Anomalous temperature dependence of optical and acoustic phonons in Bi$_2$Se$_3$ arising from stacking faults

TL;DR

This study investigates the unusual temperature dependence of optical and acoustic phonons in Bi2Se3, attributing anomalies to stacking faults confirmed by first-principles calculations, with implications for understanding layered topological insulators.

Contribution

It provides experimental and theoretical evidence linking stacking faults to anomalous phonon behavior in Bi2Se3, highlighting the role of spin-orbit coupling in fault formation.

Findings

Anomalous phonon behavior around 180 K observed.

Stacking faults are identified as the cause of anomalies.

Spin-orbit coupling influences fault energetics.

Abstract

The class of layered 3D-topological insulators have shown intriguingly anomalous temperature dependence in their thermal expansion coefficients. It was proposed that stacking faults are the origin of the observed anomalous thermal expansion. Here, using femtosecond pump-probe differential reflectivity measurements we probe the carrier and coherently generated totally symmetric A1g1 optical phonons in Bi2Se3. Transient signals also show a low frequency (~GHz) oscillations due to coherent longitudinal acoustic phonons. We extract temperature dependence of optical constants, sound velocity and Young's modulus of Bi2Se3 using the strain pulse propagation model. A remarkable anomalous behavior around ~180 K is observed in the temperature dependence of optical and acoustic phonons as well as the optical constants. First-principles density functional theory (DFT) reveals that thermally activated formation of stacking faults is responsible for the anomalies observed in Bi2Se3, similar to case of Sb2Te3. We also show that inclusion of spin-orbit coupling plays an important role in reducing the total energy difference between the pristine and the faulted structures.