ArticleProceedings of the National Academy of Sciences of the United States of America2022
Direct visualization of polaron formation in the thermoelectric SnSe.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2022. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 9 papers.
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9 citing papers in PubMed.
- Symmetry-protected topological polarons.Proceedings of the National Academy of Sciences of the United States of America · 2026Article
- Ultrafast surface melting of orbital order in LaNature materials · 2026Article
- Optical Conductivity and Photo-Induced Polaronic Formation in CoAdvanced science (Weinheim, Baden-Wurttemberg, Germany) · 2024Article
- Recent Progresses of Polarons: Fundamentals and Roles in Photocatalysis and Photoelectrocatalysis.Advanced science (Weinheim, Baden-Wurttemberg, Germany) · 2024Review
- Coherent charge hopping suppresses photoexcited small polarons in ErFeOScience advances · 2024Article
- Ultrafast electron diffuse scattering as a tool for studying phonon transport: Phonon hydrodynamics and second sound oscillations.Structural dynamics (Melville, N.Y.) · 2024Article
- Nonequilibrium Phonon Dynamics and Its Impact on the Thermal Conductivity of the Benchmark Thermoelectric Material SnSe.ACS nano · 2023Article
- Giant acceleration of polaron transport by ultrafast laser-induced coherent phonons.Science advances · 2023Article
- Direct Observation of Ultrafast Lattice Distortions during Exciton-Polaron Formation in Lead Halide Perovskite Nanocrystals.ACS nano · 2023Article
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Authors and funding
6 authors.
Funding
No grant is acknowledged in the PubMed record.
Abstract
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.
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