scholarly journals Direct visualization of polaron formation in the thermoelectric SnSe

2022 ◽  
Vol 119 (3) ◽  
pp. e2113967119
Author(s):  
Laurent P. René de Cotret ◽  
Martin R. Otto ◽  
Jan-Hendrik Pöhls ◽  
Zhongzhen Luo ◽  
Mercouri G. Kanatzidis ◽  
...  

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.

2021 ◽  
Vol 6 (1) ◽  
Author(s):  
Qing Dong ◽  
Quanjun Li ◽  
Shujia Li ◽  
Xuhan Shi ◽  
Shifeng Niu ◽  
...  

AbstractThe adoption of high pressure not only reinforces the comprehension of the structure and exotic electronic states of transition metal dichalcogenides (TMDs) but also promotes the discovery of intriguing phenomena. Here, 1T-TaS2 was investigated up to 100 GPa, and re-enhanced superconductivity was found with structural phase transitions. The discovered I4/mmm TaS2 presents strong electron–phonon coupling, revealing a good superconductivity of the nonlayered structure. The P–T phase diagram shows a dome shape centered at ~20 GPa, which is attributed to the distortion of the 1T structure. Accompanied by the transition to nonlayered structure above 44.5 GPa, the superconducting critical temperature shows an increasing trend and reaches ~7 K at the highest studied pressure, presenting superior superconductivity compared to the original layered structure. It is unexpected that the pressure-induced re-enhanced superconductivity was observed in TMDs, and the transition from a superconductor with complicated electron-pairing mechanism to a phonon-mediated superconductor would expand the field of pressure-modified superconductivity.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Kwangrae Kim ◽  
Hoon Kim ◽  
Jonghwan Kim ◽  
Changil Kwon ◽  
Jun Sung Kim ◽  
...  

AbstractCoulomb attraction between electrons and holes in a narrow-gap semiconductor or a semimetal is predicted to lead to an elusive phase of matter dubbed excitonic insulator. However, direct observation of such electronic instability remains extremely rare. Here, we report the observation of incipient divergence in the static excitonic susceptibility of the candidate material Ta2NiSe5 using Raman spectroscopy. Critical fluctuations of the excitonic order parameter give rise to quasi-elastic scattering of B2g symmetry, whose intensity grows inversely with temperature toward the Weiss temperature of TW ≈ 237 K, which is arrested by a structural phase transition driven by an acoustic phonon of the same symmetry at TC = 325 K. Concurrently, a B2g optical phonon becomes heavily damped to the extent that its trace is almost invisible around TC, which manifests a strong electron-phonon coupling that has obscured the identification of the low-temperature phase as an excitonic insulator for more than a decade. Our results unambiguously reveal the electronic origin of the phase transition.


2002 ◽  
Vol 65 (12) ◽  
Author(s):  
F. S. Tautz ◽  
M. Eremtchenko ◽  
J. A. Schaefer ◽  
M. Sokolowski ◽  
V. Shklover ◽  
...  

2016 ◽  
Vol 170 ◽  
pp. 357-363 ◽  
Author(s):  
M.G. Lahoud ◽  
R.C.G. Frem ◽  
D.A. Gálico ◽  
G. Bannach ◽  
M.M. Nolasco ◽  
...  

1978 ◽  
Vol 56 (5) ◽  
pp. 560-564
Author(s):  
Robert Barrie ◽  
H. -C. Chow

Special cases of the general result for Raman scattering from an impurity in a semiconductor are discussed. For weak electron–phonon coupling the zero-phonon and one-phonon scattering intensities are derived. For strong electron–phonon coupling a comparison is made between two different approximations that have been previously used.


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