Critical behavior of the dimerized Si(001) surface: Continuous order-disorder phase transition in the two-dimensional Ising universality class

The critical behavior of the order-disorder phase transition in the buckled dimer structure of the Si(001) surface is investigated both theoretically by means of first-principles calculations and experimentally by spot profile analysis low-energy electron diffraction (SPA-LEED). We use density functional theory (DFT) with three different functionals commonly used for Si to determine the coupling constants of an effective lattice Hamiltonian describing the dimer interactions. Experimentally, the phase transition from the low-temperature $c(4\times 2)$- to the high-temperature $p(2\times 1)$-reconstructed surface is followed through the intensity and width of the superstructure spots within the temperature range $78–400K$. Near the critical temperature $T_c=190.6K$, we observe universal critical behavior of spot intensities and correlation lengths, which falls into the universality class of the two-dimensional (2D) Ising model. From the ratio of correlation lengths along and across the dimer rows we determine effective nearest-neighbor couplings of an anisotropic 2D Ising model, $J_{\parallel }=(-24.9\pm 0.9_{\mathrm{stat}}\pm 1.3_{\mathrm{sys}})\mathrm{meV}$ and $J_{\perp }=(-0.8\pm 0.1_{\mathrm{stat}})\mathrm{meV}$. We find that the experimentally determined coupling constants of the Ising model can be reconciled with those of the more complex lattice Hamiltonian from DFT when the critical behavior is of primary interest. The anisotropy of the interactions derived from the experimental data via the 2D Ising model is best matched by DFT calculations using the PBEsol functional. The trends in the calculated anisotropy are consistent with the surface stress anisotropy predicted by the DFT functionals, pointing towards the role of surface stress reduction as a driving force for establishing the $c(4\times 2)$-reconstructed ground state.