Influence of Discrete Defects on Observed Acoustic-Phonon Dynamics in Layered Materials Probed with Ultrafast...

The structural anisotropy of layered materials leads to disparate lattice responses along different crystallographic directions following femtosecond photoexcitation. Ultrafast scattering methods are well-suited to resolving such responses, though probe size and specimen structure and morphology must be considered when interpreting results. Here we use ultrafast electron microscopy (UEM) imaging and diffraction to study the influence of individual multilayer terraces and few-layer step-edges on acoustic-phonon dynamics in 1T-TaS₂ and 2H-MoS₂. In TaS₂, we find that a multilayer terrace produces distinct, localized responses arising from thickness-dependent c-axis phonon dynamics. Convolution of the responses is demonstrated with ultrafast selected-area diffraction by limiting the probe size and training it on the region of interest. This results in a reciprocal-space frequency response that is a convolution of the spatially separated behaviors. Sensitivity of phonon dynamics to few-layer step-edges in MoS₂ and the capability of UEM imaging to resolve the influence of such defects are also demonstrated. Spatial frequency maps from the UEM image series reveal regions separated by a four-layer step-edge having 60.0 GHz and 63.3 GHz oscillation frequencies, again linked to c-axis phonon propagation. As with ultrafast diffraction, signal convolution is demonstrated by continuous increase of the size of the selected region of interest used in the analysis.