Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c02500
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Funding
- University Grants Commission (UGC), New Delhi
- INSPIRE fellowship from SERB, New Delhi
- SERB [CRG/2020/000084, STR/2021/000001]
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Semiconductor nanostructures with near-unity photoluminescence quantum yields (PLQYs) are crucial for light-emitting diodes and display devices. This study achieved a high PLQY by stabilizing Sn2+ in a perovskite structure, and found that a longer spacer molecule and out-of-plane octahedral tilting favored higher PLQY. Self-trapped excitons (STEs) were also identified and their characteristics under different conditions were analyzed.
Semiconductor nanostructures with near-unity photoluminescence quantum yields (PLQYs) are imperative for light-emitting diodes and display devices. A PLQY of 99.7 +/- 0.3% has been obtained by stabilizing 91% Sn2+ in the Dion-Jacobson (8N8)SnBr4 (8N8 DJ) perovskite with 1,8-diaminooctane (8N8) spacer. The PLQY is favored by a longer spacer molecule and out-of-plane octahedral tilting. The PLQY shows one-month ambient stability under high relative humidity (RH) and temperature. With n-octylamine (8N) spacer, Ruddlesden-Popper (8N)2SnBr4 (8N-RP) also shows PLQY of 91.7 +/- 0.6%, but it has poor ambient stability. The 5-300 K PL experiments decipher the self-trapped excitons (STEs) where the self-trapping depth is 25.6 +/- 0.4 meV below the conduction band because of strong carrier-phonon coupling. The microsecond long-lived STE dominates over the band edge (BE) peaks at lower excitation wavelengths and higher temperatures. The higher PLQY and stability of 8N8-DJ are due to the stronger interaction between SnBr64- octahedra and 8N8 spacer, leading to a rigid structure.
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