Ground State Instability in Spin Polarization for Electrons Confined in Two-Dimensional Square Quantum Dots

Abstract

We present a theoretical study of the ground state electronic structure and the spin polarization for four electrons confined in two-dimensional (2D) square quantum dots (SQDs). We employ standard mean field theory (MFT) approaches using the unrestricted Hartree–Fock (UHF) and density functional theory calculations. The resonant UHF configuration interaction (res-UHF CI) calculation was also performed in order to incorporate the electron correlation more intuitively. The MFT ground state is expected to be spin-polarized when SQDs have a small confinement length L or aspect ratio δ= Lx/Ly = 1, in agreement with Hund's rule. In contrast, the spin-unpolarized ground state singlet is expected in all in other SQDs. Thus, the MFT calculations produce the anti-Hund state, where the spin-density wave forms having the zero of the total spin, even though the SQD has the point group symmetry D4h. However, the res-UHF CI calculation restores the geometrical symmetry in the resulting ground state when the Coulomb interaction is strengthened. Nevertheless, the res-UHF CI ground state maintains the zero total spin. Thus, ground state instability is expected in the spin-polarization of the SQD system, which eventually violates Hund's rule in accordance with the Coulomb interaction.