Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 25, Issue 21, Pages 5480-5488Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201805370
Keywords
bismuth; doping; luminescence; photochemistry; perovskite phases
Categories
Funding
- National Natural Science Foundation of China [21674006]
- 100 Top Young Scientists Program by Chinese Academy of Sciences [QYZDBSSW-SLH033]
- Natural Science Foundation of China [21674006, 21875012]
- One Thousand Young Talents Program of China
- 111 Project [B14009]
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A comprehensive study unveiling the impact of heterovalent doping with Bi3+ on the structural, semiconductive, and photoluminescent properties of a single crystal of lead halide perovskites (CH3NH3PbBr3) is presented. As indicated by single-crystal XRD, a perfect cubic structure in Bi3+-doped CH3NH3PbBr3 crystals is maintained in association with a slight lattice contraction. Time-resolved and power-dependent photoluminescence (PL) spectroscopy illustrates a progressively quenched PL of visible emission, alongside the appearance of a new PL signal in the near-infrared (NIR) regime, which is likely to be due to energy transfer to the Bi sites. These optical characteristics indicate the role of Bi-3 dopants as nonradiative recombination centers, which explains the observed transition from bimolecular recombination in pristine CH3NH3PbBr3 to a dominant trap-assisted monomolecular recombination with Bi3+ doping. Electrically, it is found that the mobility in pristine perovskite crystals can be boosted with a low Bi3+ concentration, which may be related to a trap-filling mechanism. Aided by temperature (7)-dependent measurements, two temperature regimes are observed in association with different activation energies (E-a) for electrical conductivity. The reduction of E-a at lower T may be ascribed to suppression of ionic conduction induced by doping. The modified electrical properties and NIR emission with the control of Bi3+ concentration shed light on the opportunity to apply heterovalent doping of perovskite single crystals for NIR optoelectronic applications.
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