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Metal Coordination Sphere Deformation Induced Highly Stokes-Shifted,Ultra Broadband Emission in 2D Hybrid Lead-Bromide Perovskites and Investigation of Its Origin
Authors:Benny Febriansyah  Dr Tetiana Borzda  Dr Daniele Cortecchia  Dr Stefanie Neutzner  Dr Giulia Folpini  Dr Teck Ming Koh  Dr Yongxin Li  Prof Nripan Mathews  Prof Annamaria Petrozza  Prof Jason England
Institution:1. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore, 637371 Singapore

Energy Research Institute at Nanyang Technological University (ERI@N), Research Techno Plaza, X-Frontier Block Level 5, 50 Nanyang Drive, Singapore, 637553 Singapore

Interdiscipinary Graduate School (IGS), 50 Nanyang Avenue, Singapore, 639798 Singapore

These authors contributed equally to this work.;2. Center for Nano Science and Technology@Polimi, Istituto Italiano di Tecnologia, 8 via Giovanni Pascoli 70/3, 20133 Milan, Italy

These authors contributed equally to this work.;3. Center for Nano Science and Technology@Polimi, Istituto Italiano di Tecnologia, 8 via Giovanni Pascoli 70/3, 20133 Milan, Italy;4. Energy Research Institute at Nanyang Technological University (ERI@N), Research Techno Plaza, X-Frontier Block Level 5, 50 Nanyang Drive, Singapore, 637553 Singapore;5. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore, 637371 Singapore;6. Energy Research Institute at Nanyang Technological University (ERI@N), Research Techno Plaza, X-Frontier Block Level 5, 50 Nanyang Drive, Singapore, 637553 Singapore

School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798 Singapore

Abstract:Published studies of layered (2D) (100)-oriented hybrid lead-bromide perovskites evidence a correlation between increased inter-octahedral (Pb-Br-Pb) distortions and the appearance of broadband white light emission. However, the impact of distortions within their constituent PbBr6]4? octahedra has yet to be assessed. Herein, we report two new (100)-oriented 2D Pb-Br perovskites, whose structures display unusually high intra-octahedral distortions, whilst retaining minimal inter-octahedral distortions. Using a combination of temperature-dependent, power-dependent and time-resolved photoluminescence spectroscopic measurements, we show that increased intra-octahedral distortion induces exciton localization processes and leads to formation of multiple photoinduced emissive colour centres. Ultimately, this leads to highly Stokes-shifted, ultrabroad white light emission at room temperature.
Keywords:crystal engineering  intra-octahedral distortion  lead-bromide perovskites  photophysics  white-light emission
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