Tandem solar cells that pair silicon with a metal halide perovskite are a promising option for surpassing the single-cell efficiency limit. We report a monolithic perovskite/silicon tandem with a certified power conversion efficiency of 29.15%. The perovskite absorber, with a bandgap of 1.68 electron volts, remained phase-stable under illumination through a combination of fast hole extraction and minimized nonradiative recombination at the hole-selective interface. These features were made possible by a self-assembled, methyl-substituted carbazole monolayer as the hole-selective layer in the perovskite cell. The accelerated hole extraction was linked to a low ideality factor of 1.26 and single-junction fill factors of up to 84%, while enabling a tandem open-circuit voltage of as high as 1.92 volts. In air, without encapsulation, a tandem retained 95% of its initial efficiency after 300 hours of operation.

The performance of perovskite solar cells (PSCs) is predominantly limited by non-radiative recombination, either through trap-assisted recombination in the absorber layer or via minority carrier recombination at the perovskite/transport layer interfaces. Here we use transient and absolute photoluminescence imaging to visualize all non-radiative recombination pathways in planar pin-type PSCs with undoped organic charge transporting layers. We find significant quasi-Fermi level splitting losses (135 meV) in the perovskite bulk, while interfacial recombination results in an additional free energy loss of 80 meV at each individual interface which limits the open-circuit voltage ( OC ) of the complete cell to ~1.12 V. Inserting ultrathin interlayers between the perovskite and transport layers allows substantial reduction of these interfacial losses at both the p and n contacts. Using this knowledge and approach, we demonstrate reproducible dopant-free 1 cm 2 PSCs surpassing 20% efficiency (19.83% certified) with stabilized power output, a high OC (1.17 V) and record fill factor (> 81%).

We quantify recombination losses in the bulk and interfaces for different perovskite compositions and popular charge transport layers.

Perovskite solar cells (PSCs) are currently one of the most promising photovoltaic technologies for highly efficient and cost-effective solar energy production. In only a few years, an unprecedented progression of preparation procedures and material compositions delivered lab-scale devices that have now reached record power conversion efficiencies (PCEs) higher than 20%, competing with most established solar cell materials such as silicon, CIGS, and CdTe. However, despite a large number of researchers currently involved in this topic, only a few groups in the world can reproduce >20% efficiencies on a regular n−i−p architecture. In this work, we present detailed protocols for preparing PSCs in regular (n−i−p) and inverted (p−i−n) architectures with ≥20% PCE. We aim to provide a comprehensive, reproducible description of our device fabrication protocols. We encourage the practice of reporting detailed and transparent protocols that can be more easily reproduced by other laboratories. A better reporting standard may, in turn, accelerate the development of perovskite solar cells and related research fields.

Organic solar cells are currently experiencing a second golden age thanks to the development of novel non‐fullerene acceptors (NFAs). Surprisingly, some of these blends exhibit high efficiencies despite a low energy offset at the heterojunction. Herein, free charge generation in the high‐performance blend of the donor polymer PM6 with the NFA Y6 is thoroughly investigated as a function of internal field, temperature and excitation energy. Results show that photocurrent generation is essentially barrierless with near‐unity efficiency, regardless of excitation energy. Efficient charge separation is maintained over a wide temperature range, down to 100 K, despite the small driving force for charge generation. Studies on a blend with a low concentration of the NFA, measurements of the energetic disorder, and theoretical modeling suggest that CT state dissociation is assisted by the electrostatic interfacial field which for Y6 is large enough to compensate the Coulomb dissociation barrier.

Perovskite solar cells combine high carrier mobilities with long carrier lifetimes and high radiative efficiencies. Despite this, full devices suffer from significant nonradiative recombination losses, limiting their VOC to values well below the Shockley–Queisser limit. Here, recent advances in understanding nonradiative recombination in perovskite solar cells from picoseconds to steady state are presented, with an emphasis on the interfaces between the perovskite absorber and the charge transport layers. Quantification of the quasi‐Fermi level splitting in perovskite films with and without attached transport layers allows to identify the origin of nonradiative recombination, and to explain the VOC of operational devices. These measurements prove that in state‐of‐the‐art solar cells, nonradiative recombination at the interfaces between the perovskite and the transport layers is more important than processes in the bulk or at grain boundaries. Optical pump‐probe techniques give complementary access to the interfacial recombination pathways and provide quantitative information on transfer rates and recombination velocities. Promising optimization strategies are also highlighted, in particular in view of the role of energy level alignment and the importance of surface passivation. Recent record perovskite solar cells with low nonradiative losses are presented where interfacial recombination is effectively overcome—paving the way to the thermodynamic efficiency limit.

photoluminescence yields (>20%). [5] In principle, this would allow open-circuit voltages (V OC ) very close to the radiative limit (≈1.3 V for a bandgap of 1.6 eV) using already existing perovskites. However, despite the tremendous effort devoted by the scientific community on the improvement of this solar cell technology, the experimental efficiencies are still far from the Shockely-Queisser (S.Q.) theoretical predictions of power conversion efficiency (PCE) up to 30%. [6] Specifically, in order to further improve the PCE, the effort must be focused on increasing the V OC and the fill factor (FF) through the reduction of nonradiative recombination losses. Moreover, a better understanding on the predominant energy loss mechanisms in the working device has to be accomplished.Perovskite solar cells generally consist of a 300-500 nm layer of photoactive absorber, sandwiched between two charge transporting layers that have the function of selectively transporting the photogenerated electrons (holes) to the cathode (anode). In an ideal solar cell, all photons are absorbed in the perovskite films, generating electrons and holes with unity efficiency, and-under open-circuit conditions-the only recombination channel is the radiative recombination of free electrons and holes in the same layer where they are generated. Commonly, reported values for V OC are much lower due to unwanted nonradiative recombination. During the past years, many studies have evaluated recombination in perovskites layers and suggested that defects at the perovskite surface or at grain boundaries as possible reasons Today's perovskite solar cells (PSCs) are limited mainly by their open-circuit voltage (V OC ) due to nonradiative recombination. Therefore, a comprehensive understanding of the relevant recombination pathways is needed. Here, intensity-dependent measurements of the quasi-Fermi level splitting (QFLS) and of the V OC on the very same devices, including pin-type PSCs with efficiencies above 20%, are performed. It is found that the QFLS in the perovskite lies significantly below its radiative limit for all intensities but also that the V OC is generally lower than the QFLS, violating one main assumption of the Shockley-Queisser theory. This has far-reaching implications for the applicability of some well-established techniques, which use the V OC as a measure of the carrier densities in the absorber. By performing drift-diffusion simulations, the intensity dependence of the QFLS, the QFLS-V OC offset and the ideality factor are consistently explained by trap-assisted recombination and energetic misalignment at the interfaces. Additionally, it is found that the saturation of the V OC at high intensities is caused by insufficient contact selectivity while heating effects are of minor importance. It is concluded that the analysis of the V OC does not provide reliable conclusions of the recombination pathways and that the knowledge of the QFLS-V OC relation is of great importance.       J J qV n k T radiative recombination current J rad...

High fill factor, large area perovskite solar cells are realized with undoped organic transport layers by optimizing the charge carrier transit through PTAA.