Real-time dynamics of the two-step charge-density-wave transition in bulk 1T-TaS$_2$

Abstract

The charge-density wave (CDW) of bulk 1T-TaS2 is built from Star-of-David (SoD) clusters tiling a sqrt{13} x sqrt{13} superlattice, and it melts through a two-step sequence accompanied by order-of-magnitude changes in resistivity. Whether these steps proceed by collapse of the SoD amplitude or by rearrangement of the SoD lattice has remained unresolved, because the relevant dynamics occur on length and time scales beyond the reach of ab initio molecular dynamics. Here we follow the CDW transitions in real time using a machine-learning force field trained on first-principles data, giving access to 1404-atom supercells over 5 ns. The two steps are mechanistically distinct. Above 200 K, SoD clusters translate coherently by transiently dissolving and re-forming about shifted centers, a deformation-formation process that preserves the local SoD amplitude while randomizing the interlayer stacking order and nucleating domain walls. Only near 350 K does the SoD distortion itself collapse. These results provide microscopic support for the recently proposed two-step model of the CDW transition and offer a framework for interpreting light-induced hidden phases and cavity-modified transition temperatures in 1T-TaS2.