Surface atomic order of compound III-V semiconductor alloys at finite temperature

We investigate the role of alloying, atomic-size mismatch strain, and thermal effects on ordering and reconstruction stability of As-rich (2×4) surfaces on (In_xGa_1−x)As (001) ternary III-V alloys (in the dilute limit) using a first-principles cluster-expansion and Monte Carlo simulations. The cluster expansion accounts for configurational degrees of freedom associated with As dimer adsorption/desorption as well as Ga-In disorder in subsurface cation sites. We analyze the α2(2×4)-β2(2×4) transition at finite temperature and directly examine the entropy and cation-site filling in both reconstructions. A compositionally dependent “zigzag” ordering of dimers in the α2(2×4) is predicted as well as a hybrid α2(2×4)-β2(2×4) reconstruction, found to be stable in a reasonably large chemical-potential range. The hybrid dimer ordering drives pronounced nanoscale composition modulation of surface cations.