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 L-point. 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.

The complex band structure and carrier decay response upon photoexcitation of the chiral semiconductor tellurium remain to be unveiled. Here, the authors report unusual dynamic band modifications in Te near band-edge structure due to photoinduced symmetry breaking and strong anisotropy in carrier decay dynamics.

Details

Title
Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets
Author
Giriraj, Jnawali 1   VIAFID ORCID Logo  ; Yuan, Xiang 2   VIAFID ORCID Logo  ; Linser, Samuel M 1 ; Shojaei, Iraj Abbasian 1 ; Wang Ruoxing 3 ; Qiu Gang 4   VIAFID ORCID Logo  ; Chao, Lian 5 ; Wong, Bryan M 5   VIAFID ORCID Logo  ; Wu Wenzhuo 3 ; Ye, Peide D 4 ; Leng Yongsheng 2 ; Jackson, Howard E 1 ; Smith, Leigh M 1   VIAFID ORCID Logo 

 University of Cincinnati, Department of Physics and Astronomy, Cincinnati, USA (GRID:grid.24827.3b) (ISNI:0000 0001 2179 9593) 
 The George Washington University, Department of Mechanical & Aerospace Engineering, Washington, USA (GRID:grid.253615.6) (ISNI:0000 0004 1936 9510) 
 Purdue University, School of Industrial Engineering, West Lafayette, USA (GRID:grid.169077.e) (ISNI:0000 0004 1937 2197) 
 Purdue University, School of Electrical and Computer Engineering, West Lafayette, USA (GRID:grid.169077.e) (ISNI:0000 0004 1937 2197) 
 University of California, Riverside, Department of Chemical & Environmental Engineering, Materials Science & Engineering Program, Riverside, USA (GRID:grid.266097.c) (ISNI:0000 0001 2222 1582) 
Publication year
2020
Publication date
2020
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2432264257
Copyright
© The Author(s) 2020. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.