Emerging Two-Dimensional Organic Semiconductor-Incorporated Perovskites─A Fascinating Family of Hybrid Electronic Materials

Abstract

Halide perovskites have attracted a great amount of attention owing to their unique materials chemistry, excellent electronic properties, and low-cost manufacturing. Two-dimensional (2D) halide perovskites, originating from three-dimensional (3D) perovskite structures, are structurally more diverse and therefore create functional possibilities beyond 3D perovskites. The much less restrictive size constraints on the organic component of these hybrid materials particularly provide an exciting platform for designing unprecedented materials and functionalities at the molecular level. In this Perspective, we discuss the concept and recent development of a sub-class of 2D perovskites, namely, organic semiconductor-incorporated perovskites (OSiPs). OSiPs combine the electronic functionality of organic semiconductors with the soft and dynamic halide perovskite lattice, offering opportunities for tailoring the energy landscape, lattice and carrier dynamics, and electron/ion transport properties for various fundamental studies, as well as device applications. Specifically, we summarize recent advances in the design, synthesis, and structural analysis of OSiPs with various organic conjugated moieties as well as the application of OSiPs in photovoltaics, light-emitting devices, and transistors. Lastly, challenges and further opportunities for OSiPs in molecular design, integration of novel functionality, film quality, and stability issues are addressed.

Nonadiabatic Molecular Dynamics with Non-Condon Effect of Charge Carrier Dynamics

“…A thorough understanding of ultrafast excited carrier dynamics is crucial for optoelectronic devices, − quantum materials, − and other materials science. − Charge carrier dynamics encompass a myriad of complex processes, pushing the boundaries of both experimental and theoretical research tools. , The emergence of sophisticated experimental methods in the ultrafast dynamics domain, ,− i.e., ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES), ,− offers an accurate mapping of band structures, providing in-depth energy and momentum data while tracking electron activity at a femtosecond time scale. However, there is still a significant gap in the development of comparable theoretical tools, especially for first-principles approaches.…”

Room-Temperature Photoferroelectrics Semiconductor Driven by the Interlayer Confinement Effect

“…The interlayer spacings of (IPA) 2 PbBr 4 , (IBA) 2 PbBr 4 , and (IAA) 2 PbBr 4 are 5.797, 7.734, and 10.473 Å, respectively (Scheme ). We know that the configuration of interlayer cations has an undeniable impact on the degree of distortion of the inorganic framework and the structure/property of the entire compound. − For example, Yaffe and co-workers studied the effect of the organic cations on the structural dynamics of the inorganic scaffold . Zhou et al compared the photovoltaic performance of 2D OIHPs constructed with different configurations of interlayer cations .…”

Two-Dimensional Dion-Jacobson Tin Perovskite Transistors with Enhanced Ambient Stability

“…Sn 2+ perovskites have a lower effective mass than lead-based materials, showing high potential as p-type semiconducting materials. − Initially, the exploration of 2D Sn 2+ perovskites concentrated on Ruddlesden–Popper (RP) perovskites with a chemical formula of A 2 ′A n –1 M n X 3 n +1 , where A′ is a monovalent organic cation spacer, A is also a monovalent cation, M is a divalent metal cation, X is a halide anion, and n is the number of corner-sharing [MX 6 ] 4– octahedral cage layers. The two adjacent monovalent organic spacers are connected through van der Waals interaction. − Research on 2D RP perovskites has expanded to include the design of new organic spacers with specific functional groups, − additive engineering, − molecular doping, , and device engineering. − …”