1-(2-methoxyethyl)-1-methylpiperidinium thiocyanate (MMP-SCN) exhibit higher power conversion efficiency (PCE) and long-term stability against light, heat, and moisture than those containing 1-butyl-1-methylpiperidinium thiocyanate (BMP-SCN). PSCs with MMP-SCN achieve PCEs over 20% with FF of over 84% and demonstrate long-term operational stability of 1000 h.

All-Round Passivation Strategy Yield Flexible Perovskite/CuInGaSe2 Tandem Solar Cells with Efficiency Exceeding 26.5.

The perovskite/Cu(InGa)Se2 (CIGS) tandem solar cells (TSCs) presents a compelling technological combination poised for the next generation of flexible and lightweight photovoltaic (PV) tandem devices, featuring a tunable bandgap, high power conversion efficiency (PCE), lightweight flexibility, and enhanced stability and durability. Over the years, the imperative to enhance the performance of wide bandgap (WBG) perovskite solar cells (PSCs) has grown significantly, particularly in the context of a flexible tandem device. In this study, an all-round passivation strategy known as Dual Passivation at Grains and Interfaces (DPGI) is introduced for WBG PSCs in perovskite/CIGS tandem structures. The implementation of DPGI is tailored to improve film crystallinity and passivate defects across the solar cell structure, leading to a substantial performance enhancement for WBG PSCs. Subsequently, both rigid and flexible tandem devices are assembled. Impressively, a fully flexible 4T perovskite/CIGS TSCs is successfully fabricated with a PCE of 26.57%, making it the highest value in this field and highlighting its potential applications in the next generation of flexible lightweight PV tandem devices.

π-π Stacking at the Perovskite/C60 Interface Enables High-Efficiency Wide-Bandgap Perovskite Solar Cells.

Interface passivation is a key method for improving the efficiency of perovskite solar cells, and 2D/3D perovskite heterojunction is the mainstream passivation strategy. However, the passivation layer also produces a new interface between 2D perovskite and fullerene (C60), and the properties of this interface have received little attention before. Here, the underlying properties of the 2D perovskite/C60 interface by taking the 2D TEA2PbX4 (TEA=C6H10NS; X=I, Br, Cl) passivator as an example are systematically expounded. It is found that the 2D perovskite preferentially exhibits (002) orientation with the outermost surface featuring an oriented arrangement of TEACl, where the thiophene groups face outward. The outward thiophene groups further form a strong π-π stacking system with C60 molecule, strengthening the interaction force with C60 and facilitating the creation of a superior interface. Based on the vacuum-assisted blade coating, wide-bandgap (WBG, 1.77eV) perovskite solar cells achieved impressive records of 19.28% (0.09cm2) and 18.08% (1.0cm2) inefficiency, respectively. This research not only provides a new understanding of interface processing for future perovskite solar cells but also lays a solid foundation for realizing efficient large-area devices.

Delaying crystallization and anchoring the grain boundaries defects via π-π stacked molecules for efficient and stable wide-bandgap perovskite solar cells

Owing to the easy migration of halogen ions in wide-bandgap perovskite, it will lead to the formation of a large number of uncoordinated Pb2+ to form deep-level defects, which seriously affects the power conversion efficiency (PCE) and stability of wide-bandgap perovskite solar cells (PSCs). The introduction of additives has been recognized as an effective method to improve these defects, especially Lewis acid-base additives. Herein, Lewis base molecule dibenzofuran (DBF) with π-conjugated system, which can form π-π stacked dimer, is used as a perovskite additive. The detailed crystallization process of perovskite main precursor triggered by DBF is measured by using laser scanning confocal microscopy. It is demonstrated that the addition of DBF in perovskite samples resulted in a deceleration of the crystallization process, which is due to the formation of Lewis acid-base complexes between DBF π-π stacked dimer and perovskite, which can obtain perovskite films with reduced defect density. As a result, the champion PCE of the wide-bandgap (1.68 eV) perovskite device reaches 20.18 %, significantly higher than the control device (17.79 %). Additionally, the device with no encapsulation demonstrates better stability, as it maintains over 90 % of the initial PCE under an air environment with 30–40 % relative humidity (RH) and 25 °C for 1200 h.

Homogenizing Morphology and Composition of Methylammonium‐Free Wide‐Bandgap Perovskite for Efficient and Stable Tandem Solar Cells

AbstractA facile and eco‐friendly dimethyl sulfoxide‐mediated solution aging (DMSA) treatment is presented to control the crystallization dynamics of methylammonium (MA)‐free wide‐bandgap (WBG) perovskite films, enhancing film quality, and morphology for high‐performance tandem solar cells. The comprehensive structural, morphological, and characterization analyses reveal that the DMSA treatment significantly enhances composition and morphology homogeneity while suppressing halide segregation. Consequently, opaque, and semi‐transparent MA‐free WBG perovskite solar cells (PSCs) exhibit remarkable power conversion efficiencies (PCEs) of 18.28% and 17.61%, respectively. Notably, the unencapsulated DMSA‐treated devices maintain 95% of the initial PCE after 900 h of continuous operation at 55 °C ± 5 °C. Furthermore, stacking semi‐transparent DMSA‐treated PSCs as top cells in a 4T tandem configuration, along with silicon heterojunction (SHJ), lead–tin (Pb–Sn) alloyed PSCs, and organic photovoltaics (OPV) as bottom cells, yields impressive PCEs of 28.09%, 26.09%, and 25.28%, respectively, for the fabricated tandem cells. This innovative approach opens new avenues for enhancing the photo‐stability and photovoltaic performance of perovskite‐based tandem solar cells.

Phase-stable wide-bandgap perovskites enabled by suppressed ion migration

Wide-bandgap (>1.7 eV) perovskites suffer from severe light-induced phase segregation due to high bromine content, causing irreversible damage to devices stability. However, the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed. Here, we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride (4-ATpHCl) with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film. 4-ATpH+ impeded halogen ion migration by anchoring on the perovskite surface, leading to the inhibition of phase segregation and thus the passivation of defects, which is ascribed to the interaction of 4-ATpH+ with perovskite and the formation of low-dimensional perovskites. Finally, the champion device achieved an efficiency of 19.32% with an open-circuit voltage (VOC) of 1.314 V and a fill factor of 83.32%. Moreover, 4-ATpHCl modified device exhibited significant improved stability as compared with control one. The target device maintained 80% of its initial efficiency after 519 h of maximum power output (MPP) tracking under 1 sun illumination, however, the control device showed a rapid decrease in efficiency after 267 h. Finally, an efficiency of 27.38% of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.

Tail states suppression via surface-modification of wide-bandgap perovskites for high-efficiency all-perovskite photovoltaic tandems

As an essential light-absorbing material in perovskite-based tandem solar cells, wide-bandgap (WBG) perovskite has garnered extensive attention. Nevertheless, due to severe non-radiative recombination from tail states, as well as photoinduced phase segregation and unoptimized charge transfer, WBG perovskite solar cells (PSCs) typically display significant open-circuit voltage (VOC) loss and low fill factor (FF). In this work, we report to modify the 1.68 eV WBG perovskite film upon optimized surface passivation with 1,3-propane-diammonium iodide (PDAI2). Time-resolved microwave conductivity measurement is employed to analyze the tail states, mobilities of charge carriers and the rate constants of recombination in perovskite films. The results indicate that the optimized surface modification strategy not only enhances film quality, boosts carrier transport, but also suppresses tail states and therefore diminishes non-radiative recombination, consequently elevating the VOC and FF of the device. Hence, the PDAI2-assisted WBG PSCs deliver an optimal efficiency of 21.48 %, accompanied by a VOC of 1.243 V. Furthermore, the integration of a narrow-bandgap tin–lead PSC with a semi-transparent WBG PSC results in a four-terminal perovskite/perovskite tandem solar cell, showcasing an efficiency surpassing 28 %. Our research offers a practical approach for producing efficient WBG PSCs and tandem solar cells.

Functionalized wide-bandgap photoanode via dimensional design using amine fluoride salt to maximize the performance of perovskite solar cells

For Wide-bandgap (WBG) perovskite solar cells (PSCs), severe open-circuit voltage loss (Vloss) and device stability limit its photovoltaic performance. Dimensional design has been considered as a potential way to construct more efficient perovskite photoanodes. Herein, this article introduces 3-(trifluoromethyl) phenethylamine hydroiodide (CF3PEAI) to form dimensionally graded perovskite film was fabricated with 2D (two dimensional) CF3PEA2PbI4 forming on the 3D(three dimensional) perovskite layer. Studies have found that the deposited 2D perovskite can effectively regulate the energy level with minimized mismatch. Besides the functional groups in CF3PEAI can deactivate varieties of traps in perovskite through various interactions such as coordination of I- with Pb2+, hydrogen bonding of CF3 with formamidine, and ionic interactions of NH3+ with lead halide anions, thereby reducing the charge carrier recombination at the interface, and promoting the hole transfer from perovskite to Spiro-OMeTAD. Consequently, the resulting WBG perovskite(1.75 eV) system obtained a high open-circuit voltage of 1.29 V, with power conversion efficiency (PCE) increased from 16.12% to 18.70%. In addition, the wet stability of the WBG PSCs is significantly improved due to the fluorination effect of 2D perovskite for isolating water and oxygen.

Defect passivation and carrier management via a multifunctional additive for efficient and stable wide-bandgap perovskite solar cells with high fill factor

Wide-bandgap (WBG) Methylammonium (MA)-free based perovskite solar cells (PSCs) have attracted widespread research interests due to their broad applicability in multijunction tandem. Nevertheless, the efficiency of WBG PSCs is restricted by unfulfilled potential in fill factor and large deficits in open-circuit voltage. The imbalanced carrier mobility not only plays a critical role in bulk non-radiative recombination loss but also hinders efficient charge collection for mixed I/Br WBG perovskites. Herein, we introduced additive named 2,8-Diiododibenzothiophene to overcome above issues. Inverted devices with enhanced photostability and a record fill factor of 85.7 % are demonstrated. Moreover, combining the semitransparent WBG PSCs with 1.25 eV-bandgap perovskite bottom cells, we realized 4-terminal tandem devices and a champion PCE of 28 % is achieved. The multifunctional additive strategy demonstrated here, will open new avenues for improving WBG PSCs’ performance.