Impact of metal ns2 lone pair on luminescence quantum efficiency in low-dimensional halide perovskites

Shi, Hongliang; Han, Dan; Chen, Shiyou; Du, Mao-Hua

doi:10.1103/PhysRevMaterials.3.034604

Title: Impact of metal $n s^{2}$ lone pair on luminescence quantum efficiency in low-dimensional halide perovskites

Journal Article · Tue Mar 12 00:00:00 EDT 2019 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.3.034604· OSTI ID:1502553

Shi, Hongliang ^[1];

^[2]; Chen, Shiyou ^[3];

^[4]

Beihang University, Beijing (China)
East China Normal University, Shanghai (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
East China Normal University, Shanghai (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Based on first-principles calculations, we show that chemically active metal ns² lone pairs play an important role in exciton relaxation and dissociation in low-dimensional halide perovskites. Here, we studied excited-state properties of several recently discovered luminescent all-inorganic and hybrid organic-inorganic zero-dimensional (0D) Sn and Pb halides. The results show that, despite the similarity in ground-state electronic structure between Sn and Pb halide perovskites, the chemically more active Sn²⁺ lone pair leads to stronger excited-state structural distortion and larger Stokes shift in Sn halides. The enhanced Stokes shift hinders excitation energy transport, which reduces energy loss to defects and increases the photoluminescence quantum efficiency. Finally, the presence of the ns² metal cations in the 0D halide perovskites also promotes the exciton dissociation into electron and hole polarons especially in all-inorganic compounds, in which the coupling between metal-halide clusters is significant.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1502553

Alternate ID(s):: OSTI ID: 1499071

Journal Information:: Physical Review Materials, Vol. 3, Issue 3; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 59 works

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Title: Impact of metal $n s^{2}$ lone pair on luminescence quantum efficiency in low-dimensional halide perovskites