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Band hybridization at the semimetal-semiconductor transition of Ta2NiSe5 enabled by mirror-symmetry breaking

Matthew D. Watson, Igor Marković, Edgar Abarca Morales, Patrick Le Fèvre, Michael Merz, Amir A. Haghighirad, and Philip D. C. King
Phys. Rev. Research 2, 013236 – Published 2 March 2020
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Abstract

We present a combined study from angle-resolved photoemission and density-functional-theory calculations of the temperature-dependent electronic structure in the excitonic insulator candidate Ta2NiSe5. Our experimental measurements unambiguously establish the normal state as a semimetal with a significant band overlap of >100 meV. Our temperature-dependent measurements indicate how these low-energy states hybridize when cooling through the well-known 327 K phase transition in this system. From our calculations and polarization-dependent photoemission measurements, we demonstrate the importance of a loss of mirror symmetry in enabling the band hybridization, driven by a shearlike structural distortion which reduces the crystal symmetry from orthorhombic to monoclinic. Our results thus point to the key role of the lattice distortion in enabling the phase transition of Ta2NiSe5.

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  • Received 5 December 2019
  • Accepted 31 January 2020
  • Corrected 27 August 2020

DOI:https://doi.org/10.1103/PhysRevResearch.2.013236

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Corrections

27 August 2020

Correction: A missing statement of support has been inserted in the Acknowledgments.

Authors & Affiliations

Matthew D. Watson1,*, Igor Marković1,2, Edgar Abarca Morales1,2, Patrick Le Fèvre3, Michael Merz4, Amir A. Haghighirad4, and Philip D. C. King1,†

  • 1SUPA, School of Physics and Astronomy, University of St Andrews, St Andrews KY16 9SS, United Kingdom
  • 2Max Planck Institute for Chemical Physics of Solids, Nöthnitzer Strasse 40, 01187 Dresden, Germany
  • 3Synchrotron SOLEIL, L'Orme des Merisiers, Saint-Aubin-BP48, 91192 Gif-sur-Yvette, France
  • 4Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology, 76021 Karlsruhe, Germany

  • *matthew.watson@diamond.ac.uk
  • philip.king@st-andrews.ac.uk

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Vol. 2, Iss. 1 — March - May 2020

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  • Figure 1
    Figure 1

    (a) Crystal structure of Ta2NiSe5. (b) Subset of Ta 5d and Ni 3d orbital states which are relevant to the low-energy bands structure, following Ref. [16]. Note their opposite parities with respect to the mirror plane perpendicular to the chains (horizontal dashed line). (c) Schematic of expected low-energy band structure in the orthorhombic phase. (d), (e) ARPES measurements taken at T=350 K (above Tc), measured along the Γ-X direction using (d) LV and (e) LH polarized light. Note that at such elevated temperatures, the chemical potential may be significantly different from the T=0 charge neutrality point where the valence and conduction bands overlap. The photoemission geometry is represented in (b), where the crystallographic chains (a axis) are parallel to the analyzer entrance slit, while the scattering plane is coincident with the σ mirror plane. (f) Momentum distribution curves extracted from the region shown in (e), demonstrating an electronlike band dispersing upwards away from the intense “blob” of spectral weight at the conduction-band minimum.

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  • Figure 2
    Figure 2

    (a)–(c) Temperature-dependent ARPES data, measured along the Γ-X direction for temperatures of (a) 350 K, (b) 295 K, and (c) 113 K. (d), (f) “Curvature” analysis of (a) and (c), respectively. (e) Energy distribution curves (EDCs) of the data at kx = 0. All data obtained at hν = 24 eV, in LH polarization.

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  • Figure 3
    Figure 3

    (a) Projection of the 3D Brillouin zone in the kz,kx plane; the high-symmetry points are labeled (see also Fig. SM-1 in the SM). (b) Intensity map obtained for a constant energy of 0.15 eV, a little below the flattened hybridized state found at Γ, showing closed 2D contours. (c) Equivalent measurement at 0.42 eV below μ, also clearly showing features dispersing in both kz and kx directions. Dashed red lines are the Brillouin-zone boundaries. (d) Dispersion in the kz direction, obtained from the mapping data. (e)–(g) High-symmetry dispersions as indicated in (c). All data measured at hν=24 eV in LH polarization.

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  • Figure 4
    Figure 4

    (a), (b) Top view of the crystal structures in the orthorhombic and monoclinic phases. The white and green arrows in (b) represent the atomic displacements arising due to the shear distortion. This results in a loss of the σ and σ mirror symmetries for the low-temperature structure. (c), (d) Corresponding DFT calculations using the mBJ exchange potential in the orthorhombic and monoclinic phases. Blue, red, and green colors are used to represent where the maximum atomic character of the band is Ta, Ni, or Se, respectively. (e), (f) ARPES data in the orthorhombic and monoclinic phases, reproduced from Fig, 2, but now referenced to the valence-band maximum. In (e), the data are divided by the Fermi function to better highlight the spectral weight above EF. The optical gap of 0.16 eV [12] is shown in (f) for comparison.

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