δ‐CsPbI3 Intermediate Phase Growth Assisted Sequential Deposition Boosts Stable and High‐Efficiency Triple Cation Perovskite Solar Cells

Cs/FA/MA triple cation perovskite films have been well developed in the antisolvent dripping method, attributable to its outstanding photovoltaic and stability performances. However, a facile and effective strategy is still lacking for fabricating high‐quality large‐grain triple cation perovskite films via sequential deposition method a, which is one of the key technologies for high efficiency perovskite solar cells. To address this issue, a δ‐CsPbI₃ intermediate phase growth (CsPbI₃‐IPG) assisted sequential deposition method is demonstrated for the first time. The approach not only achieves incorporation of controllable cesium into (FAPbI₃)_1–x(MAPbBr₃)_x perovskite, but also enlarges the perovskite grains, manipulates the crystallization, modulates the bandgap, and improves the stability of final perovskite films. The photovoltaic performances of the devices based on these Cs/FA/MA perovskite films with various amounts of the δ‐CsPbI₃ intermediate phase are investigated systematically. Benefiting from moderate cesium incorporation and intermediate phase‐assisted grain growth, the optimized Cs/FA/MA perovskite solar cells exhibit a significantly improved power conversion efficiency and operational stability of unencapsulated devices. This facile strategy provides new insights into the compositional engineering of triple or quadruple cation perovskite materials with enlarged grains and superior stability via a sequential deposition method.     

Short‐Chain Ligand‐Passivated Stable α‐CsPbI3 Quantum Dot for All‐Inorganic Perovskite Solar Cells

Cubic phase CsPbI₃ (α‐CsPbI₃) perovskite quantum dots (QDs) have received extensive attention due to their all‐inorganic composition and suitable band gap (1.73 eV). However, α‐CsPbI₃ QDs might convert to δ‐CsPbI₃ (orthorhombic phase with indirect band gap of 2.82 eV) due to easy loss of surface ligands. In addition, commonly used long‐chain ligands (oleic acid, OA, and oleylamine, OLA) hinder efficient charge transport in optoelectronic devices. In order to relieve these drawbacks, OA, OLA, octanoic acid, and octylamine are used as capping ligands for synthesizing high‐quality α‐CsPbI₃ QDs. The results indicate that these QDs exhibit excellent optical properties and long‐term stability compared to QDs capped only with OA and OLA. Moreover, QDs with shorter ligands exhibit an enhanced charge transport rate, which improves the power conversion efficiency of photovoltaic devices from 7.76% to 11.87%.     

Chromium-Based Metal–Organic Framework as A-Site Cation in CsPbI2Br Perovskite Solar Cells

Inorganic CsPbI_xBr_3−x perovskite solar cells (PSCs) have gained enormous interest due to their excellent thermal stabilities. However, their intrinsically poor moisture stability hampers their further development. Herein, a chromium-based metal–organic framework group is intercalated inside the inorganic Pb I framework, resulting in a new multiple-dimensional electronically coupled CsPbI₂Br perovskite. In this structurally and electronically coupled perovskite, the π-conjugated terpyridyl can delocalize the excited valence electrons of metal Cr³⁺ ion, enabling multi-interactive charge-carrier transport channels within CsPbI₂Br perovskites. The stability and efficiency of the produced devices are substantially enhanced in comparison to their counterparts with only a pristine CsPbI₂Br active layer. The optimized all-inorganic PSC yields a power conversion efficiency (PCE) as high as 17.02%. Remarkably, the stabilized device retains 80% of its PCE after 1000 h in the ambient atmosphere. This study provides a new paradigm toward addressing the stability challenge of the inorganic perovskite while enhancing its carrier transport ability.     

Highly-Stable CsPbI3 Perovskite Solar Cells with an Efficiency of 21.11% via Fluorinated 4-Amino-Benzoate Cesium Bifacial Passivation

The poor interface quality between cesium lead triiodide (CsPbI₃) perovskite and the electron transport layer limits the stability and efficiency of CsPbI₃ perovskite solar cells (PSCs). Herein, a 4-amino-2,3,5,6-tetrafluorobenzoate cesium (ATFC) is designed as a bifacial defect passivator to tailor the perovskite/TiO₂ interface. The comprehensive experiments demonstrate that ATFC can not only optimize the conductivity, electron mobility, and energy band structure of the TiO₂ layer by passivation of the undercoordinated Ti⁴⁺, oxygen vacancy (V_O), and free  OH defects but also promote the yield of high-quality CsPbI₃ film by synergistic passivation of undercoordinated Pb²⁺ defects with the  CO group and F atom, and limiting I⁻ migration via F···I interaction. Benefiting from the above interactions, the ATFC-modified CsPbI₃ device yields a champion power conversion efficiency (PCE) of 21.11% and an excellent open-circuit voltage (V_OC) of 1.24 V. Meanwhile, the optimized CsPbI₃ PSC maintains 92.74% of its initial efficiency after aging 800 h in air atmosphere, and has almost no efficiency attenuation after tracking at maximum power point for 350 h.     

2D/3D Heterostructure for Semitransparent Perovskite Solar Cells with Engineered Bandgap Enables Efficiencies Exceeding 25% in Four‐Terminal Tandems with Silicon and CIGS

Wide‐bandgap perovskite solar cells (PSCs) with optimal bandgap (E_g) and high power conversion efficiency (PCE) are key to high‐performance perovskite‐based tandem photovoltaics. A 2D/3D perovskite heterostructure passivation is employed for double‐cation wide‐bandgap PSCs with engineered bandgap (1.65 eV ≤ E_g ≤ 1.85 eV), which results in improved stabilized PCEs and a strong enhancement in open‐circuit voltages of around 45 mV compared to reference devices for all investigated bandgaps. Making use of this strategy, semitransparent PSCs with engineered bandgap are developed, which show stabilized PCEs of up to 25.7% and 25.0% in four‐terminal perovskite/c‐Si and perovskite/CIGS tandem solar cells, respectively. Moreover, comparable tandem PCEs are observed for a broad range of perovskite bandgaps. For the first time, the robustness of the four‐terminal tandem configuration with respect to variations in the perovskite bandgap for two state‐of‐the‐art bottom solar cells is experimentally validated.     

Controlled n‐Doping in Air‐Stable CsPbI2Br Perovskite Solar Cells with a Record Efficiency of 16.79%

Cesium‐based inorganic perovskites, such as CsPbI₂Br, are promising candidates for photovoltaic applications owing to their exceptional optoelectronic properties and outstanding thermal stability. However, the power conversion efficiency of CsPbI₂Br perovskite solar cells (PSCs) is still lower than those of hybrid PSCs and inorganic CsPbI₃ PSCs. In this work, passivation and n‐type doping by adding CaCl₂ to CsPbI₂Br is demonstrated. The crystallinity of the CsPbI₂Br perovskite film is enhanced, and the trap density is suppressed after adding CaCl₂. In addition, the Fermi level of the CsPbI₂Br is changed by the added CaCl₂ to show heavy n‐type doping. As a result, the optimized CsPbI₂Br PSC shows a highest open circuit voltage of 1.32 V and a record efficiency of 16.79%. Meanwhile, high air stability is demonstrated for a CsPbI₂Br PSC with 90% of the initial efficiency remaining after more than 1000 h aging in air.     

Stable α‐CsPbI3 Perovskite Nanowire Arrays with Preferential Crystallographic Orientation for Highly Sensitive Photodetectors

All‐inorganic metal‐halide perovskites CsPbX₃ (X = Cl, Br, I) exhibit higher stability than their organic–inorganic hybrid counterparts, but the thermodynamically instable perovskite α phase at room temperature of CsPbI₃ restricts the practical optoelectronic applications. Although the stabilization of α‐CsPbI₃ polycrystalline thin films is extensively studied, the creation of highly crystalline micro/nanostructures of α‐CsPbI₃ with large grain size and suppressed grain boundary remains challenging, which impedes the implementations of α‐CsPbI₃ for lateral devices, such as photoconductor‐type photodetectors. In this work, stable α‐CsPbI₃ perovskite nanowire arrays are demonstrated with large grain size, high crystallinity, regulated alignment, and position by controlling the dewetting dynamics of precursor solution on an asymmetric‐wettability topographical template. The correlation between the higher photoluminescence (PL) intensity and longer PL lifetime indicates the nanowires exhibit stable α phase and suppressed trap density. The preferential (100) orientation is characterized by discrete diffraction spots in grazing incidence wide‐angle scattering patterns, suggesting the long‐range crystallographic order of these nanowires. Based on these high‐quality nanowire arrays, highly sensitive photodetectors are realized with a responsivity of 1294 A W^?1 and long‐term stability with 90% performance retention after 30‐day ambient storage.     

Inorganic Ammonium Halide Additive Strategy for Highly Efficient and Stable CsPbI3 Perovskite Solar Cells

All-inorganic perovskite cesium lead iodide (CsPbI₃) exhibits excellent prospects for commercial application as a light absorber in single-junction or tandem solar cells due to its outstanding thermal stability and proper bandgap. However, the device performance of CsPbI₃-based perovskite solar cells (PSCs) is still restricted by the unsatisfactory crystal quality and severe non-radiative recombination. Herein, inorganic additive ammonium halides are introduced into the precursor solution to regulate the nucleation and crystallization of the CsPbI₃ film by exploiting the atomic interaction between the ammonium group and the Pb–I framework. The grain boundaries and interfacial contact of the CsPbI₃ film have been improved, which leads to significant suppression in the non-radiative recombination and an enhancement in the charge transport ability. With these benefits, a high efficiency of 18.7% together with an extraordinarily high fill factor of 0.83–0.84 has been achieved, comparable to the highest records reported so far. Moreover, the cell exhibits ultra-high photoelectrical stability under continuous light illumination and high bias voltage with 96% of its initial power-conversion efficiency being sustained after 2000 h operation, even superior to the world-champion CsPbI₃ solar cell. The findings are promising for the development and application of all-inorganic PSCs using a simple inorganic additive strategy.     

Buried Interface Modulation via Preferential Crystallization in All-Inorganic Perovskite Solar Cells: The Case of Multifunctional Ti3C2Tx

Despite inorganic CsPbI_3−xBr_x perovskite solar cells (PSCs) being promising in thermal stability, the perovskite degradation and severe nonradiative recombination at the interface hamper their further development. Herein, the typical MXene material, that is, Ti₃C₂T_x, is employed to be the buried interface prior to the perovskite absorber layer in the device, which multi-functionalizes the as-prepared electron-transfer layers by means of both fascinating preferential crystallization of perovskite and/or accelerating the charge extraction with respect to an ideal energy-level alignment and suppressed trap states. Accordingly, the power conversion efficiency of the modified PSC device is substantially enhanced by as high as 19.56% in comparison to their counterparts with only the pristine CsPbI_3−xBr_x active layer. More importantly, MXene modification is favorable to improve the wettability of perovskite precursor solution with enhanced grain size and crystallinity, thereby increasing the UV long-term stability of solar cells. This work provides a new paradigm toward alleviating the severe nonradiative recombination at the interface in the device whilst enhancing the long-term stability via the preferential crystallization process.     

Dual‐Phase All‐Inorganic Cesium Halide Perovskites for Conducting‐Bridge Memory‐Based Artificial Synapses

Neuromorphic computing, which mimics biological neural networks, can overcome the high‐power and large‐throughput problems of current von Neumann computing. Two‐terminal memristors are regarded as promising candidates for artificial synapses, which are the fundamental functional units of neuromorphic computing systems. All‐inorganic CsPbI₃ perovskite‐based memristors are feasible to use in resistive switching memory and artificial synapses due to their fast ion migration. However, the ideal perovskite phase α‐CsPbI₃ is structurally unstable at ambient temperature and rapidly degrades to a non‐perovskite δ‐CsPbI₃ phase. Here, dual‐phase (Cs₃Bi₂I₉)_0.4?(CsPbI₃)_0.6 is successfully fabricated to achieve improved air stability and surface morphology compared to each single phase. Notably, the Ag/polymethylmethacrylate/(Cs₃Bi₂I₉)_0.4?(CsPbI₃)_0.6/Pt device exhibits non‐volatile memory functions with an endurance of ≈10³ cycles and retention of ≈10⁴ s with low operation voltages. Moreover, the device successfully emulates synaptic behavior such as long‐term potentiation/depression and spike timing/width‐dependent plasticity. This study will contribute to improving the structural and mechanical stability of all‐inorganic halide perovskites (IHPs) via the formation of dual phase. In addition, it proves the great potential of IHPs for use in low‐power non‐volatile memory devices and electronic synapses.     

Constructing All-Inorganic Perovskite/Fluoride Nanocomposites for Efficient and Ultra-Stable Perovskite Solar Cells

Organic-inorganic hybrid perovskite solar cells (PSCs) have rapidly developed over the past decade and have achieved the latest certified power conversion efficiency (PCE) up to 25.5%. However, unsatisfactory long-term operational stability for these hybrid PSCs remains a huge obstacle to further development and commercialization. Herein, a unique hetero-structured CsPbI₃/CaF₂ perovskite/fluoride nanocomposites (PFNCs) is fabricated via a newly developed facile two-step hetero-epitaxial growth strategy to deliver efficient and ultra-stable PSCs. After being incorporated into the crystal lattice of α-phase CsPbI₃ perovskite, the cubic-phase CaF₂ in the resultant CsPbI₃/CaF₂ PFNCs can not only passivate the intrinsic defects of CsPbI₃ perovskite itself but also effectively suppress the notorious ion migration in hybrid perovskite Cs_0.05FA_0.81MA_0.14PbI_2.55Br_0.45 (CsFAMA) thin-films of PSCs. As such, the CsFAMA PSC devices based on CsPbI₃/CaF₂-deposited perovskite thin-film achieve a mean PCE of 20.45%, in sharp contrast to 19.33% of the control devices without deposition. Specifically, the CsPbI₃/CaF₂-deposited PSC retains 85% of its original PCE after 1000 h continuous operation at the maximum power point under AM 1.5G solar light, far better than those of the control and CsPbI₃-deposited PSCs with a device T₈₅ lifetime of 315 and 125 h, respectively.     

Precursor Engineering for All‐Inorganic CsPbI2Br Perovskite Solar Cells with 14.78% Efficiency

The optoelectronic properties of perovskite films are closely related to the film quality, so depositing dense, uniform, and stable perovskite films is crucial for fabricating high‐performance perovskite solar cells (PSCs). CsPbI₂Br perovskite, prized for its superb stability toward light soaking and thermal aging, has received a great deal of attention recently. However, the air instability and poor performance of CsPbI₂Br PSCs are hindering its further progress. Here, an approach is reported for depositing high‐quality CsPbI₂Br films via the Lewis base adducts PbI₂(DMSO) and PbBr₂(DMSO) as precursors to slow the crystallization of the perovskite film. This process produces CsPbI₂Br films with large‐scale crystalline grains, flat surfaces, low defects, and long carrier lifetimes. More interestingly, PbI₂(DMSO) and PbBr₂(DMSO) adducts could significantly improve the stability of CsPbI₂Br films in air. Using films prepared by this technique, a power conversion efficiency (PCE) of 14.78% is obtained in CsPbI₂Br PSCs, which is the highest PCE value reported for CsPbI₂Br‐based PSCs to date. In addition, the PSCs based on DMSO adducts show an extended operational lifetime in air. These excellent performances indicate that preparing high‐quality inorganic perovskite films by using DMSO adducts will be a potential method for improving the performance of other inorganic PSCs.     

All-Inorganic CsPbI3 Quantum Dot Solar Cells with Efficiency over 16% by Defect Control

All-inorganic CsPbI₃ quantum dots (QDs) have shown great potential in photovoltaic applications. However, their performance has been limited by defects and phase stability. Herein, an anion/cation synergy strategy to improve the structural stability of CsPbI₃ QDs and reduce the pivotal iodine vacancy (V_I) defect states is proposed. The Zn-doped CsPbI₃ (Zn:CsPbI₃) QDs have been successfully synthesized employing ZnI₂ as the dopant to provide Zn²⁺ and extra I⁻. Theoretical calculations and experimental results demonstrate that the Zn:CsPbI₃ QDs show better thermodynamic stability and higher photoluminescence quantum yield (PLQY) compared to the pristine CsPbI₃ QDs. The doping of Zn in CsPbI₃ QDs increases the formation energy and Goldschmidt tolerance factor, thereby improving the thermodynamic stability. The additional I⁻ helps to reduce the V_I defects during the synthesis of CsPbI₃ QDs, resulting in the higher PLQY. More importantly, the synergistic effect of Zn²⁺ and I⁻ in CsPbI₃ QDs can prevent the iodine loss during the fabrication of CsPbI₃ QD film, inhibiting the formation of new V_I defect states in the construction of solar cells. Consequently, the anion/cation synergy strategy affords the CsPbI₃ quantum dot solar cells (QDSC) a power conversion efficiency over 16%, which is among the best efficiencies for perovskite QDSCs.     

Perovskite‐Based Tandem Solar Cells: Get the Most Out of the Sun

Tandem solar cells (TSCs) comprising stacked narrow‐bandgap and wide‐bandgap subcells are regarded as the most promising approach to break the Shockley–Queisser limit of single‐junction solar cells. As the game‐changer in the photovoltaic community, organic–inorganic hybrid perovskites became the front‐runner candidate for mating with other efficient photovoltaic technologies in the tandem configuration for higher power conversion efficiency, by virtue of their tunable and complementary bandgaps, excellent photoelectric properties, and solution processability. In this review, a perspective that critically dilates the progress of perovskite material selection and device design for perovskite‐based TSCs, including perovskite/silicon, perovskite/copper indium gallium selenide, perovskite/perovskite, perovskite/CdTe, and perovskite/GaAs are presented. Besides, all‐inorganic perovskite CsPbI₃ with high thermal stability is proposed as the top subcell in TSCs due to its suitable bandgap of ≈1.73 eV and rapidly increasing efficiency. To minimize the optical and electrical losses for high‐efficiency TSCs, the optimization of transparent electrodes, recombination layers, and the current‐matching principles are highlighted. Through big data analysis, wide‐bandgap perovskite solar cells with high open‐circuit voltage (V_oc) are in dire need in further study. In the end, opportunities and challenges to realize the commercialization of TSCs, including long‐term stability, area upscaling, and mitigation of toxicity, are also envisioned.     

3D Polydentate Complexing Agents for Passivating Defects and Modulating Crystallinity for High-Performance Perovskite Solar Cells

The grain boundaries (GBs)/surface defects within perovskite film directly impede the further improvement of photoelectric conversion efficiency (PCE) and stability of planar perovskite solar cells (PSCs). Herein, 3D phytic acid (PA) and phytic acid dipotassium (PAD) with polydentate are explored to synchronously passivate the defects of perovskite absorber directly in multiple spatial directions. The strong electron-donating groups ( H₂PO₄) in the PA molecule afford six anchor sites to bind firmly with uncoordinated Pb²⁺ at the GBs/surface and modulate perovskite crystallization, thus enhancing the quality of perovskite film. Particularly, PAD containing an additional (K→PO) push–pull structure promotes the dominant coordination of phosphate group (PO) with Pb²⁺ and passivates halide anion defects due to the complexation of potassium ions (K⁺) with iodide ions (I^-). Consequently, the PAD-complexed PSCs deliver a champion PCE of 23.18%, which is remarkably higher than that of the control device (19.94%). Meanwhile, PAD-complexed PSCs exhibit superior moisture and thermal stability, remaining 79% of their initial PCE after 1000 h under continuous illumination, while the control device remain only 48% of their PCE after 1000 h. This work provides important insights into designing multifunctional 3D passivators for the purpose of simultaneously enhancing the efficiency and stability of devices.     

NbF5: A Novel α‐Phase Stabilizer for FA‐Based Perovskite Solar Cells with High Efficiency

The HC(NH₂)₂⁺(FA⁺) is a well‐known substitute to CH₃NH₃⁺(MA⁺) for its capability to extend light utilization for improved power conversion efficiency for perovskite solar cells; unfortunately, the dark cubic phase (α‐phase) can easily transition to the yellow orthorhombic phase (δ‐phase) at room temperature, an issue that prevents its commercial application. In this report, an inorganic material (NbF₅) is developed to stabilize the desired α‐phase perovskite material by incorporating NbF₅ additive into the perovskite films. It is found that the NbF₅ additive effectively suppresses the formation of the yellow δ‐phase in the perovskite synthesis and aging process, thus enhancing the humidity and light‐soaking stability of the perovskite film. As a result, the perovskite solar cells with the NbF₅ additive exhibit improved air stability by tenfold, retaining nearly 80% of their initial efficiency after aging in air for 50 d. In addition, under full‐sun AM 1.5 G illumination of a xenon lamp without any UV‐reduction, the perovskite solar cells with the NbF₅ additive also show fivefold improved illumination stability than the control devices without NbF₅.     

All‐Inorganic CsPbI3 Perovskite Phase‐Stabilized by Poly(ethylene oxide) for Red‐Light‐Emitting Diodes

Despite the excellent photoelectronic properties of the all‐inorganic cesium lead iodide (CsPbI₃) perovskite, which does not contain volatile and hygroscopic organic components, only a few CsPbI₃ devices are developed mainly owing to the frequent formation of an undesirable yellow δ‐phase at room temperature. Herein, it is demonstrated that a small quantity of poly(ethylene oxide) (PEO) added to the precursor solution effectively inhibits the formation of the yellow δ‐phase during film preparation, and promotes the development of a black α‐phase at a low crystallization temperature. A systematic study reveals that a thin, dense, pinhole‐free CsPbI₃ film is produced in the α‐phase and is stabilized with PEO that effectively reduces the grain size during crystallization. A thin α‐phase CsPbI₃ film with excellent photoluminescence is successfully employed in a light‐emitting diode with an inverted configuration of glass substrate/indium tin oxide/zinc oxide/poly(ethyleneimine)/α‐CsPbI₃/poly(4‐butylphenyl‐diphenyl‐amine)/WO₃/Al, yielding the characteristic red emission of the perovskite film at 695 nm with brightness, external quantum efficiency, and emission band width of ≈101 cd m^?2, 1.12%, and 32 nm, respectively.     

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.     

Uniform Stepped Interfacial Energy Level Structure Boosts Efficiency and Stability of CsPbI2Br Solar Cells

All-inorganic CsPbI₂Br perovskite has attracted great attention as an absorber for perovskite solar cells (PSCs) due to its excellent thermal and light resistance. However, its device performance is restricted by the large energy level offset between CsPbI₂Br and the most commonly used hole-transporting layer (HTL). Herein, multicarbazolyl-substituted benzonitrile (4t-5CzBn) is inserted into the interface between CsPbI₂Br and HTL to form a uniform stepped (0.24 eV) interfacial energy level structure, which reduces the energy loss and boosts the hole extraction of CsPbI₂Br PSCs. The incorporation of 4t-5CzBn induces the increase in open-circuit voltage and fill factor from 1.256 V and 74.5% to 1.335 V and 82.3%, respectively. The optimized device achieves a power conversion efficiency of 17.34%, which is among the highest reported values of CsPbI₂Br PSCs. Besides the energy level tuning effect, the tert-butyl groups in 4t-5CzBn improve the moisture-resistance of CsPbI₂Br PSCs. The unencapsulated device maintains over 75% of its initial efficiency after 700 h storage in air. These results demonstrate that the rational tuned energy level step benefits the performance improvement of CsPbI₂Br PSCs.     

Modification of Energy Level Alignment for Boosting Carbon-Based CsPbI2Br Solar Cells with 14% Certified Efficiency

Hole transfer material (HTM)-free, carbon-based all-inorganic perovskite solar cells (C-PSCs) are promising alternatives to conventional organic–inorganic hybrid PSCs in addressing thermal and moisture instability issues. However, the energy level mismatch between the inorganic perovskite and carbon electrode coupled, together with the incapability of the carbon electrode to reflect incident light for reabsorption, limits the power conversion efficiency (PCE) of C-PSCs. To address these issues, herein, a new strategy of a hexyltrimethylammonium bromide (HTAB)-modified CsPbI₂Br perovskite surface is devised to reduce this energy offset from 0.70 to 0.32 eV and increase the built-in potential by 70 mV for the final devices. Additionally, a CsPbI₂Br perovskite film with a thickness of up to 800 nm is realized via a hot-flow-assisted spin coating approach in an ambient atmosphere with humidity of less than 80%. Reduced energy offset coupled with suppressed charge recombination and thick perovskite layer boosts the champion PCE of CsPbI₂Br C-PSCs to 14.3% (J_sc = 14.1 mA cm⁻², V_oc = 1.26 V, and fill factor = 0.806), and the average PCE to 13.9% under one sun illumination. A new certified efficiency record of 14.0% is obtained for HTM-free inorganic C-PSCs. Meanwhile, the moisture-resistant barrier from the alkyl chain in HTAB improves the stability of the final devices.