Snaith group

Abstract:

Substantial VOC loss and halide segregation in wide-bandgap (WBG) perovskite sub-cells pose significant challenges for advancing all-perovskite tandem solar cells (APTSCs). Regarding this, one of the most impactful developments is the application of hole-selective self-assembled monolayers (SAMs), leading to the advancement in APTSC technology. However, SAMs with poor polar-solvent resistance would be inevitably delaminated from substrates during perovskite precursor coating, remaining great challenge in achieving a complete SAMs coverage with derivatization issues, e.g. defective perovskite and considerable interface energy loss. Here, we introduced an in-situ molecular compensation strategy to address the inherent flaw of SAMs within WBG perovskites via incorporating 5-ammonium valeric acid iodide (5-AVAI). The larger-dipole 5-AVAI spontaneously accumulates toward the buried interface to compensate the SAMs-deficient sites when depositing WBG perovskite, effectively minimizing interfacial energy loss. Simultaneously, amphoteric 5-AVAI with amino and carboxyl groups can compensate the defects at grain boundaries for solid passivation. Consequently, a champion efficiency of 20.23% with a record VOC of 1.376 V was realized on WBG devices, enabling an efficiency of 28.9% for the APTSCs. Encouragingly, the tandems showed good operational stability and retained 87.3% of their efficiency after 800 hours of tracking.

Abstract:

<jats:p>In this work, we demonstrate that time-resolved photoluminescence data of metal halide perovskites can be effectively evaluated by combining Bayesian inference with a Markov-chain Monte-Carlo algorithm and a physical model. This approach enables us to infer a high number of parameters that govern the performance of metal halide perovskite-based devices, alongside the probability distributions of those parameters, as well as correlations among all parameters. Via studying a set of halfstacks, comprising electron- and hole-transport materials contacting perovskite thin films, we determine surface recombination velocities at these interfaces with high precision. From the probability distributions of all inferred parameters, we can simulate intensity-dependent photoluminescence quantum efficiency and compare it to experimental data. Finally, we estimate mobility values for vertical charge-carrier transport, which is perpendicular to the plane of the substrate, for all samples using our approach. Since this mobility estimation is derived from charge-carrier diffusion over the length scale of the film thickness and in the vertical direction, it is highly relevant for transport in photovoltaic and light-emitting devices. Our approach of coupling spectroscopic measurements with advanced computational analysis will help speed up scientific research in the field of optoelectronic materials and devices and exemplifies how carefully constructed computational algorithms can derive valuable plurality of information from simple datasets. We expect that our approach can be expanded to a variety of other analysis techniques and that our method will be applicable to other semiconductors.</jats:p> <jats:sec> <jats:title/> <jats:supplementary-material> <jats:permissions> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material> </jats:sec>

Abstract:

In this work we demonstrate that time-resolved photoluminescence data of metal halide perovskites can be effectively evaluated by combining Bayesian inference with a Markov-Chain Monte-Carlo algorithm and a physical model. This approach enables us to infer a high number of parameters which govern the performance of metal halide perovskite-based devices, alongside the probability distributions of those parameters, as well as correlations among all parameters. Via studying a set of "half-stacks’‘, comprising electron and hole transport materials contacting perovskite thin-films, we determine surface recombination velocities at these interfaces with high precision. From the probability distributions of all inferred parameters, we can simulate intensity-dependent photoluminescence quantum efficiency and compare it to the experimental data. Finally, we estimate mobility values for the "vertical’’ charge carrier transport, that perpendicular to the plane of the substrate, for all samples using our approach. Since this mobility estimation is derived from charge carrier diffusion over the length-scale of the film thickness and in the vertical direction, it is highly relevant to transport in photovoltaic and light emitting devices. Our approach of coupling spectroscopic measurements with advanced, computational analysis will help speed up scientific research in the field of optoelectronic materials and devices and exemplifies how carefully constructed computational algorithms can derive valuable plurality of information from simple datasets. We expect that our approach will be expandable to a variety of other analysis techniques and that our method will be applicable to other semiconductors.

Abstract:

All-perovskite tandem photovoltaics are a potentially cost-effective technology to power chemical fuel production, such as green hydrogen. However, their application is limited by deficits in open-circuit voltage and, more challengingly, poor operational stability of the photovoltaic cell. Here we report a laboratory-scale solar-assisted water-splitting system using an electrochemical flow cell and an all-perovskite tandem solar cell. We begin by treating the perovskite surface with a propane-1,3-diammonium iodide solution that reduces interface non-radiative recombination losses and achieves an open-circuit voltage above 90% of the detailed-balance limit for single-junction solar cells between the bandgap of 1.6-1.8 eV. Specifically, a high open-circuit voltage of 1.35 V and maximum power conversion efficiency of 19.9% are achieved at a 1.77 eV bandgap. This enables monolithic all-perovskite tandem solar cells with a 26.0% power conversion efficiency at 1 cm2 area and a pioneering photovoltaic-electrochemical system with a maximum solar-to-hydrogen efficiency of 17.8%. The system retains over 60% of its peak performance after operating for more than 180 h. We find that the performance loss is mainly due to the degradation of the photovoltaic component. We observe severe charge collection losses in the narrow-bandgap sub-cell that can be attributed to the interface degradation between the narrow-bandgap perovskite and the hole-transporting layer. Our study suggests that developing chemically stable absorbers and contact layers is critical for the applications of all-perovskite tandem photovoltaics.

Abstract:

All-perovskite tandem photovoltaics are a potentially cost-effective technology to power chemical fuel production, such as green hydrogen. However, their application is limited by deficits in open-circuit voltage and, more challengingly, poor operational stability of the photovoltaic cell. Here we report a laboratory-scale solar-assisted water-splitting system using an electrochemical flow cell and an all-perovskite tandem solar cell. We begin by treating the perovskite surface with a propane-1,3-diammonium iodide solution that reduces interface non-radiative recombination losses and achieves an open-circuit voltage above 90% of the detailed-balance limit for single-junction solar cells between the bandgap of 1.6–1.8 eV. Specifically, a high open-circuit voltage of 1.35 V and maximum power conversion efficiency of 19.9% are achieved at a 1.77 eV bandgap. This enables monolithic all-perovskite tandem solar cells with a 26.0% power conversion efficiency at 1 cm² area and a pioneering photovoltaic-electrochemical system with a maximum solar-to-hydrogen efficiency of 17.8%. The system retains over 60% of its peak performance after operating for more than 180 h. We find that the performance loss is mainly due to the degradation of the photovoltaic component. We observe severe charge collection losses in the narrow-bandgap sub-cell that can be attributed to the interface degradation between the narrow-bandgap perovskite and the hole-transporting layer. Our study suggests that developing chemically stable absorbers and contact layers is critical for the applications of all-perovskite tandem photovoltaics.