In perovskite solar cells, the interfaces between the perovskite and charge-transporting layers contain high concentrations of defects (about 100 times that within the perovskite layer), specifically, deep-level defects, which substantially reduce the power conversion efficiency of the devices1–3. Recent efforts to reduce these interfacial defects have focused mainly on surface passivation4–6. However, passivating the perovskite surface that interfaces with the electron-transporting layer is difficult, because the surface-treatment agents on the electron-transporting layer may dissolve while coating the perovskite thin film. Alternatively, interfacial defects may not be a concern if a coherent interface could be formed between the electron-transporting and perovskite layers. Here we report the formation of an interlayer between a SnO2 electron-transporting layer and a halide perovskite light-absorbing layer, achieved by coupling Cl-bonded SnO2 with a Cl-containing perovskite precursor. This interlayer has atomically coherent features, which enhance charge extraction and transport from the perovskite layer, and fewer interfacial defects. The existence of such a coherent interlayer allowed us to fabricate perovskite solar cells with a power conversion efficiency of 25.8 per cent (certified 25.5 per cent)under standard illumination. Furthermore, unencapsulated devices maintained about 90 per cent of their initial efficiency even after continuous light exposure for 500 hours. Our findings provide guidelines for designing defect-minimizing interfaces between metal halide perovskites and electron-transporting layers. An atomically coherent interlayer between the electron-transporting and perovskite layers in perovskite solar cells enhances charge extraction and transport from the perovskite, enabling high power conversion efficiency.

Perovskite solar cells with atomically coherent interlayers on SnO2 electrodes.

A stable perovskite heterojunction was constructed for inverted solar cells through surface sulfidation of lead (Pb)–rich perovskite films. The formed lead-sulfur (Pb-S) bonds upshifted the Fermi level at the perovskite interface and induced an extra back-surface field for electron extraction. The resulting inverted devices exhibited a power conversion efficiency (PCE) >24% with a high open-circuit voltage of 1.19 volts, corresponding to a low voltage loss of 0.36 volts. The strong Pb-S bonds could stabilize perovskite heterojunctions and strengthen underlying perovskite structures that have a similar crystal lattice. Devices with surface sulfidation retained more than 90% of the initial PCE after aging at 85°C for 2200 hours or operating at the maximum power point under continuous illumination for 1000 hours at 55° ± 5°C. Description Inverted solar cells’ surface sulfidation Perovskite solar cells (PSCs) with high power conversion efficiency (PCE) and stability have been reported in regular n-i-p devices, but inverted p-i-n PSCs that could be easier to use in tandem solar cells usually have lower PCEs (22 to 23%) Li et al. sulfurized a lead-rich layer with hexamethyldisilathiane, and the lead-sulfur bonds shifted the Fermi level of perovskite-transporter layer interface to create an electric field that enhanced electron extraction. The inverted PSCs had PCEs >24%, and the strong lead-sulfur bonds helped to maintain >90% of this efficiency during illuminated operation for 1000 hours at 55°C and after dark aging at 85°C for 2200 hours. —PDS Surface sulfidation of perovskite film increases its stability and improves electron extraction through band bending.

Constructing heterojunctions by surface sulfidation for efficient inverted perovskite solar cells

As the most promising lead-free one, tin-halides based perovskite solar cells still suffer from the severe bulk-defect due to the easy oxidation of tin from divalent to tetravalent. Here, a general and effective strategy is delivered to modulate the microstructure of 2D/3D heterogeneous tin-perovskite absorber films by substituting FAI with FPEABr in FASnI3 . The introduction of 2D phase can induce highly oriented growth of 3D FASnI3 and it is revealed in the optimal 2D/3D film that 2D phase embraces 3D grains and locates at the surfaces and grain boundaries. The FPEA+ based 2D tin-perovskite capping layer can offer a reducing atmosphere for vulnerable 3D FASnI3 grains. The unique microstructure effectively suppresses the well-known oxidation from Sn2+ to Sn4+ , as well as decreasing defect density, which leads to a remarkable enhanced device performance from 9.38% to 14.81% in conversion efficiency. The certified conversion efficiency of 14.03% announces a new record and moves a remarkable step from the last one (12.4%). Besides of this breakthrough, this work definitely paves a new way to fabricate high-quality tin-perovskite absorber film by constructing effective 2D/3D microstructures.

Heterogeneous 2D/3D Tin-Halides Perovskite Solar Cells with Certified Conversion Efficiency Breaking 14.

Owing to their insufficient light absorption and charge transport, 2D Ruddlesden-Popper (RP) perovskites show relatively low efficiency. In this work, methylammonium (MA), formamidinum (FA), and FA/MA mixed 2D perovskite solar cells (PSCs) are fabricated. Incorporating FA cations extends the absorption range and enhances the light absorption. Optical spectroscopy shows that FA cations substantially increase the portion of 3D-like phase to 2D phases, and X-ray diffraction (XRD) studies reveal that FA-based 2D perovskite possesses an oblique crystal orientation. Nevertheless, the ultrafast interphase charge transfer results in an extremely long carrier-diffusion length (≈1.98 µm). Also, chloride additives effectively suppress the yellow δ-phase formation of pure FA-based 2D PSCs. As a result, both FA/MA mixed and pure FA-based 2D PSCs exhibit a greatly enhanced power conversion efficiency (PCE) over 20%. Specifically, the pure FA-based 2D PSCs achieve a record PCE of 21.07% (certified at 20%), which is the highest efficiency for low-dimensional PSCs (n ≤ 10) reported to date. Importantly, the FA-based 2D PSCs retain 97% of their initial efficiency at 85 °C persistent heating after 1500 h. The results unambiguously demonstrate that pure-FA-based 2D PSCs are promising for achieving comparable efficiency to 3D perovskites, along with a better device stability.

Over 21% Efficiency Stable 2D Perovskite Solar Cells

This work provides an efficient way to facilitate both electron and hole extraction in the designated interfaces of perovskite solar cells. A record power conversion efficiency of 23.6% for mixed Sn–Pb perovskite solar cell devices is realized. 

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Optimized carrier extraction at interfaces for 23.6% efficient tin–lead perovskite solar cells

The stabilization of black-phase formamidinium lead iodide (α-FAPbI3) perovskite under various environmental conditions is considered necessary for solar cells. However, challenges remain regarding the temperature sensitivity of α-FAPbI3 and the requirements for strict humidity control in its processing. Here we report the synthesis of stable α-FAPbI3, regardless of humidity and temperature, based on a vertically aligned lead iodide thin film grown from an ionic liquid, methylamine formate. The vertically grown structure has numerous nanometer-scale ion channels that facilitate the permeation of formamidinium iodide into the lead iodide thin films for fast and robust transformation to α-FAPbI3 A solar cell with a power-conversion efficiency of 24.1% was achieved. The unencapsulated cells retain 80 and 90% of their initial efficiencies for 500 hours at 85°C and continuous light stress, respectively.

Stabilizing black-phase formamidinium perovskite formation at room temperature and high humidity.

A‐Site Cation Engineering of Metal Halide Perovskites: Version 3.0 of Efficient Tin‐Based Lead‐Free Perovskite Solar Cells

Architecture of p-i-n Sn-Based Perovskite Solar Cells: Characteristics, Advances, and Perspectives

Crystallization Dynamics of Sn-Based Perovskite Thin Films: Toward Efficient and Stable Photovoltaic Devices

Recently, the power conversion efficiency (PCE) of perovskite solar cells (PSC) based on organic-inorganic hybrid Pb halide perovskites has reached 25.2 %. However, the toxicity of Pb has still been a main concern for the large-scale commercialization of Pb-based PSCs. Efforts have been made during the past few years to seek eco-friendly Pb-free perovskites, and it is a growing consensus that Sn is the best choice as Pb alternative over any other Pb-free metal elements. Among Sn-based perovskites, all-inorganic cells are promising candidates for PSCs owing to their more suitable bandgap, better stability, and higher charge mobility compared to the organic-inorganic hybrid counterparts. However, the poor phase stability of all-inorganic Sn-based perovskites (AISPs) and low PCE of their PSCs are most challenging in the field at present. Herein, recent developments on PSCs based on AISPs, including CsSnX3 and Cs2 SnX6 (X=Br, I), are comprehensively reviewed. Primarily, the intrinsic characteristics of the two AISPs are overviewed, including crystallographic property, band structure, charge carrier property, and defect property. Sequentially, state-of-the-art progress, regarding the photovoltaic application of AISPs as light absorber, is summarized. At last, current challenges and future opportunities of AISP-based PSCs are also discussed.

He Dong

Papers

Stabilizing black-phase formamidinium perovskite formation at room temperature and high humidity.

A‐Site Cation Engineering of Metal Halide Perovskites: Version 3.0 of Efficient Tin‐Based Lead‐Free Perovskite Solar Cells

Architecture of p-i-n Sn-Based Perovskite Solar Cells: Characteristics, Advances, and Perspectives

Crystallization Dynamics of Sn-Based Perovskite Thin Films: Toward Efficient and Stable Photovoltaic Devices

All-inorganic Sn-based Perovskite Solar Cells: Status, Challenges, and Perspectives.