Lattice Anisotropy-Driven Reduction of Phonon Velocities in Black Phosphorus

Abstract

Phonon dynamics and transport determine how heat is utilized and dissipated in materials. In 2D systems for optoelectronics and thermoelectrics, the impact of nanoscale material structure on phonon propagation is central to controlling thermal conduction. Here, we directly observe in-plane coherent acoustic phonon propagation in black phosphorus (BP) using ultrafast electron microscopy. We identify a significant reduction of the group velocities in directions intermediate to the armchair and zigzag lattice directions. Using a machine learning-based model with an >8000 atom supercell, we find that this slowing results from the mixing of in-plane transverse and longitudinal acoustic phonons and is independent of broken symmetries of edge reconstructions. This work demonstrates how coherent phonon transport is sensitive to propagation direction in the lattice plane.

Keywords: black phosphorus; lattice anisotropy; phonon transport; thermoelectrics; ultrafast electron microscopy.