Disorder and diffuse scattering in single-chirality (TaSe4)2I crystals

The quasi-one-dimensional chiral compound (TaSe4)2I has been extensively studied as a prime example of a topological Weyl semimetal. Upon crossing its phase transition temperature T_CDW ≈ 263 K, (TaSe4)2I exhibits incommensurate charge density wave (CDW) modulations described by the well-defined propagation vector ∼(0.05, 0.05, 0.11), oblique to the TaSe4 chains. Although optical and transport properties greatly depend on chirality, there is no systematic report about chiral domain size for (TaSe4)2I. In this study, our single-crystal scattering refinements reveal a bulk iodine deficiency, and Flack parameter measurements on multiple crystals demonstrate that separate (TaSe4)2I crystals have uniform handedness, supported by direct imaging and helicity dependent THz emission spectroscopy. Our single-crystal X-ray scattering and calculated diffraction patterns identify multiple diffuse features and create a real-space picture of the temperature-dependent (TaSe4)2I crystal structure. The short-range diffuse features are present at room temperature and decrease in intensity as the CDW modulation develops. These transverse displacements, along with electron pinning from the iodine deficiency, help explain why (TaSe4)2I behaves as an electronic semiconductor at temperatures above and below T_CDW, despite a metallic band structure calculated from density functional theory of the ideal structure.

Name thesis:degree_name

M.S.

Level thesis:degree_level

Thesis

Discipline thesis:degree_discipline

Materials Science & Engr

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2023

Author dc:creator

• Christensen, Jacob Andrew

Contributors dc:contributor

• Shoemaker, Daniel P

• Charge Density Waves
• Peierls Transition
• Topological Materials
• Pump-probe Spectroscopy
• Scanning Transmission Electron Microscopy
• X-ray Diffraction
• Chiral Symmetry
• Lattice Modeling

Statement dc:rights

• Copyright 2023 Jacob Andrew Christensen

Language dc:language

en, eng

Handle dc:identifier

https://hdl.handle.net/2142/122172

OAI record oai:identifier

https://www.ideals.illinois.edu/oai-pmh?verb=GetRecord&metadataPrefix=etdms&identifier=oai%3Awww.ideals.illinois.edu%3A2142%2F122172