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Spectral shifts upon halide segregation in perovskite nanocrystals observed via transient absorption spectroscopy

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Abstract

Lead halide perovskite nanocrystals (NCs) are promising for applications in light emitting devices owing to a strong emission spectrum that is tunable throughout the visible region by altering halide composition. However, in mixed-halide perovskite systems photoinduced migration drives formation of halide-segregated domains, altering the emission spectrum. The mechanism by which this segregation occurs is currently the subject of intense investigation. Processes involving the perovskite surface are expected to be of enhanced prevalence in NCs due to their large surface area to volume ratio. In this work, we use transient absorption spectroscopy to probe the excited-state dynamics of NCs before and after halide segregation. Comparison of global fit spectra of the measured signals suggests the accumulation of iodide at the surface, resulting in a redshifted emission spectrum.

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Acknowledgments

MLC acknowledges financial support from ARCS Oregon Chapter. This work was partially funded by the Engineering and Physical Sciences Research Council (EPSRC) UK through Grants EP/M005143/1 and EP/M015254/2. The authors thank Aditya Sadhalana (Clarendon Laboratory, Department of Physics, University of Oxford and Cavendish Laboratory, University of Cambridge) for assistance with sample preparation.

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Authors and Affiliations

  1. Department of Chemistry and Biochemistry, University of Oregon, Eugene, Oregon, 97403, USA

    Michael L. Crawford, James C. Sadighian & Cathy Y. Wong

  2. Clarendon Laboratory, Department of Physics, University of Oxford, Parks Road, Oxford, OX1 3PU, UK

    Yasser Hassan & Henry J. Snaith

  3. Oregon Center for Optical, Molecular, and Quantum Science, University of Oregon, Eugene, Oregon, 97403, USA

    Cathy Y. Wong

  4. Materials Science Institute, University of Oregon, Eugene, Oregon, 97403, USA

    Cathy Y. Wong

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  1. Michael L. Crawford
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  2. James C. Sadighian
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  3. Yasser Hassan
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  4. Henry J. Snaith
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  5. Cathy Y. Wong
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Crawford, M.L., Sadighian, J.C., Hassan, Y. et al. Spectral shifts upon halide segregation in perovskite nanocrystals observed via transient absorption spectroscopy. MRS Advances 5, 2613–2621 (2020). https://doi.org/10.1557/adv.2020.307

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  • DOI: https://doi.org/10.1557/adv.2020.307

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