Magneto-spectroscopy studies provide direct evidence for the coupling of excitons to organic ligand vibrations in 2D RP perovskites
Joanna Urban a, Gabriel Chehade a, Mateusz Dyksik b c, Matan Menahem d, Alessandro Surrente b, Galle Trippé-Allard a, Duncan Maude b, Damien Garrot e, Omer Yaffe d, Emmauelle Deleporte a, Paulina Plochocka b, Michal Baranowski b c
a Laboratoire Lumière, Matière et Interfaces, Université Paris-Saclay, ENS Paris-Saclay, CNRS, CentraleSupelec, 91405 Orsay Cedex, France
b Laboratoire National des Champs Magnétiques Intenses, UPR 3228,CNRS-UGA-UPS-INSA, Grenoble and Toulouse, France
c Department of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, Wroclaw, Poland
d Department of Materials and Interfaces, Weizmann Institute of Science, Rehovot 76100, Israel
e Groupe d’Etude de la Matière Condensée, Université de Versailles Saint Quentin En Yvelines, Université Paris-Saclay, Avenue des États Unis, 45, Versailles, France
International Conference on Hybrid and Organic Photovoltaics
Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Online, Spain, 2021 May 24th - 28th
Organizers: Marina Freitag, Feng Gao and Sam Stranks
Oral, Joanna Urban, presentation 014
Publication date: 11th May 2021

Layered Ruddlesden-Popper (RP) perovskites are promising candidates for optoelectronic applications due to their excellent stability and excitonic properties. These natural quantum well structures consisting of inorganic layers separated by large organic spacers have been known since several decades. However, only lately attention has turned towards investigating the distinctive nature of the exciton-phonon coupling as the driving mechanism for  many of their unique properties [1].

In this work we show that despite the assumed confinement of the excitons withing the inorganic layers, for certain ligands significant coupling of the excitons to the vibrations of the organic part can occur. We investigated the RP perovskite (PEA)2(MA)n-1PbnI3n+1 (PEPI) [2] with a varying number of inorganic layers n=1,2,3 using magneto-transmission in magnetic fields up to 68 T [3]. In the transmission spectra we could identify periodically spaced features separated by around 40 meV which we assign as phonon replicas of the main excitonic transition. Our interpretation is strongly supported by the identical shifts of the features in magnetic field suggesting their common origin. The mode around 40 meV has been previously identified as the vibration of the PEA cation [1]. The observed coupling is an evidence of the leakage of the excitonic wavefunction into the organic barrier layer due to weaker dielectric confinement  induced by the PEA cations as compared to alkyl chains.

M.B. and P.P. appreciates support from National Science Centre Poland within the OPUS program (grant no. 2019/33/B/ST3/01915). This work was partially supported by OPEP project, which received funding from the ANR-10-LABX-0037-NEXT. J.M.U., E.D., G.T.-A., and G.C. have received fundings from the Agence Nationale pour la Recherche, ANR-18-CE24-006 (EMIPERO). M.D. appreciates support from the Polish National Agency for Academic Exchange within the Bekker programme (grant no. PPN/BEK/2019/1/00312/U/00001).

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