摘要
Zero-dimensional(0D)hybrid metal halides are considered as promising light-emitting materials due to their unique broadband emission from self-trapped excitons(STEs).Despite substantial progress in the development of these materials,the photoluminescence quantum yields(PLQY)of hybrid Sb-Br analogs have not fully realized the ca-pabilities of these materials,necessitating a better fundamental understanding of the structure-property relation-ship.Here,we have achieved a pressure-induced emission in 0D(EATMP)SbBr5(EATMP=(2-aminoethyl)trimethylphosphanium)and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations.The pressure-induced reduction in the overlap between the STE states and ground states(GSs)results in the suppression of phonon-assisted non-radiative decay.The photoluminescence(PL)evo-lution is systematically demonstrated to be controlled by the pressure-regulated exciton-phonon coupling,which can be quantified using Huang-Rhys factorS.Through detailed studies of the S-PLQY relation in a series of 0D hybrid antimony halides,we establish a quantitative structure-property relationship that regulating S value toward 21 leads to the optimized emission.This work not only sheds light on pressure-induced emission in 0D hybrid metal halides but also provides valuable insights into the design principles for enhancing the PLQY in this class of materials.
基金
supported by the National Natural Science Foundation of China(Nos.22275004,17N1051-0213,and 51872315)
Shanghai Science and Technology Committee(No.22JC1410300)
Shanghai Key Laboratory of Novel Extreme Condition Materials(No.22dz2260800)
the Science Foundation of the Chinese Academy of Sciences
Some experiments are supported by the Synergetic Extreme Condition User Facility.Portions of this work were performed at GeoSoilEnviroCARS(The University of Chicago,Sector 13),Advanced Photon Source(APS),and Argonne Na-tional Laboratory.GeoSoilEnviroCARS is supported by the National Science Foundation-Earth Sciences(EAR-1634415)
This research used resources of the Advanced Photon Source,a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC02-06CH11357.