Snaith group

Abstract:

Tin-containing metal halide perovskites have enormous potential as photovoltaics, both in narrow band gap mixed tin–lead materials for all-perovskite tandems and for lead-free perovskites. The introduction of Sn(II), however, has significant effects on the solution chemistry, crystallization, defect states, and other material properties in halide perovskites. In this perspective, we summarize the main hurdles for tin-containing perovskites and highlight successful attempts made by the community to overcome them. We discuss important research directions for the development of these materials and propose some approaches to achieve a unified understanding of Sn incorporation. We particularly focus on the discussion of charge carrier dynamics and nonradiative losses at the interfaces between perovskite and charge extraction layers in p-i-n cells. We hope these insights will aid the community to accelerate the development of high-performance, stable single-junction tin-containing perovskite solar cells and all-perovskite tandems.

Abstract:

2H-Benzotriazol-2-ylethylammonium bromide and iodide and its difluorinated derivatives are synthesized and employed as interlayers for passivation of formamidinium lead triiodide (FAPbI₃) solar cells. In combination with PbI₂ and PbBr₂, these benzotriazole derivatives form two-dimensional (2D) Ruddlesden-Popper perovskites (RPPs) as evidenced by their crystal structures and thin film characteristics. When used to passivate n-i-p FAPbI₃ solar cells, the power conversion efficiency improves from 20% to close to 22% by enhancing the open-circuit voltage. Quasi-Fermi level splitting experiments and scanning electron microscopy cathodoluminescence hyperspectral imaging reveal that passivation provides a reduced nonradiative recombination at the interface between the perovskite and hole transport layer. Photoluminescence spectroscopy, angle-resolved grazing-incidence wide-angle X-ray scattering, and depth profiling X-ray photoelectron spectroscopy studies of the 2D/three-dimensional (3D) interface between the benzotriazole RPP and FAPbI₃ show that a nonuniform layer of 2D perovskites is enough to passivate defects, enhance charge extraction, and decrease nonradiative recombination.

Abstract:

Piezoelectric materials convert between mechanical and electrical energy and are a basis for self-powered electronics. Current piezoelectrics exhibit either large charge (d₃₃) or voltage (g₃₃) coefficients but not both simultaneously, and yet the maximum energy density for energy harvesting is determined by the transduction coefficient: d₃₃*g₃₃. In prior piezoelectrics, an increase in polarization usually accompanies a dramatic rise in the dielectric constant, resulting in trade off between d₃₃ and g₃₃. This recognition led us to a design concept: increase polarization through Jahn-Teller lattice distortion and reduce the dielectric constant using a highly confined 0D molecular architecture. With this in mind, we sought to insert a quasi-spherical cation into a Jahn-Teller distorted lattice, increasing the mechanical response for a large piezoelectric coefficient. We implemented this concept by developing EDABCO-CuCl₄ (EDABCO = N-ethyl-1,4-diazoniabicyclo[2.2.2]octonium), a molecular piezoelectric with a d₃₃ of 165 pm/V and g₃₃ of ~2110 × 10^-3 V m N^-1, one that achieved thusly a combined transduction coefficient of 348 × 10^-12 m³ J^-1. This enables piezoelectric energy harvesting in EDABCO-CuCl₄@PVDF (polyvinylidene fluoride) composite film with a peak power density of 43 µW/cm² (at 50 kPa), the highest value reported for mechanical energy harvesters based on heavy-metal-free molecular piezoelectric.