Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites

Author:

Posmyk Katarzyna1ORCID,Dyksik Mateusz1ORCID,Surrente Alessandro1ORCID,Zalewska Katarzyna1,Śmiertka Maciej1,Cybula Ewelina1,Paritmongkol Watcharaphol2ORCID,Tisdale William A.2ORCID,Plochocka Paulina13ORCID,Baranowski Michał1ORCID

Affiliation:

1. Department of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, Poland

2. Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

3. Laboratoire National des Champs Magnétiques Intenses, EMFL, CNRS UPR 3228, Université Toulouse, Université Toulouse 3, INSA-T, 31400 Toulouse, France

Abstract

Two-dimensional van der Waals materials exhibit particularly strong excitonic effects, which causes them to be an exceptionally interesting platform for the investigation of exciton physics. A notable example is the two-dimensional Ruddlesden–Popper perovskites, where quantum and dielectric confinement together with soft, polar, and low symmetry lattice create a unique background for electron and hole interaction. Here, with the use of polarization-resolved optical spectroscopy, we have demonstrated that the simultaneous presence of tightly bound excitons, together with strong exciton–phonon coupling, allows for observing the exciton fine structure splitting of the phonon-assisted transitions of two-dimensional perovskite (PEA)2PbI4, where PEA stands for phenylethylammonium. We demonstrate that the phonon-assisted sidebands characteristic for (PEA)2PbI4 are split and linearly polarized, mimicking the characteristics of the corresponding zero-phonon lines. Interestingly, the splitting of differently polarized phonon-assisted transitions can be different from that of the zero-phonon lines. We attribute this effect to the selective coupling of linearly polarized exciton states to non-degenerate phonon modes of different symmetries resulting from the low symmetry of (PEA)2PbI4 lattice.

Funder

National Science Centre Poland

U.S. Department of Energy, Office of Science, Basic Energy Sciences

EUR

Publisher

MDPI AG

Subject

General Materials Science,General Chemical Engineering

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