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We report correlative crystallographic and morphological studies of defect-dependent phonon dynamics in single flakes of 1T-TaS2 and 2H-WSe2 using selected-area diffraction and bright-field imaging in an ultrafast electron microscope. In both materials, we observe in-plane speed-of-sound acoustic-phonon wave trains, the dynamics of which (i.e., emergence, propagation, and interference) are strongly dependent upon discrete interfacial features (e.g., vacuum/crystal and crystal/crystal interfaces). In TaS2, we observe cross-propagating in-plane acoustic-phonon wave trains of differing frequencies that undergo coherent interference approximately 200 ps after initial emergence from distinct interfacial regions. With ultrafast bright-field imaging, the properties of the interfering wave trains are observed to correspond to the beat frequency of the individual oscillations, while intensity oscillations of Bragg spots generated from selected areas within the region of interest match well with the real-space dynamics. In WSe2, distinct acoustic-phonon dynamics are observed emanating and propagating away from structurally dissimilar morphological discontinuities (vacuum/crystal interface and crystal terrace), and results of ultrafast selected-area diffraction reveal thickness-dependent phonon frequencies. The overall observed dynamics are well-described using finite element analysis and time-dependent linear-elastic continuum mechanics.
Bibliographical noteFunding Information:
This work was supported primarily by the National Science Foundation through the University of Minnesota MRSEC under Award No. DMR-1420013 and in part by the Arnold and Mabel Beckman Foundation through a 2015 Beckman Young Investigator Award. Both D.R.C. and D.A.P. acknowledge support in the form of a Doctoral Dissertation Fellowship received from the Graduate School at the University of Minnesota. We thank Spencer Reisbick for helpful discussions regarding TaS2.
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PubMed: MeSH publication types
- Journal Article