Evidence of Large Polarons in Photoemission Band Mapping of the Perovskite Semiconductor CsPbBr_{3}.


Journal

Physical review letters
ISSN: 1079-7114
Titre abrégé: Phys Rev Lett
Pays: United States
ID NLM: 0401141

Informations de publication

Date de publication:
22 May 2020
Historique:
revised: 30 03 2020
received: 02 09 2019
accepted: 14 04 2020
entrez: 6 6 2020
pubmed: 6 6 2020
medline: 6 6 2020
Statut: ppublish

Résumé

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 CsPbBr_{3} by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass of 0.26±0.02 m_{e}, 50% heavier than the bare mass m_{0}=0.17 m_{e} predicted by density functional theory. 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=1.81. A good agreement with our experimental data is obtained within the Feynman polaron model, validating a viable theoretical method to predict the carrier effective mass of LHPs ab initio.

Identifiants

pubmed: 32501104
doi: 10.1103/PhysRevLett.124.206402
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

206402

Auteurs

M Puppin (M)

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

S Polishchuk (S)

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

N Colonna (N)

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.

A Crepaldi (A)

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

D N Dirin (DN)

Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland.
Laboratory for Thin Films and Photovoltaics, EMPA Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland.

O Nazarenko (O)

Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland.
Laboratory for Thin Films and Photovoltaics, EMPA Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland.

R De Gennaro (R)

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.

G Gatti (G)

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

S Roth (S)

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

T Barillot (T)

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

L Poletto (L)

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

R P Xian (RP)

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

L Rettig (L)

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

M Wolf (M)

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

R Ernstorfer (R)

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

M V Kovalenko (MV)

Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland.
Laboratory for Thin Films and Photovoltaics, EMPA Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland.

N Marzari (N)

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.

M Grioni (M)

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

M Chergui (M)

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

Classifications MeSH