Direct visualization of polaron formation in the thermoelectric SnSe

SnSe is a layered material that currently holds the record for bulk thermoelectric efficiency. The primary determinant of this high efficiency is thought to be the anomalously low thermal conductivity resulting from strong anharmonic coupling within the phonon system. Here we show that the nature of...

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Bibliographic Details
Published in:Proceedings of the National Academy of Sciences - PNAS 2022-01, Vol.119 (3)
Main Authors: René de Cotret, Laurent P, Otto, Martin R, Pöhls, Jan-Hendrik, Luo, Zhongzhen, Kanatzidis, Mercouri G, Siwick, Bradley J
Format: Article
Language:English
Subjects:
Anharmonicity
Anisotropy
CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Coupling
Electron diffraction
electron-phonon coupling
Electrons
Localization
MATERIALS SCIENCE
Phonons
Physical Sciences
Polarons
Thermal conductivity
thermoelectric
Thermoelectricity
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Summary:SnSe is a layered material that currently holds the record for bulk thermoelectric efficiency. The primary determinant of this high efficiency is thought to be the anomalously low thermal conductivity resulting from strong anharmonic coupling within the phonon system. Here we show that the nature of the carrier system in SnSe is also determined by strong coupling to phonons by directly visualizing polaron formation in the material. We employ ultrafast electron diffraction and diffuse scattering to track the response of phonons in both momentum and time to the photodoping of free carriers across the bandgap, observing the bimodal and anisotropic lattice distortions that drive carrier localization. Relatively large (18.7 Å), quasi-one-dimensional (1D) polarons are formed on the 300-fs timescale with smaller (4.2 Å) 3D polarons taking an order of magnitude longer (4 ps) to form. This difference appears to be a consequence of the profoundly anisotropic electron-phonon coupling in SnSe, with strong Fröhlich coupling only to zone-center polar optical phonons. These results demonstrate a high density of polarons in SnSe at optimal doping levels. Strong electron-phonon coupling is critical to the thermoelectric performance of this benchmark material and, potentially, high performance thermoelectrics more generally.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.2113967119