The Physics of Interlayer Exciton Delocalization in Ruddlesden-Popper Lead Halide Perovskites
David Giovanni a, Sankaran Ramesh a b, Marcello Righetto a, Jia Wei Melvin Lim a b, Qiannan Zhang a, Yue Wang a, Senyun Ye a, Qiang Xu a, Nripan Mathews c d, Tze Chien Sum a
a NTU Singapore - Nanyang Technological University, Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Link, 21, Singapore, Singapore
b Energy Research Institute @NTU (ERI@N), Interdisciplinary Graduate Programme, Nanyang Technological University, Singapore
c Energy Research Institute @ NTU (ERI@N), Research Technoplaza, Nanyang Technological University, Singapore, Nanyang Drive, Singapore, Singapore
d NTU Singapore - Nanyang Technological University, School of Materials Science and Engineering, Nanyang Avenue, 50, Singapore, Singapore
Proceedings of Online Conference on Perovskites for Energy Harvesting: From Fundamentals to Devices (PERENHAR)
Online, Spain, 2020 November 19th - 20th
Organizers: Dinesh Kabra, Sandheep Ravishankar, Angshuman Nag and Priya Mahadevan
Poster, Sankaran Ramesh, 068
Publication date: 2nd November 2020

Two-dimensional (2D) lead halide Ruddlesden-Popper perovskites (RPP) recently emerged as a prospective material system for optoelectronic applications. Their self-assembled multi quantum-well structure gives rise to the novel inter-well energy funnelling phenomenon, which is of broad interests for photovoltaics, light-emission applications and in emerging technologies (e.g., spintronics). Herein, we developed a realistic finite quantum-well superlattice model that corroborates the hypothesis of exciton delocalization across different quantum-wells in RPP. Such delocalization leads to a sub-50 fs coherent energy transfer between adjacent wells, with the efficiency depending on the RPP phase matching and the organic large cation barrier lengths. Our approach provides a coherent and comprehensive account for both steady-state and transient dynamical experimental results in RPPs. Importantly, these findings pave the way for a deeper understanding of the physics underpinning these systems crucial for establishing materials design-rules to realize efficient RPP-based devices.

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