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Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden−Popper Hybrid Lead Iodide Perovskites

Publication ,  Journal Article
Li, T; Chen, X; Wang, X; Lu, H; Yan, Y; Beard, MC; Mitzi, DB
Published in: ACS Energy Letters
February 14, 2020

Hybrid organic−inorganic lead halide perovskites have shown promising results as active layers in light-emitting diodes, typically utilizing the near-monochromatic, free exciton emission. Some perovskite compounds, however, show broad-band emission that is more intense than the free exciton counterpart. In this study, we show that the light emission properties of Ruddlesden−Popper hybrid perovskites PEA2MAn−1PbnI3n+1 (PEA = phenethylammonium, MA = methylammonium) can be tuned by Sn alloying and are highly sensitive to Sn %. With increasing dimensionality, the broad-band emission quantum yield decreases drastically, from 23% in n = 1 to <1% for the n = 3 compound. Using density functional theory calculations and transient reflectance spectroscopy, the broad emission is identified as originating from self-trapped excitons. A dynamic picture of the formation process is also presented, for which ultrafast (<5 ps) hole-trapping at the Sn site is the first step, followed by electron localization from Coulombic interaction. These findings are especially valuable for designing perovskite materials with intense room-temperature broad-band emission for solid-state lighting applications.

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Published In

ACS Energy Letters

DOI

EISSN

2380-8195

Publication Date

February 14, 2020

Volume

5

Issue

2

Start / End Page

347 / 352

Related Subject Headings

  • 40 Engineering
  • 34 Chemical sciences
 

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Li, T., Chen, X., Wang, X., Lu, H., Yan, Y., Beard, M. C., & Mitzi, D. B. (2020). Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden−Popper Hybrid Lead Iodide Perovskites. ACS Energy Letters, 5(2), 347–352. https://doi.org/10.1021/acsenergylett.9b02490
Li, T., X. Chen, X. Wang, H. Lu, Y. Yan, M. C. Beard, and D. B. Mitzi. “Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden−Popper Hybrid Lead Iodide Perovskites.” ACS Energy Letters 5, no. 2 (February 14, 2020): 347–52. https://doi.org/10.1021/acsenergylett.9b02490.
Li T, Chen X, Wang X, Lu H, Yan Y, Beard MC, et al. Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden−Popper Hybrid Lead Iodide Perovskites. ACS Energy Letters. 2020 Feb 14;5(2):347–52.
Li, T., et al. “Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden−Popper Hybrid Lead Iodide Perovskites.” ACS Energy Letters, vol. 5, no. 2, Feb. 2020, pp. 347–52. Scopus, doi:10.1021/acsenergylett.9b02490.
Li T, Chen X, Wang X, Lu H, Yan Y, Beard MC, Mitzi DB. Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden−Popper Hybrid Lead Iodide Perovskites. ACS Energy Letters. 2020 Feb 14;5(2):347–352.
Journal cover image

Published In

ACS Energy Letters

DOI

EISSN

2380-8195

Publication Date

February 14, 2020

Volume

5

Issue

2

Start / End Page

347 / 352

Related Subject Headings

  • 40 Engineering
  • 34 Chemical sciences