Two-dimensional (2D) hybrid perovskites are stoichiometric compounds consisting of alternating inorganic metal-halide sheets and organoammonium cationic layers. This materials class is widely tailorable in composition, structure, and dimensionality and is providing an intriguing playground for the solid-state chemistry and physics communities to uncover structure-property relationships. In this Perspective, we describe semiconducting 2D perovskites containing lead and tin halide inorganic frameworks. In these 2D perovskites, charges are typically confined to the inorganic framework because of strong quantum and dielectric confinement effects, and exciton binding energies are many times greater than kT at room temperature. We describe the role of the heavy atoms in the inorganic framework; the geometry and chemistry of organic cations; and the "softness" of the organic-inorganic lattice on the electronic structure and dynamics of electrons, excitons, and phonons that govern the physical properties of these materials.
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Sci Rep
January 2025
Fujian Provincial Key Laboratory of Ecology-Toxicological Effects & Control for Emerging Contaminants, Key Laboratory of Ecological Environment and Information Atlas (Fujian Provincial University), College of Environmental and Biological Engineering, Putian University, Putian, 351100, Fujian, China.
The type of electron acceptor group has a significant effect on the photovoltaic properties of solar cell sensitizers. In this study, on the basis of previous studies of the π1- and π2-linked groups of D-π1-A1-π2-A2-type sensitizers, the photoelectric properties of Ullazine-Based photosensitizing dyes were further optimized by adjusting the electron-absorbing groups at the A1 and A2 positions. DFT and TDDFT calculations revealed that substituting the A1 position with a BTD moiety led to a substantial increase in the light absorption capacity of the dye.
View Article and Find Full Text PDFNanomaterials (Basel)
January 2025
Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics, Central South University, Changsha 410083, China.
Two-dimensional (2D) layered materials have received much attention due to the unique properties stemming from their van der Waals (vdW) interactions, quantum confinement, and many-body interactions of quasi-particles, which drive their exotic optical and electronic properties, making them critical in many applications. Here, we review our past years' findings, focusing on many-body interactions in 2D layered materials, including phonon anharmonicity, electron-phonon coupling (), exciton dynamics, and phonon anisotropy based on temperature (polarization)-dependent Raman spectroscopy and Photoluminescence (PL). Our review sheds light on the role of quasi-particles in tuning the material properties, which could help optimize 2D materials for future applications in electronic and optoelectronic devices.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, Graduate School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan.
Light-driven spin hyperpolarization of organic molecules is a crucial technique for spin-based applications such as quantum information science (QIS) and dynamic nuclear polarization (DNP). Synthetic chemistry provides the design of spins with atomic precision and enables the scale-up of individual spins to hierarchical structures. The high designability and extended pore structure of metal-organic frameworks (MOFs) can control interactions between spins and guest molecules.
View Article and Find Full Text PDFUsing the first principle calculations, we propose a boron and nitrogen cluster incorporated graphene system for efficient valley polarization. The broken spatial inversion symmetry results in high Berry curvature at and valleys of the hexagonal Brillouin zone in this semiconducting system. The consideration of excitonic quasiparticles within the approximation along with their scattering processes using the many-body Bethe-Salpeter equation gives rise to an optical gap of 1.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
MOE Key Laboratory of Macromolecular Synthesis and Functionalization, State Key Laboratory of Silicon and Advanced Semiconductor Materials, Department of Polymer Science and Engineering, Zhejiang University, Hangzhou 310027, P. R. China.
Organic solar cells have seen significant progress in the past 2 decades with power conversion efficiencies (PCEs) exceeding 20% but mostly based on high-cost photovoltaic materials. Polythiophenes (PTs) without a fused-ring structure are good candidates as low-cost donor materials, deserving more attention for studying. In this work, ester-substituted thiazole (E-Tz) was explored as the electron-withdrawing unit to design PTs, and further optimization on the fluorinated/nonfluorinated donor segment contents via copolymerization strategy was simultaneously performed, yielding polymer donors of PTETz-100F, PTETz-80F, and PTETz-0F.
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