Pressure‐Suppressed Carrier Trapping Leads to Enhanced Emission in Two‐Dimensional Perovskite (HA)2(GA)Pb2I7

Guo, Songhao; Zhao, Yongsheng; Bu, Kejun; Fu, Yongping; Luo, Hui; Chen, Mengting; Hautzinger, Matthew P.; Wang, Yingqi; Jin, Song; Yang, Wenge; Lü, Xujie

doi:10.1002/anie.202001635

Cited by 96 publications

(62 citation statements)

References 42 publications

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“…[9] In combination with in situ characterization methods, high-pressure research can further our fundamental understandings of the unique properties in hybrid metal halides. Recently, numerous studies of pressure-induced and/or enhanced PL in metal halides have been reported, [10] while the microscopic mechanisms of the pressure effects are still lively debated. Our recent work has revealed that lattice compression stabilizes the STE states by increasing the exciton binding energy of 1D C 4 N 2 H 14 PbBr 4 , resulting in the enhanced PL efficiency.…”

Section: Introductionmentioning

confidence: 99%

Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

et al. 2021

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Low-dimensional hybrid metal halides are emerging as a highly promising class of single-component white-emitting materials for their unique broadband emission from self-trapped excitons (STEs). Despite substantial progress in the development of these metal halides, many challenges remain to be addressed to obtain a better fundamental understanding of the structure-property relationship and realize the full potentials of this class of materials. Here, via pressure regulation, a near 100% photoluminescence quantum yield (PLQY) of broadband emission is achieved in a corrugated 1D hybrid metal halide C 5 N 2 H 16 Pb 2 Br 6 , which possesses a highly distorted structure with an initial PLQY of 10%. Compression reduces the overlap between STE states and ground state, leading to a suppressed phonon-assisted non-radiative decay. The PL evolution is systematically demonstrated to be controlled by the pressure-regulated exciton-phonon coupling which can be quantified using Huang-Rhys factor S. Detailed studies of the S-PLQY relation for a series of 1D hybrid metal halides

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Section: Introductionmentioning

confidence: 99%

Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

et al. 2021

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“…The length and coordination preference should fulfil the strict limitation of the Goldschmidt's tolerance factor concept [20]. Notably, some 2D Ruddlesden-Popper materials containing large-radius cations in metal-halide perovskite cavities were recently obtained, such as guanidine (~278 pm) and dimethylamine (DMA,~272 pm) [21][22][23]. Despite the attempts to explore new candidates, studies on their physical attributes and potential optoelectronic applications remain quite scarce.…”

Section: Introductionmentioning

confidence: 99%

Rational alloying of secondary and aromatic ammonium cations in a metal-halide perovskite toward crystal-array photodetection

et al. 2021

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Two-dimensional (2D) hybrid perovskites with the Ruddlesden-Popper lattice (A') 2 (A) n−1 M n X 3n+1 are emerging as the promising optoelectronic candidates, both the inorganic and organic ingredients of which can be tailored to modulate the physical properties. Nevertheless, there is a scarcity of 2D multilayered motifs with the A-site large-size cations occupying perovskite cavities. Here, by rational mixedcation alloying, we present a new 2D hybrid perovskite, (4-TFBMA) 2 (DMA)Pb 2 I 7 (1), in which the secondary cation of CH 3 NH 2 CH 3 + (DMA) is located inside the perovskite cage while the aromatic 4-(trifluoromethyl)benzylammonium (4-TFBMA) cation acts as a spacer moiety. Benefiting from the quantum structure of alternating organic spacers and inorganic networks, crystal-array detectors of 1 show fascinating in-plane photodetection responses of large detectivity (~2.95 × 10 12 Jones) and responsivity (~1.97 A W −1 ), comparable to those of some inorganic 2D counterparts. In addition, a fast response rate (~264 µs) and a low dark current are also realized, related to the high crystalline quality and suppression of the hopping barrier due to the insulating organic spacing layers. This result sheds light on the further exploration of new 2D hybrid perovskites toward high-performance photodetector applications.

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“…Most 2D Perovskites are malleable because of their soft nature lattice and flexible organic cations. The relationship between crystal structure and photoluminescence (PL) emission of 2D perovskite compressive by DAC pressure has received significant attention 17 , 28 . However, the local plastic deformation resulting from femtosecond laser shocking has more advantages in strain control than elastic deformation induced by DAC pressure processing.…”

Section: Resultsmentioning

confidence: 99%

“…Regulating the structure of 2D perovskite and exciton transport dynamics is a key to improve its efficiency. Because of the soft lattice nature and the flexibility of sizeable organic spacer cations, the pressure control in the 2D perovskite structure becomes a vital means 17 , 18 . Currently, most of the research focuses on structure modulation via diamond anvil cell (DAC), while the kinetics of exciton transport after pressure is of little concern 19 , 20 .…”

Section: Introductionmentioning

confidence: 99%

Ultrafast femtosecond pressure modulation of structure and exciton kinetics in 2D halide perovskites for enhanced light response and stability

et al. 2021

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The carriers’ transportation between layers of two-dimensional (2D) perovskites is inhibited by dielectric confinement. Here, for the first time, we employ a femtosecond laser to introduce ultrafast shock pressure in the range of 0~15.45 GPa to reduce dielectric confinement by modulating the structure and exciton dynamics in a perovskite single crystal (PSCs), e.g. (F-PEA)2PbI4 (4-fluorophenethylammonium, F-PEA). The density functional theory (DFT) simulation and experimental results show that the inorganic framework distortion results in a bandgap reduction. It was found that the exciton-optical phonon coupling and free excitons (FEs) binding energy are minimized at 2.75 GPa shock pressure due to a reduction in dielectric confinement. The stability testing under various harsh light and humid thermal conditions shows that femtosecond laser shocking improves the stability of (F-PEA)2PbI4 PSCs. Femtosecond laser shock processing provides a new approach for regulating the structure and enhancing halide perovskite properties.

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Pressure‐Suppressed Carrier Trapping Leads to Enhanced Emission in Two‐Dimensional Perovskite (HA)₂(GA)Pb₂I₇

Cited by 96 publications

References 42 publications

Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

Rational alloying of secondary and aromatic ammonium cations in a metal-halide perovskite toward crystal-array photodetection

Ultrafast femtosecond pressure modulation of structure and exciton kinetics in 2D halide perovskites for enhanced light response and stability

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