Synergy of 3D and 2D Perovskites for Durable, Efficient Solar Cells and Beyond

Abstract

Three-dimensional (3D) organic–inorganic lead halide perovskites have emerged in the past few years as a promising material for low-cost, high-efficiency optoelectronic devices. Spurred by this recent interest, several subclasses of halide perovskites such as two-dimensional (2D) halide perovskites have begun to play a significant role in advancing the fundamental understanding of the structural, chemical, and physical properties of halide perovskites, which are technologically relevant. While the chemistry of these 2D materials is similar to that of the 3D halide perovskites, their layered structure with a hybrid organic–inorganic interface induces new emergent properties that can significantly or sometimes subtly be important. Synergistic properties can be realized in systems that combine different materials exhibiting different dimensionalities by exploiting their intrinsic compatibility. In many cases, the weaknesses of each material can be alleviated in heteroarchitectures. For example, 3D-2D halide perovskites can demonstrate novel behavior that neither material would be capable of separately. This review describes how the structural differences between 3D halide perovskites and 2D halide perovskites give rise to their disparate materials properties, discusses strategies for realizing mixed-dimensional systems of various architectures through solution-processing techniques, and presents a comprehensive outlook for the use of 3D-2D systems in solar cells. Finally, we investigate applications of 3D-2D systems beyond photovoltaics and offer our perspective on mixed-dimensional perovskite systems as semiconductor materials with unrivaled tunability, efficiency, and technologically relevant durability.

Advancing Evidence-Based Data Interpretation in UV–Vis and Fluorescence Analysis for Nanomaterials: An Analytical Chemistry Perspective

“…Optical spectroscopic techniques, dedicated to studying such interactions, have emerged as indispensable tools in scientific research, technology advancement, and education. Their applications in nano research are especially prominent because of the tunability in nanoparticle optical properties as a function of particle size, shapes, chemical composition, even internal packings and surface morphology including surface defect. − This unique photoelectronic property makes nanomaterials increasingly popular in diverse disciplines including energy, chemistry, medicine, environment, and materials sciences. − Reliable quantification of nanomaterials’ optical properties, including their absorption, scattering, and emission activities, is essential for rational nanomaterials design and applications.…”

Polar Bilayered Dion–Jacobson Hybrid Perovskite Single Crystal with Bulk Photovoltaic Effect for Self-Driven X-ray–Ultraviolet–Visible Photodetection

“…The flexibility of interlayer organic cations and the stability of inorganic components endow two-dimensional (2D) hybrid organic–inorganic perovskite (HOIP) semiconductors with versatility in composition and structure. − Among them, 2D Ruddlesden–Popper (RP) type and Dion–Jacobson (DJ) type HOIPs are widely used in photovoltaic field due to their high stability and strong performance adjustability. − Especially, the application of HOIPs in photodetection has also received increasing attention from multiple disciplines. − At present, 2D HOIPs are mainly used for photodetection in two forms: thin-film and single-crystalline. − For polycrystalline thin films, the internal grain boundaries and defects increase the scattering and recombination of photoinduced carriers, which reduces the carrier transmission efficiency and limits the performance of devices. Compared with polycrystalline thin films, single-crystalline materials have been proved to have the advantages of a low trap density and high mobility, which are considered ideal for constructing high-performance optoelectronic devices. − In this case, a series of 2D HOIPs single crystals are used for broadband photodetection.…”

Anomalous Electron–Phonon Coupling in Cesium-Substituted Methylammonium Lead Iodide Perovskites

“…Most metal halide perovskites (MHPs) with general formula ABX 3 , where B is a metal (Pb or Sn) and X is a halogen atom (Cl, Br, and I), crystallize under ambient conditions in a cubic or tetragonal arrangement of corner-sharing BX 6 octahedrons, enclosing the loosely bound A-site cations in their voids. , The A-site cations that can fit in the inorganic cage voids, according to Goldschmidt’s tolerance-factor criterium, are atomic Cs or organic molecules such as methylammonium (MA) or formamidinium (FA). A peculiarity of MHPs is that the A-site cations are free to move (translate, rotate, and librate) inside the cage voids, exhibiting a fast roto-translational dynamics which is fully or partially (in-plane) unfolded in the cubic and tetragonal phases, respectively, whereas in less symmetric orthorhombic phases, the A-site cations are locked in certain positions and orientations inside the voids .…”