Many-body description of two-dimensional van der Waals ferroelectric $\alpha -$In${}_2$Se${}_3$

Abstract

Two-dimensional (2D) van der Waals ferroelectrics are recognized for enabling many applications, from memory and logic to neuromorphic computing, as well as transforming other materials to control electronic phase transitions and topological states. While these materials are typically weakly correlated and expected to have their ground-state properties well described with the commonly used density functional theory, by focusing on bilayers and trilayers of In${}_2$Se${}_3$ we show that this approach may not be reliable. The underlying electronic structure strongly depends on the polarization structure of the multilayer system and is surprisingly challenging to accurately calculate, requiring a high-fidelity many-body theory of the quasiparticle self-consistent \textit{GW} approximation. We develop this underlying description by extending the capabilities of Green function implementation within the open-source Questaal package. We show that even a sophisticated hybrid functional approach may fail to predict a nonvanishing gap in a bilayer In${}_2$Se${}_3$ and yields charge density, polarization, and band offsets that strongly deviate from the many-body picture. We discuss the implications of these computational advances for future opportunities in 2D ferroelectrics.

arXiv comment17 pages, 7 figures, Invited article APL Comput. Phys. (in press)

References in corpus (46)

• The GW method
• Quasiparticle Self-Consistent GW Theory
• A Ferroelectric Semiconductor Field-Effect Transistor
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• Colloquium: Quantum anomalous Hall effect
• Quasiparticle self-consistent $GW$ method; a basis for the independent-particle approximation
• A polarity-induced defect mechanism for conductivity and magnetism at polar-nonpolar oxide interfaces
• Antiferroelectric Altermagnets: Antiferroelectricity Alters Magnets
• Ferroelectric switchable altermagnetism
• Adequacy of Approximations in GW Theory
• Questaal: a package of electronic structure methods based on the linear muffin-tin orbital technique
• Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons
• Thickness-dependent Dielectric Constant of Few-layer In2Se3 Nano-flakes
• Exciton-plasmon states in nanoscale materials: breakdown of the Tamm-Dancoff approximation
• Room-temperature ferroelectric switching of spin-to-charge conversion in GeTe
• Strong quantum confinement effect in the optical properties of ultrathin α-In2Se3
• Reversible spin texture in ferroelectric HfO2
• What Makes Effective Gating Possible in Two-Dimensional Heterostructures?
• Ferroelectric control of magnetic skyrmions in two-dimensional van der Waals heterostructures
• Two-Dimensional Ferroelectric Altermagnets: From Model to Material Realization
• Spin-Lasers: Spintronics Beyond Magnetoresistance
• Accurate optical properties from first principles: a Quasiparticle Self consistent GW plus Bethe-Salpeter Equation approach
• QS$G\hat{W}$: Quasiparticle Self consistent $GW$ with ladder diagrams in $W$
• Quantum Spin-Valley Hall Kink States: From Concept to Materials Design
• Magnetic Properties and Electronic Structure of Magnetic Topological Insulator MnBi${}_2$Se${}_4$
• First-Principles Description of Charge Transfer in Donor-Acceptor Compounds from Self-Consistent Many-Body Perturbation Theory
• Giant proximity exchange and valley splitting in transition metal dichalcogenide/$h\mathrm{BN}$/(Co, Ni) heterostructures
• Optically Probing Tunable Band Topology in Atomic Monolayers
• First principles vs second principles: Role of charge self-consistency in strongly correlated systems
• First-Principles Study of Two-Dimensional Ferroelectrics Using Self-Consistent Hubbard Parameters
• Justifying quasiparticle self-consistent schemes via gradient optimization in Luttinger-Ward theory
• A switchable two-dimensional electron gas based on ferroelectric Ca:SrTiO${}_3$
• Ferroelectricity-tuned band topology and superconductivity in two-dimensional materials and related heterostructures
• Excitonic signatures of ferroelectric order in parallel-stacked MoS${}_2$
• Emergent Multiferroic Altermagnets and Spin Control via Noncollinear Molecular Polarization
• Quantum Confinement and Electronic Structure at the Surface of van der Waals Ferroelectric α-In${}_2$Se${}_3$
• Altermagnetic Proximity Effect
• Unveiling multiferroic proximity effect in graphene
• Ferroelectric control of charge-to-spin conversion in WTe${}_2$
• Lattice fluctuations, not excitonic correlations, mediated electronic localization in TiSe${}_2$
• Opto-electronic properties of alpha-In2Se3: single-layer to bulk
• Multiferroic nematic d-wave altermagnetism driven by orbital-order on the honeycomb lattice
• Giant asymmetric proximity-induced spin-orbit coupling in twisted graphene/SnTe heterostructure
• Perpendicular magnetic anisotropy in bulk and thin-film CuMnAs for antiferromagnetic memory applications
• Movable Dirac Points with Ferroelectrics: Kink States and Berry Curvature Dipoles
• Ferroelectric switching control of spin current in graphene proximitized by In${}_2$Se${}_3$