4.8 Article

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

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 40, Pages 17533-17539

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202001635

Keywords

carrier trapping; high-pressure chemistry; phase transitions; photoluminescence enhancement; 2D halide perovskites

Funding

  1. National Nature Science Foundation of China (NSFC) [51527801, U1530402]
  2. DOE-NNSA's Office of Experimental Sciences
  3. National Science Foundation-Earth Sciences [EAR-1634415]
  4. Department of Energy GeoSciences [DE-FG02-94ER14466]
  5. COMPRES through NSF [EAR-1661511]
  6. DOE Office of Science [DE-AC02-06CH11357]
  7. U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-09ER46664]

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A remarkable PL enhancement by 12 fold is achieved using pressure to modulate the structure of a recently developed 2D perovskite (HA)(2)(GA)Pb2I7(HA=n-hexylammonium, GA=guanidinium). This structure features a previously unattainable, extremely large cage. In situ structural, spectroscopic, and theoretical analyses reveal that lattice compression under a mild pressure within 1.6 GPa considerably suppresses the carrier trapping, leading to significantly enhanced emission. Further pressurization induces a non-luminescent amorphous yellow phase, which is retained and exhibits a continuously increasing band gap during decompression. When the pressure is released to 1.5 GPa, emission can be triggered by above-band gap laser irradiation, accompanied by a color change from yellow to orange. The obtained orange phase could be retained at ambient conditions and exhibits two-fold higher PL emission compared with the pristine (HA)(2)(GA)Pb2I7.

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