Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites

Bo Wu, Haifeng Yuan, Qiang Xu, Julian A. Steele, David Giovanni, Pascal Puech, Jianhui Fu, Yan Fong Ng, Nur Fadilah Jamaludin, Ankur Solanki, Subodh Mhaisalkar, Nripan Mathews, Maarten B. J. Roeffaers, Michael Grätzel, Johan Hofkens () and Tze Chien Sum ()
Additional contact information
Bo Wu: South China Normal University
Haifeng Yuan: KU Leuven
Qiang Xu: Nanyang Technological University
Julian A. Steele: KU Leuven
David Giovanni: Nanyang Technological University
Pascal Puech: University of Toulouse
Jianhui Fu: Nanyang Technological University
Yan Fong Ng: Nanyang Technological University
Nur Fadilah Jamaludin: Nanyang Technological University
Ankur Solanki: Nanyang Technological University
Subodh Mhaisalkar: Nanyang Technological University
Nripan Mathews: Nanyang Technological University
Maarten B. J. Roeffaers: KU Leuven
Michael Grätzel: Energy Research Institute @NTU (ERI@N), Research Techno Plaza
Johan Hofkens: KU Leuven
Tze Chien Sum: Nanyang Technological University

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications.

Date: 2019
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DOI: 10.1038/s41467-019-08326-7

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