2D materials, such as transition metal dichalcogenides (TMDs), graphene, and boron nitride, are seen as promising materials for future high power/high frequency electronics. However, the large difference in the thermal expansion coefficient (TEC) between many of these 2D materials could impose a serious challenge for the design of monolayer‐material‐based nanodevices. To address this challenge, alloy engineering of TMDs is used to tailor their TECs. Here, in situ heating experiments in a scanning transmission electron microscope are combined with electron energy‐loss spectroscopy and first‐principles modeling of monolayer Mo1−
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Abstract x Wx S2with different alloying concentrations to determine the TEC. Significant changes in the TEC are seen as a function of chemical composition in Mo1−x Wx S2, with the smallest TEC being reported for a configuration with the highest entropy. This study provides key insights into understanding the nanoscale phenomena that control TEC values of 2D materials.
