Since the establishment of perovskite solar cells (PSCs), there has been an intense search for alternative materials to replace lead and improve their stability toward moisture and light. As single-metal perovskite structures have yielded unsatisfactory performances, an alternative is the use of double perovskites that incorporate a combination of metals. To this day, only a handful of these compounds have been synthesized, but most of them have indirect bandgaps and/or do not have bandgaps energies well-suited for photovoltaic applications. Here we report the synthesis and characterization of a unique mixed metal ⟨111⟩-oriented layered perovskite, CsCuSbCl (1), that incorporates Cu and Sb into layers that are three octahedra thick (n = 3). In addition to being made of abundant and nontoxic elements, we show that this material behaves as a semiconductor with a direct bandgap of 1.0 eV and its conductivity is 1 order of magnitude greater than that of MAPbI (MA = methylammonium). Furthermore, 1 has high photo- and thermal-stability and is tolerant to humidity. We conclude that 1 is a promising material for photovoltaic applications and represents a new type of layered perovskite structure that incorporates metals in 2+ and 3+ oxidation states, thus significantly widening the possible combinations of metals to replace lead in PSCs.
Antimony and bismuth ⟨111⟩ layered perovskites have recently attracted significant attention as possible, nontoxic alternatives to lead halide perovskites. Unlike lead halide perovskites, however, ⟨111⟩ halide perovskites have shown limited ability to tune their optical and electronic properties. Herein, we report on the metal alloying of manganese and copper into the family of materials with formula Cs 4 Mn 1−x Cu x Sb 2 Cl 12 (x = 0−1). By changing the concentration of manganese and copper, we show the ability to modulate the bandgap of this family of compounds over the span of 2 electron volts, from 3.0 to 1.0 eV. Furthermore, we show that in doing so, we can also adjust other relevant properties such as their magnetic behavior and their electronic structure.
Halide double perovskites have allowed the significant expansion of the possible metals and oxidation states in halide perovskites. Further, they have shown some remarkable properties and applications. Akin to the dimensional reduction in halide perovskites to generate layered perovskites, it has recently been shown that it is also possible to dimensionally reduce double perovskites to generate layered double perovskites (LDPs). The implications of such realization are tremendous from several different perspectives. First, it widens the space of possible metals, as LDPs can be made of B I , B II , and B III cations and their permutations. Second, it allows the modulation of the materials' electronic structure through dimensional reduction and quantum confinement effects. Third, it allows the incorporation of many more organic cations, thereby providing a more chemically, structurally, and electronically diverse pool of materials. The combinations of these three factors result in a potentially infinite family of new materials with new or improved properties and applications. Herein, we describe the emergence of this new family and the known chemical, structural, and electronic features and review their proved and potential applications. Finally, we highlight some of the challenges and propose some future avenues of research and areas of opportunity for these materials.
Akin to the expansion in compositional diversity that halide double perovskites provided to three-dimensional perovskites, layered double perovskites could further expand the diversity of two-dimensional (2D) perovskites, and therefore, they could also enhance the properties or expand the possible applications of such materials. Despite the great promise of halide 2D double perovskites, up to date, there are only four confirmed members of this family of materials. Herein, we explore 90 hypothetical new members of this family of materials by a combined theoretical, computational, and experimental method. The combination of these tactics allowed us to predict several new materials, out of which we experimentally synthesized and characterized five new layered double perovskites, some of which show promising properties for their use in photovoltaics and optoelectronics. Further, our work highlights the vast diversity of compositions and therefore of applications that double-layered perovskites have yet to offer.
Halide perovskites offer great promise for optoelectronic applications, but stability issues continue to hinder its implementation and long-term stability. The stability of all-inorganic halide perovskites and the inherent quantum confinement of low dimensional perovskites can be harnessed to synthesize materials with high PL efficiency. An example of such materials is the recently reported new family of layered double perovskites, Cs4Mn1−xCdxBi2Cl12. Herein, we report a new synthetic procedure that enhances the maximum PLQY of this family materials to up 79.5%, a 20% enhancement from previous reports and the highest reported for a Mn-doped halide perovskite. Importantly, stability tests demonstrate that these materials are very stable towards humidity, UV irradiation, and temperature. Finally, we investigated the photophysics, the effects of magnetic coupling and temperature in the PL efficiency and proposed a mechanism for the emission process. Our results highlight the potential of this family of materials and related layered all-inorganic perovskites for solid-state lighting and optoelectronic applications.
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