Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets
Abstract
Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H4 and H5 and the degenerate H6 valence bands (VB) and the lowest degenerate H6 conduction band (CB) as well as a higher energy transition at the Lpoint. Surprisingly, the degeneracy of the H6 CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations, we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along the c-axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentiallymore »
- Authors:
-
- Univ. of Cincinnati, OH (United States). Dept. of Physics and Astronomy
- George Washington Univ., Washington, DC (United States). Dept. of Mechanical & Aerospace Engineering
- Purdue Univ., West Lafayette, IN (United States). School of Industrial Engineering
- Purdue Univ., West Lafayette, IN (United States). School of Electrical and Computer Engineering
- Univ. of California, Riverside, CA (United States). Materials Science & Engineering Program. Dept. of Chemical & Environmental Engineering
- Publication Date:
- Research Org.:
- Univ. of California, Riverside, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1802904
- Grant/Contract Number:
- SC0016269
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 77 NANOSCIENCE AND NANOTECHNOLOGY; Science & Technology - Other Topics
Citation Formats
Jnawali, Giriraj, Xiang, Yuan, Linser, Samuel M., Shojaei, Iraj Abbasian, Wang, Ruoxing, Qiu, Gang, Lian, Chao, Wong, Bryan M., Wu, Wenzhuo, Ye, Peide D., Leng, Yongsheng, Jackson, Howard E., and Smith, Leigh M. Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets. United States: N. p., 2020.
Web. doi:10.1038/s41467-020-17766-5.
Jnawali, Giriraj, Xiang, Yuan, Linser, Samuel M., Shojaei, Iraj Abbasian, Wang, Ruoxing, Qiu, Gang, Lian, Chao, Wong, Bryan M., Wu, Wenzhuo, Ye, Peide D., Leng, Yongsheng, Jackson, Howard E., & Smith, Leigh M. Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets. United States. https://doi.org/10.1038/s41467-020-17766-5
Jnawali, Giriraj, Xiang, Yuan, Linser, Samuel M., Shojaei, Iraj Abbasian, Wang, Ruoxing, Qiu, Gang, Lian, Chao, Wong, Bryan M., Wu, Wenzhuo, Ye, Peide D., Leng, Yongsheng, Jackson, Howard E., and Smith, Leigh M. Mon .
"Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets". United States. https://doi.org/10.1038/s41467-020-17766-5. https://www.osti.gov/servlets/purl/1802904.
@article{osti_1802904,
title = {Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets},
author = {Jnawali, Giriraj and Xiang, Yuan and Linser, Samuel M. and Shojaei, Iraj Abbasian and Wang, Ruoxing and Qiu, Gang and Lian, Chao and Wong, Bryan M. and Wu, Wenzhuo and Ye, Peide D. and Leng, Yongsheng and Jackson, Howard E. and Smith, Leigh M.},
abstractNote = {Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H4 and H5 and the degenerate H6 valence bands (VB) and the lowest degenerate H6 conduction band (CB) as well as a higher energy transition at the Lpoint. Surprisingly, the degeneracy of the H6 CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations, we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along the c-axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentially due to contributions of intervalley processes in the recombination rate. These new findings shed light on the strong correlation between photoinduced carriers and electronic structure in anisotropic crystals, which opens a potential pathway for designing novel Te-based devices that take advantage of the topological structures as well as strong spin-related properties.},
doi = {10.1038/s41467-020-17766-5},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Mon Aug 10 00:00:00 EDT 2020},
month = {Mon Aug 10 00:00:00 EDT 2020}
}
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