Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites

Jonathan Zerhoch; Stanislav Bodnar; James E. Lerpinière; Shangpu Liu; Timo Neumann; Barbara Sergl; Markus W. Heindl; Andrii Shcherbakov; Ahmed Elghandour; Rüdiger Klingeler; Alison B. Walker; Felix Deschler

doi:10.1021/acs.jpclett.3c03466

Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites

Jonathan Zerhoch, Stanislav Bodnar, James E. Lerpinière, Shangpu Liu, Timo Neumann, Barbara Sergl, Markus W. Heindl, Andrii Shcherbakov, Ahmed Elghandour, Rüdiger Klingeler, Alison B. Walker, Felix Deschler

Research output: Contribution to journal › Article › peer-review

Abstract

Spin-orbit coupling in the electronic states of solution-processed hybrid metal halide perovskites forms complex spin-textures in the band structures and allows for optical manipulation of the excited state spin-polarizations. Here, we report that motional narrowing acts on the photoexcited spin-polarization in CH₃NH₃PbBr₃ thin films, which are doped at percentage-level with Mn²⁺ ions. Using ultrafast circularly polarized broadband transient absorption spectroscopy at cryogenic temperatures, we investigate the spin population dynamics in these doped hybrid perovskites and find that spin relaxation lifetimes are increased by a factor of 3 compared to those of undoped materials. Using quantitative analysis of the photoexcitation cooling processes, we reveal increased carrier scattering rates in the doped perovskites as the fundamental mechanism driving spin-polarization-maintaining motional narrowing. Our work reports transition-metal doping as a concept to extend spin lifetimes of hybrid perovskites.

Original language	English
Pages (from-to)	2851-2858
Number of pages	8
Journal	Journal of Physical Chemistry Letters
Volume	15
Issue number	10
Early online date	5 Mar 2024
DOIs	https://doi.org/10.1021/acs.jpclett.3c03466
Publication status	Published - 14 Mar 2024

Data Availability Statement

Data files presented in this manuscript can be found at https://doi.org/10.11588/data/VM8ZKT.

Funding

This project has received funding from the European Research Council (ERC Starting Grant agreement no. 852084 ─ TWIST). J.E.L. would like to thank the University of Bath for a studentship and the UK Engineering and Physical Sciences Research Council grant Supergen Solar Network+, EP/S000763/1 for travel funding. T.N. acknowledges funding from the Winton programme for the Physics of Sustainability.

Funders	Funder number
Engineering and Physical Sciences Research Council	EP/S000763/1
European Research Council	852084
University of Bath

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

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10.1021/acs.jpclett.3c03466Licence: CC BY

Cite this

Zerhoch, J., Bodnar, S., Lerpinière, J. E., Liu, S., Neumann, T., Sergl, B., Heindl, M. W., Shcherbakov, A., Elghandour, A., Klingeler, R., Walker, A. B., & Deschler, F. (2024). Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites. Journal of Physical Chemistry Letters, 15(10), 2851-2858. https://doi.org/10.1021/acs.jpclett.3c03466

Zerhoch, J, Bodnar, S, Lerpinière, JE, Liu, S, Neumann, T, Sergl, B, Heindl, MW, Shcherbakov, A, Elghandour, A, Klingeler, R, Walker, AB & Deschler, F 2024, 'Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites', Journal of Physical Chemistry Letters, vol. 15, no. 10, pp. 2851-2858. https://doi.org/10.1021/acs.jpclett.3c03466

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abstract = "Spin-orbit coupling in the electronic states of solution-processed hybrid metal halide perovskites forms complex spin-textures in the band structures and allows for optical manipulation of the excited state spin-polarizations. Here, we report that motional narrowing acts on the photoexcited spin-polarization in CH3NH3PbBr3 thin films, which are doped at percentage-level with Mn2+ ions. Using ultrafast circularly polarized broadband transient absorption spectroscopy at cryogenic temperatures, we investigate the spin population dynamics in these doped hybrid perovskites and find that spin relaxation lifetimes are increased by a factor of 3 compared to those of undoped materials. Using quantitative analysis of the photoexcitation cooling processes, we reveal increased carrier scattering rates in the doped perovskites as the fundamental mechanism driving spin-polarization-maintaining motional narrowing. Our work reports transition-metal doping as a concept to extend spin lifetimes of hybrid perovskites.",

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AU - Zerhoch, Jonathan

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AU - Liu, Shangpu

AU - Neumann, Timo

AU - Sergl, Barbara

AU - Heindl, Markus W.

AU - Shcherbakov, Andrii

AU - Elghandour, Ahmed

AU - Klingeler, Rüdiger

AU - Walker, Alison B.

AU - Deschler, Felix

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AB - Spin-orbit coupling in the electronic states of solution-processed hybrid metal halide perovskites forms complex spin-textures in the band structures and allows for optical manipulation of the excited state spin-polarizations. Here, we report that motional narrowing acts on the photoexcited spin-polarization in CH3NH3PbBr3 thin films, which are doped at percentage-level with Mn2+ ions. Using ultrafast circularly polarized broadband transient absorption spectroscopy at cryogenic temperatures, we investigate the spin population dynamics in these doped hybrid perovskites and find that spin relaxation lifetimes are increased by a factor of 3 compared to those of undoped materials. Using quantitative analysis of the photoexcitation cooling processes, we reveal increased carrier scattering rates in the doped perovskites as the fundamental mechanism driving spin-polarization-maintaining motional narrowing. Our work reports transition-metal doping as a concept to extend spin lifetimes of hybrid perovskites.

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Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites

Abstract

Data Availability Statement

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