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Evidence of large polarons in photoemission band mapping of the perovskite semiconductor CsPbBr3

Michele Puppin1*, Serhii Polishchuk1, Nicola Colonna2*, Alberto Crepaldi3, Dmitry Dirin4,5, Olga Nazarenko4,5, Riccardo De Gennaro2*, Gianmarco Gatti3, Silvan Roth3, Thomas Barillot1, Luca Poletto6, Rui Patrick Xian7, Laurenz Rettig7, Martin Wolf7, Ralph Ernstorfer7, Maksym V. Kovalenko4,5, Nicola Marzari2*, Marco Grioni3*, Majed Chergui1*

1 Laboratoire de Spectroscopie Ultrarapide and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne, ISIC, Station 6, CH-1015 Lausanne, Switzerland

2 Theory and Simulations of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland

3 Institute of Physics and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland

4 Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland

5 Laboratory for Thin Films and Photovoltaics, EMPA Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland

6 National Research Council of Italy—Institute of Photonics and Nanotechnologies (CNR-IFN), via Trasea 7, 35131 Padova, Italy

7 Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany

* Corresponding authors emails: michele.puppin@epfl.ch, nicola.colonna@psi.ch, riccardo.degennaro@epfl.ch, nicola.marzari@epfl.ch, marco.grioni@epfl.ch, majed.chergui@epfl.ch
DOI10.24435/materialscloud:gb-90 [version v1]

Publication date: Oct 14, 2020

How to cite this record

Michele Puppin, Serhii Polishchuk, Nicola Colonna, Alberto Crepaldi, Dmitry Dirin, Olga Nazarenko, Riccardo De Gennaro, Gianmarco Gatti, Silvan Roth, Thomas Barillot, Luca Poletto, Rui Patrick Xian, Laurenz Rettig, Martin Wolf, Ralph Ernstorfer, Maksym V. Kovalenko, Nicola Marzari, Marco Grioni, Majed Chergui, Evidence of large polarons in photoemission band mapping of the perovskite semiconductor CsPbBr3, Materials Cloud Archive 2020.124 (2020), doi: 10.24435/materialscloud:gb-90.

Description

Lead-halide perovskite (LHP) semiconductors are emergent optoelectronic materials with outstanding transport properties which are not yet fully understood. We find signatures of large polaron formation in the electronic structure of the inorganic LHP CsPbBr3 by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass of 0.26±0.02 me, 50% heavier than the bare mass m0=0.17 me predicted by ab-initio calculations. Calculations of the electron-phonon coupling indicate that phonon dressing of the carriers mainly occurs via distortions of the Pb-Br bond with a Fröhlich coupling parameter α=1.82. A good agreement between theoretical and experimental data is obtained within the Feynman polaron model, validating a viable theoretical method to predict the carrier effective mass of LHPs ab initio.

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Keywords

EPFL MARVEL Lead halide Perovskites Fröhilch polarons Angle-resolved photoelectron spectroscopy Density functional theory Hybrid functionals GW method Electron-phonon coupling ERC SNSF

Version history:

2020.124 (version v1) [This version] Oct 14, 2020 DOI10.24435/materialscloud:gb-90