Michele Puppin^1*, Serhii Polishchuk¹, Nicola Colonna^2*, Alberto Crepaldi³, Dmitry Dirin^4,5, Olga Nazarenko^4,5, Riccardo De Gennaro^2*, Gianmarco Gatti³, Silvan Roth³, Thomas Barillot¹, Luca Poletto⁶, Rui Patrick Xian⁷, Laurenz Rettig⁷, Martin Wolf⁷, Ralph Ernstorfer⁷, Maksym V. Kovalenko^4,5, Nicola Marzari^2*, Marco Grioni^3*, Majed Chergui^1*

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.

Materials Cloud sections using this data

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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