Anisotropic Ordering in 1T′ Molybdenum and Tungsten Ditelluride Layers Alloyed with Sulfur and Selenium

Alloying is an effective way to engineer the band-gap structure of two-dimensional transition-metal dichalcogenide materials. Molybdenum and tungsten ditelluride alloyed with sulfur or selenium layers (MX_2<i>x</i>Te_{2(1–<i>x</i>)}, M = Mo, W and X = S, Se) have a large band-gap tunability from metallic to semiconducting due to the 2H-to-1T′ phase transition as controlled by the alloy concentrations, whereas the alloy atom distribution in these two phases remains elusive. Here, combining atomic resolution <i>Z</i>-contrast scanning transmission electron microscopy imaging and density functional theory (DFT), we discovered that anisotropic ordering occurs in the 1T′ phase, in sharp contrast to the isotropic alloy behavior in the 2H phase under similar alloy concentration. The anisotropic ordering is presumably due to the anisotropic bonding in the 1T′ phase, as further elaborated by DFT calculations. Our results reveal the atomic anisotropic alloyed behavior in 1T′ phase layered alloys regardless of their alloy concentration, shining light on fine-tuning their physical properties <i>via</i> engineering the alloyed atomic structure