Strain Heterogeneity and Extended Defects in Halide Perovskite Devices.

Strain is an important property in halide perovskite semiconductors used for optoelectronic applications because of its ability to influence device efficiency and stability. However, descriptions of strain in these materials are generally limited to bulk averages of bare films, which miss important property-determining heterogeneities that occur on the nanoscale and at interfaces in multilayer device stacks. Here, we present three-dimensional nanoscale strain mapping using Bragg coherent diffraction imaging of individual grains in CsFAPb(IBr) and CsFASnI (FA = formamidinium) halide perovskite absorbers buried in full solar cell devices.

Electrochemical Impedance Spectroscopy of All-Perovskite Tandem Solar Cells.

This work explores electrochemical impedance spectroscopy to study recombination and ionic processes in all-perovskite tandem solar cells. We exploit selective excitation of each subcell to enhance or suppress the impedance signal from each subcell, allowing study of individual tandem subcells. We use this selective excitation methodology to show that the recombination resistance and ionic time constants of the wide gap subcell are increased with passivation.

Substitution of lead with tin suppresses ionic transport in halide perovskite optoelectronics.

Despite the rapid rise in the performance of a variety of perovskite optoelectronic devices with vertical charge transport, the effects of ion migration remain a common and longstanding Achilles' heel limiting the long-term operational stability of lead halide perovskite devices. However, there is still limited understanding of the impact of tin (Sn) substitution on the ion dynamics of lead (Pb) halide perovskites. Here, we employ scan-rate-dependent current-voltage measurements on Pb and mixed Pb-Sn perovskite solar cells to show that short circuit current losses at lower scan rates, which can be traced to the presence of mobile ions, are present in both kinds of perovskites.

Identification and Mitigation of Transient Phenomena That Complicate the Characterization of Halide Perovskite Photodetectors.

Halide perovskites have shown promise to advance the field of light detection in next-generation photodetectors, offering performance and functionality beyond what is currently possible with traditional inorganic semiconductors. Despite a relatively high density of defects in perovskite thin films, long carrier diffusion lengths and lifetimes suggest that many defects are benign. However, perovskite photodetectors show detection behavior that varies with time, creating inconsistent device performance and difficulties in accurate characterization.

Vacuum-Deposited Wide-Bandgap Perovskite for All-Perovskite Tandem Solar Cells.

All-perovskite tandem solar cells beckon as lower cost alternatives to conventional single-junction cells. Solution processing has enabled rapid optimization of perovskite solar technologies, but new deposition routes will enable modularity and scalability, facilitating technology adoption. Here, we utilize 4-source vacuum deposition to deposit FACsPb(IBr) perovskite, where the bandgap is changed through fine control over the halide content.

Local symmetry breaking drives picosecond spin domain formation in polycrystalline halide perovskite films.

Photoinduced spin-charge interconversion in semiconductors with spin-orbit coupling could provide a route to optically addressable spintronics without the use of external magnetic fields. However, in structurally disordered polycrystalline semiconductors, which are being widely explored for device applications, the presence and role of spin-associated charge currents remains unclear. Here, using femtosecond circular-polarization-resolved pump-probe microscopy on polycrystalline halide perovskite thin films, we observe the photoinduced ultrafast formation of spin domains on the micrometre scale formed through lateral spin currents.

Charge transport in mixed metal halide perovskite semiconductors.

Investigation of the inherent field-driven charge transport behaviour of three-dimensional lead halide perovskites has largely remained challenging, owing to undesirable ionic migration effects near room temperature and dipolar disorder instabilities prevalent specifically in methylammonium-and-lead-based high-performing three-dimensional perovskite compositions. Here, we address both these challenges and demonstrate that field-effect transistors based on methylammonium-free, mixed metal (Pb/Sn) perovskite compositions do not suffer from ion migration effects as notably as their pure-Pb counterparts and reliably exhibit hysteresis-free p-type transport with a mobility reaching 5.4 cm V s.

Tunable Multiband Halide Perovskite Tandem Photodetectors with Switchable Response.

Photodetectors with multiple spectral response bands have shown promise to improve imaging and communications through the switchable detection of different photon energies. However, demonstrations to date have been limited to only two bands and lack capability for fast switching in situ. Here, we exploit the band gap tunability and capability of all-perovskite tandem solar cells to demonstrate a new device concept realizing four spectral bands of response from a single multijunction device, with fast, optically controlled switching between the bands.

Local nanoscale phase impurities are degradation sites in halide perovskites.

Understanding the nanoscopic chemical and structural changes that drive instabilities in emerging energy materials is essential for mitigating device degradation. The power conversion efficiency of halide perovskite photovoltaic devices has reached 25.7 per cent in single-junction and 29.

Ion migration drives self-passivation in perovskite solar cells and is enhanced by light soaking.

Perovskite solar cells have rapidly become the most promising emerging photovoltaic technology. This is largely due to excellent self-passivating properties of the perovskite absorber material, allowing for a remarkable ease of fabrication. However, the field is plagued by poor reproducibility and conflicting results.

Optoelectronic Properties of Low-Bandgap Halide Perovskites for Solar Cell Applications.

Riding on the coat tails of rapid developments in single-junction halide perovskite solar cells, all-perovskite multijunction solar cells have recently garnered significant attention, with the highest power-conversion efficiency already reaching 25.6%. Much of this progress has been fueled by the rapid rise in the photovoltaic performance of low-bandgap halide perovskite absorbers, materials, which, to date, have only been achievable by the partial or complete substitution of lead with tin.

Critical Assessment of the Use of Excess Lead Iodide in Lead Halide Perovskite Solar Cells.

It is common practice in the lead halide perovskite solar cell field to add a small molar excess of lead iodide (PbI) to the precursor solution to increase the device performance. However, recent reports have shown that an excess of PbI can accelerate performance loss. In addition, PbI is photoactive (band gap ∼2.

Comparing the excited-state properties of a mixed-cation-mixed-halide perovskite to methylammonium lead iodide.

Organic-inorganic perovskites are one of the most promising photovoltaic materials for the design of next generation solar cells. The lead-based perovskite prepared with methylammonium and iodide was the first in demonstrating high power conversion efficiency, and it remains one of the most used materials today. However, perovskites prepared by mixing several halides and several cations systematically yield higher efficiencies than "pure" methylammonium lead iodide (MAPbI) devices.

Unraveling the Effect of Crystal Structure on Degradation of Methylammonium Lead Halide Perovskite.

Despite the remarkable efficiencies of perovskite solar cells, moisture instability has still been the major constraint in the technology deployment. Although, some research groups have discussed the possible mechanisms involved in the perovskite degradation, no broader understanding has been developed so far. Here, we demonstrate that the crystal orientation of perovskite film plays a major role in its degradation.

Cesium-Incorporated Triple Cation Perovskites Deliver Fully Reversible and Stable Nanoscale Voltage Response.

Perovskite solar cells that incorporate small concentrations of Cs in their A-site have shown increased lifetime and improved device performance. Yet, the development of fully stable devices operating near the theoretical limit requires understanding how Cs influences perovskites' electrical properties at the nanoscale. Here, we determine how the chemical composition of three perovskites (MAPbBr, MAPbI, and Cs-mixed) affects their short- and long-term voltage stabilities, with <50 nm spatial resolution.

Partial oxidation of the absorber layer reduces charge carrier recombination in antimony sulfide solar cells.

We investigate the effect of a post heat treatment of the absorber layer in air for antimony sulfide (SbS) sensitized solar cells. Phenomenologically, exposing the SbS surface of sensitised solar cells to air at elevated temperatures is known to improve device performance. Here, we have investigated the detailed origins of this improvement.

Optical analysis of CHNHSn Pb I absorbers: a roadmap for perovskite-on-perovskite tandem solar cells.

Organic-inorganic perovskite structures in which lead is substituted by tin are exceptional candidates for broadband light absorption. Herein we present a thorough analysis of the optical properties of CHNHSn Pb I films, providing the field with definitive insights about the possibilities of these materials for perovskite solar cells of superior efficiency. We report a user's guide based on the first set of optical constants obtained for a series of tin/lead perovskite films, which was only possible to measure due to the preparation of optical quality thin layers.

Doping of TiO2 for sensitized solar cells.

This review gives a detailed summary and evaluation of the use of TiO2 doping to improve the performance of dye sensitized solar cells. Doping has a major effect on the band structure and trap states of TiO2, which in turn affect important properties such as the conduction band energy, charge transport, recombination and collection. The defect states of TiO2 are highly dependent on the synthesis method and thus the effect of doping may vary for different synthesis techniques, making it difficult to compare the suitability of different dopants.

Efficient room temperature aqueous Sb2S3 synthesis for inorganic-organic sensitized solar cells with 5.1% efficiencies.

Sb2S3 sensitized solar cells are a promising alternative to devices employing organic dyes. The manufacture of Sb2S3 absorber layers is however slow and cumbersome. Here, we report the modified aqueous chemical bath synthesis of Sb2S3 absorber layers for sensitized solar cells.