Two-dimensional (2D) organic–inorganic hybrid halide perovskites exhibit unique properties, such as long charge carrier lifetimes, high photoluminescence quantum efficiencies, and great tolerance to defects. Over the last several decades tremendous progress has occurred in the development of 2D layered halide perovskite semiconductor materials and devices. Chemical functionalization of 2D halide perovskites is an effective approach for tuning their electronic properties. A large amount of effort has been made in compositional engineering of the cations and anions in the perovskite lattice. However, few efforts have incorporated rationally designed semiconducting organic moieties into these systems to alter the overall chemical and optoelectronic properties of 2D perovskites. In fact, incorporation of large conjugated organic groups in the spatially confined inorganic perovskite matrix was found to be challenging, and this synthetic challenge hinders a deeper understanding of the materials’ structure–property relationships. Recently, exciting progress has been made regarding the molecular design, optical characterization, and device fabrication of novel 2D halide perovskite materials that incorporate functional organic semiconducting building blocks. In this article, we provide a timely review regarding this recent progress. Moreover, we discuss successes and current challenges regarding the synthesis, characterization, and device applications of such hybrid materials and provide a perspective on the true future promise of these advanced nanomaterials.
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High‐throughput computational design of halide perovskites and beyond for optoelectronics
Halide perovskites have attracted great interest as promising next‐generation materials in optoelectronics, ranging from solar cells to light‐emitting diodes. Despite their exceptional optoelectronic properties and low cost, the prototypical organic–inorganic hybrid lead halide perovskites suffer from toxicity and low stability. Therefore, it is of high demand to search for stable and nontoxic alternatives to the hybrid lead halide perovskites. Recently, high‐throughput computational materials design has emerged as a powerful approach to accelerate the discovery of new halide perovskite compositions or even novel compounds beyond perovskites. In this review, we discuss how this approach discovers halide perovskites and beyond for optoelectronics. We first overview the background of halide perovskites and methodologies in high‐throughput computational design. Then, we focus on materials properties for different optoelectronic applications, and how they are assessed with materials descriptors. Finally, we review different studies in terms of specific materials types to discuss their design principles, screening results, and experimental verification.
This article is categorized under: Structure and Mechanism > Computational Materials Science Electronic Structure Theory > Density Functional Theory
- NSF-PAR ID:
- 10360564
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- WIREs Computational Molecular Science
- Volume:
- 11
- Issue:
- 3
- ISSN:
- 1759-0876
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Halide perovskites, such as methylammonium lead halide perovskites (
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