Coherently Coupled Carrier and Phonon Dynamics in Elemental Tellurium Probed by XUV Transient Absorption

TL;DR

This study uses broadband XUV transient absorption to reveal the coherent coupling between carriers and phonons in elemental tellurium, showing how ultrafast excitation influences its electronic and lattice dynamics with potential for optical control.

Contribution

It demonstrates the simultaneous measurement of coupled carrier and phonon dynamics in tellurium, revealing phase relationships and long-lived excited states not previously observed.

Findings

Coherent coupling between hot carriers and phonons in tellurium.

Observation of a long-lived shift in the absorption edge.

Phonon-induced oscillations suggest increased metallicity.

Abstract

The narrow bandgap semiconductor elemental tellurium (Te) has a unique electronic structure due to strong spin-orbit splitting and a lack of inversion symmetry of it's helical lattice. Using broadband extreme ultraviolet core-level transient absorption, we measure simultaneously the coherently coupled photo-induced carrier and lattice dynamics at the Te N$_{4,5}$ edge initiated by a few-cycle NIR pulse. Ultrafast excitation of carriers leads to a coherently excited A$_{\rm{1}}$ phonon oscillation and the generation of a hot carrier population distribution that oscillates in temperature, and the phonon excursion and hot carrier temperature are $\pi$ out of phase with respect to each other. The depths of modulation suggest a significant coupling between the electronic and lattice degrees of freedom in Te. A long-lived shift of the absorption edge suggests an excited state of Te in a new equilibrium potential energy surface that lives on the order of the carrier recombination timescale. The observed phonon-induced oscillations of the hot carriers are supportive of a change in the metallicity, whereby Te becomes more metallic with increasing phonon-induced displacement. Additionally, near the Fermi level we observe an energy-dependent phase of the displacive excitation of the A$_{\rm{1}}$ phonon mode. The discovery of coherent coupling between the lattice and hot carriers in Te provides the basis to investigate coherent interactions between spin and orbital degrees of freedom. The results spectrally and temporally resolve the correlation between photo-excited hot carriers and coherent lattice excitations, providing insight on the optical manipulation of the Te electronic structure at high carrier densities exceeding $10^{21}\,\mathrm{cm}^{-3}$.