Photovoltaic solar cells based on metal halide perovskites have gained considerable attention over the past decade because of their potentially low production cost, earth-abundant raw materials, ease of fabrication and ever-increasing power conversion efficiencies of up to 25.2%. This type of solar cells offers the promise of generating electricity at a more competitive unit price than traditional fossil fuels by 2035. Nevertheless, the best research cell efficiencies are still below the theoretical limit defined by the Shockley-Queissier theory owing to the presence of non-radiative recombination losses. In this Review, we analyse the predominant pathways that contribute to non-radiative recombination losses in perovskite solar cells, and evaluate their impact on device performance. We then discuss how non-radiative recombination losses can be estimated through reliable characterization techniques, and highlight some notable advances in mitigating these losses, which hint at pathways towards defect-free perovskite solar cells. Finally, we outline directions for future work that will push the efficiency of perovskite solar cells towards the radiative limit.

Minimizing non-radiative recombination losses in perovskite solar cells

Two-dimensional (2D) perovskites have attracted considerable interest for their promising applications for solar cells and other optoelectronics, such as light-emitting diodes, spintronics, and photodetectors. Here, we review the recent achievements of 2D perovskites for various optoelectronic applications. First, we discuss the basic structure and optoelectronic properties of 2D perovskites, including band structure, optical properties, and charge transport. We then highlight recent achievements using 2D perovskites in solar cells and beyond solar cells, including progress on various synthesis strategies and their impact on structural and optoelectronic properties. Finally, we discuss current challenges and future opportunities to further develop 2D perovskites for various applications.

Advances in two-dimensional organic–inorganic hybrid perovskites

Two-dimensional (2D) halide perovskites have emerged as outstanding semiconducting materials thanks to their superior stability and structural diversity. However, the ever-growing field of optoelectronic device research using 2D perovskites requires systematic understanding of the effects of the spacer on the structure, properties, and device performance. So far, many studies are based on trial-and-error tests of random spacers with limited ability to predict the resulting structure of these synthetic experiments, hindering the discovery of novel 2D materials to be incorporated into high-performance devices. In this review, we provide guidelines on successfully choosing spacers and incorporating them into crystalline materials and optoelectronic devices. We first provide a summary of various synthetic methods to act as a tutorial for groups interested in pursuing synthesis of novel 2D perovskites. Second, we provide our insights on what kind of spacer cations can stabilize 2D perovskites followed by an extensive review of the spacer cations, which have been shown to stabilize 2D perovskites with an emphasis on the effects of the spacer on the structure and optical properties. Next, we provide a similar explanation for the methods used to fabricate films and their desired properties. Like the synthesis section, we will then focus on various spacers that have been used in devices and how they influence the film structure and device performance. With a comprehensive understanding of these effects, a rational selection of novel spacers can be made, accelerating this already exciting field.

The 2D Halide Perovskite Rulebook: How the Spacer Influences Everything from the Structure to Optoelectronic Device Efficiency.

Passivating surface and bulk defects of perovskite films has been proven to be an effective way to minimize nonradiative recombination losses in perovskite solar cells (PVSCs). The lattice interference and perturbation of atomic periodicity at the perovskite surfaces often significantly affect the material properties and device efficiencies. By tailoring the terminal groups on the perovskite surface and modifying the surface chemical environment, the defects can be reduced to enhance the photovoltaic performance and stability of derived PVSCs. Here, we report a rationally designed bifunctional molecule, piperazinium iodide (PI), containing both R2NH and R2NH2+ groups on the same six-membered ring, behaving both as an electron donor and an electron acceptor to react with different surface-terminating ends on perovskite films. The resulting perovskite films after defect passivation show released surface residual stress, suppressed nonradiative recombination loss, and more n-type characteristics for sufficient energy transfer. Consequently, charge recombination is significantly suppressed to result in a high open-circuit voltage (VOC) of 1.17 V and a reduced VOC loss of 0.33 V. A very high power conversion efficiency (PCE) of 23.37% (with 22.75% certified) could be achieved, which is the highest value reported for inverted PVSCs. Our work reveals a very effective way of using rationally designed bifunctional molecules to simultaneously enhance the device performance and stability.

Regulating Surface Termination for Efficient Inverted Perovskite Solar Cells with Greater Than 23% Efficiency

Further enhancing the performance and stability of inverted perovskite solar cells (PSCs) is crucial for their commercialization. We report that the functionalization of multication and halide perovskite interfaces with an organometallic compound, ferrocenyl-bis-thiophene-2-carboxylate (FcTc2), simultaneously enhanced the efficiency and stability of inverted PSCs. The resultant devices achieved a power conversion efficiency of 25.0% and maintained >98% of their initial efficiency after continuously operating at the maximum power point for 1500 hours under simulated AM1.5 illumination. Moreover, the FcTc2-functionalized devices passed the international standards for mature photovoltaics (IEC61215:2016) and have exhibited high stability under the damp heat test (85°C and 85% relative humidity). Description Organometallics stabilizing perovskites Perovskite solar cells with inverted (p-i-n) structure can have greater stability and lifetimes than conventional n-i-p structures but usually have somewhat lower power conversion efficiencies (PCEs). Li et al. report that an organometallic compound, ferrocenyl-bis-thiophene-2-carboxylate, can stabilize a multication perovskite layer of an inverted perovskite solar cells. After 1500 hours of maximum power point operation, 98% of the 25.0% PCE was maintained. The solar cell also exhibited high stability in damp heat tests. —PDS Functionalizing interfaces with an organometallic compound created an efficient and stable inverted perovskite solar cell.

Organometallic-functionalized interfaces for highly efficient inverted perovskite solar cells

Despite the notable progress in perovskite solar cells, maintaining long-term operational stability and minimizing potentially leaked lead (Pb2+) ions are two challenges that are yet to be resolved. Here we address these issues using a thiol-functionalized 2D conjugated metal–organic framework as an electron-extraction layer at the perovskite/cathode interface. The resultant devices exhibit high power conversion efficiency (22.02%) along with a substantially improved long-term operational stability. The perovskite solar cell modified with a metal–organic framework could retain more than 90% of its initial efficiency under accelerated testing conditions, that is continuous light irradiation at maximum power point tracking for 1,000 h at 85 °C. More importantly, the functionalized metal–organic framework could capture most of the Pb2+ leaked from the degraded perovskite solar cells by forming water-insoluble solids. Therefore, this method that simultaneously tackles the operational stability and lead contamination issues in perovskite solar cells could greatly improve the feasibility of large-scale deployment of perovskite photovoltaic technology. Two-dimensional conjugated metal–organic frameworks used as an electron-extraction layer enable the realization of highly stable perovskite solar cells with minimized lead ion leakage.

Tiantian Liu

Papers

2D metal-organic framework for stable perovskite solar cells with minimized lead leakage

Efficient large guanidinium mixed perovskite solar cells with enhanced photovoltage and low energy losses

Boosting Photovoltaic Performance for Lead Halide Perovskites Solar Cells with BF4− Anion Substitutions

Vertical Orientated Dion–Jacobson Quasi-2D Perovskite Film with Improved Photovoltaic Performance and Stability

Modifying Surface Termination of CsPbI3 Grain Boundaries by 2D Perovskite Layer for Efficient and Stable Photovoltaics