Pressure-controlled free exciton and self-trapped exciton emission in quasi-one-dimensional hybrid lead bromides

Bin Xu, Yawen Li, Peibin Hong, Peijie Zhang, Jiang Han, Zewen Xiao and Zewei Quan ()
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Bin Xu: Southern University of Science and Technology (SUSTech), Shenzhen
Yawen Li: Southern University of Science and Technology (SUSTech), Shenzhen
Peibin Hong: Southern University of Science and Technology (SUSTech), Shenzhen
Peijie Zhang: Southern University of Science and Technology (SUSTech), Shenzhen
Jiang Han: Southern University of Science and Technology (SUSTech), Shenzhen
Zewen Xiao: Huazhong University of Science and Technology
Zewei Quan: Southern University of Science and Technology (SUSTech), Shenzhen

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Hybrid metal halides represent a novel type of semiconductor light emitters with intriguing excitonic emission properties, including free exciton emission and self-trapped exciton emission. Achieving precise control over these two excitonic emissions in hybrid metal halides is highly desired yet remains challenging. Here, the complete transformation from intrinsically broadband self-trapped exciton emission to distinctively sharp free exciton emission in a quasi-one-dimensional hybrid metal halide (C2H10N2)8[Pb4Br18]·6Br with a ribbon width of n = 4, is successfully achieved based on high-pressure method. During compression, pressure-induced phonon hardening continuously reduces exciton–phonon coupling, therefore suppressing excitonic localization and quenching the original self-trapped exciton emission. Notably, further compression triggers excitonic delocalization to induce intense free exciton emission, accompanied with reduced carrier effective masses and improved charge distribution. Controlled high-pressure investigations indicate that the ribbon width of n > 2 is necessary to realize excitonic delocalization and generate free exciton emissions in similar quasi-one-dimensional hybrid metal halides. This work presents an important photophysical process of excitonic transitions from self-trapped exciton emission to free exciton emission in quasi-one-dimensional hybrid metal halides without chemical regulation, promoting the rational synthesis of hybrid metal halides with desired excitonic emissions.

Date: 2024
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DOI: 10.1038/s41467-024-51836-2

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