Making and breaking the exciton in layered halide hybrid perovskites
Mikael Kepenekian a, Boubacar Traore a, Jean-Christophe Blancon b, Hsinhan Tsai b, Wanyi Nie b, Konstantinos Stoumpos c, Laurent Pedesseau d, Claudine Katan a, Sergei Tretiak b, Mercouri Kanatzidis c, Jacky Even d, Aditya Mohite b
a Institut des Sciences Chimiques de Rennes, CNRS, Université de Rennes 1, Ecole Nationale Supérieure de Chimie de Rennes, INSA Rennes, Rennes, France
b Los Alamos National Laboratory, US, MS-J567, Los Alamos, NM 87545, United States
c Department of Materials Science and Engineering, Northwestern University, Evanston, Evanston, Illinois, EE. UU., Evanston, United States
d Univ Rennes, INSA Rennes, CNRS, Institut FOTON - UMR6082, France, France
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2018 (NFM18)
S7 Fundamental Aspects of Perovskite Solar Cells and Optoelectronics
Torremolinos, Spain, 2018 October 22nd - 26th
Organizers: Laura Herz and Tze-Chien Sum
Oral, Mikael Kepenekian, presentation 193
DOI: https://doi.org/10.29363/nanoge.nfm.2018.193
Publication date: 6th July 2018

Layered halide hybrid organic−inorganic perovskites [1] have been the subject of intense investigation before the rise of three-dimensional (3D) halide perovskites and their impressive performance in solar cells. Recently, layered perovskites have also been proposed as attractive alternatives for photostable solar cells [2] and revisited for light-emitting devices. Interestingly, these performances can be traced back to extremely efficient internal exciton dissociation through edge states identified on thin films and single crystals [3].

Layered perovskites present fascinating features with inherent quantum and dielectric confinements imposed by the organic layers sandwiching the inorganic core, and computational approaches have successfully help rationalized their properties (excitonic, Rashba effects, etc.) [4-6]. Here, we propose a joint spectroscopic and computational investigation to unravel the origin of the recently identified layer-edge states in layered Ruddlesden-Popper phases with inorganic layers containing n = 1 to 4 octahedra. We show that for n > 2, the system presents a localized surface state within the band gap.

Based on our conclusion, we propose an elastic model providing design principles for future layered perovskites with optimized properties for photovoltaics or light emission.

 

References

[1] L. Pedesseau et al., ACS Nano (2016), 10, 9776.

[2] H. Tsai et al.,Nature (2016), 536, 312.

[3] J.-C. Blancon et al., Science (2017), 355, 1288.

[4] M. Kepenekian et al., ACS Nano (2015), 12, 11557.

[5] D. Sapori, M. Kepenekian, L. Pedesseau, C. Katan, J. Even, Nanoscale (2016), 8, 6369.

[6] M. D. Smith et al., Chem. Sci. (2017), 8, 1960.

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