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Emergence of polar monoclinic phase in heterohalogen substituted CsGeX$_3$

Sourabh Vairat, Balachandra G. Hegde, Brajesh Tiwari, Ravi Kashikar

Abstract

The occurrence of ferroelectricity in inorganic germanium-based halide perovskites has provided an alternative to oxide counterparts. Using first-principles methods, we have studied CsGeX$_3$ materials with heterohalogen substitution at the X site in a 2:1 configuration. Structurally, such variation alters the octahedral environment more strongly than in pristine materials, giving rise to a polar monoclinic phase at room temperature. The occurrence of the monoclinic phase is also confirmed through the energetics of structures generated by the displacements of atoms in accordance with soft mode eigenvectors of the dynamical matrix along various directions. In the chemically tuned phase, the polarization is along [101] and increases by 10-15\% compared to pristine ones. The electronic structure analysis reveals that spin-splitting energy ranges from 25 to 250 meV in the valence band and from 9 to 80 meV in the conduction band in chemically tuned structures. In addition, these structures exhibit Rashba and persistent spin textures, which are coupled to the polarization direction. The parameters of the symmetry-dependent \textbf{k.p } Hamiltonian provide insights into the strength of spin-splitting and the nature of spin-texture. The semiconducting and spin-polarized nature of CsGeX$_3$ materials makes them strong candidates for Datta-Das spin transistors.

Emergence of polar monoclinic phase in heterohalogen substituted CsGeX$_3$

Abstract

The occurrence of ferroelectricity in inorganic germanium-based halide perovskites has provided an alternative to oxide counterparts. Using first-principles methods, we have studied CsGeX materials with heterohalogen substitution at the X site in a 2:1 configuration. Structurally, such variation alters the octahedral environment more strongly than in pristine materials, giving rise to a polar monoclinic phase at room temperature. The occurrence of the monoclinic phase is also confirmed through the energetics of structures generated by the displacements of atoms in accordance with soft mode eigenvectors of the dynamical matrix along various directions. In the chemically tuned phase, the polarization is along [101] and increases by 10-15\% compared to pristine ones. The electronic structure analysis reveals that spin-splitting energy ranges from 25 to 250 meV in the valence band and from 9 to 80 meV in the conduction band in chemically tuned structures. In addition, these structures exhibit Rashba and persistent spin textures, which are coupled to the polarization direction. The parameters of the symmetry-dependent \textbf{k.p } Hamiltonian provide insights into the strength of spin-splitting and the nature of spin-texture. The semiconducting and spin-polarized nature of CsGeX materials makes them strong candidates for Datta-Das spin transistors.
Paper Structure (6 sections, 2 equations, 9 figures, 5 tables)

This paper contains 6 sections, 2 equations, 9 figures, 5 tables.

Table of Contents

  1. Introduction
  2. Computational Details
  3. Results and discussion
  4. Structure and phase transition
  5. Electronic properties
  6. Conclusions

Figures (9)

  • Figure 1: (a)-(b) Structure of CsGeBr$_3$ in paraelectric (Pm$\bar{3}$m) and ferroelectric (R3m) phases. (c)-(d) Chemically tuned structures of CsGeBrI$_2$ in paraelectric (P4/mmm) and ferroelectric (Cm) phases.
  • Figure 2: (a)-(c) Phonon spectrum for centrosymmetric Pm$\bar{3}$m-CsGeBr$_3$, P4/mmm-CsGeBr$_2$I and CsGeBrI$_2$. (d)-(e) Energy variation along distortion for [001], [110], and [111] displacements for non-polar P4/mmm-CsGeBr$_2$I and CsGeBrI$_2$. (f) Amplitude of structural distortions in different modes for pristine and chemically tuned compounds.
  • Figure 3: a) Relative Phase Energy for pristine and various chemical compositions. (b) Spontaneous polarization of pristine and various chemical compositions for R3m and Cm phases, respectively.
  • Figure 4: a) Orbital resolved electronic bands structure for chemically tuned structures of CsGeBrI$_2$ in paraelectric (P4/mmm), b) and ferroelectric (Cm) phase.
  • Figure 5: (a)-(b) Spin splitting energy along high symmetry path in the Brillouin zone for conduction band and valence band for all chemically tuned structures. (c)-(d) Anisotropic spin splitting energy for various chemically tuned structures in the conduction and valence bands, respectively.
  • ...and 4 more figures