Transient hot electron dynamics in single-layer TaS2

Abstract

Using time- and angle-resolved photoemission spectroscopy, we study the response of metallic single layer TaS2 in the 1H structural modification to the generation of excited carriers by a femtosecond laser pulse. A complex interplay of band structure modifications and electronic temperature increase is observed and analyzed by direct fits of model spectral functions to the two-dimensional (energy and k-dependent) photoemission data. Upon excitation, the partially occupied valence band is found to shift to higher binding energies by up to ≈ 100 meV, accompanied by electronic temperatures exceeding 3000~K. These observations are explained by a combination of temperature-induced shifts of the chemical potential, as well as temperature-induced changes in static screening. Both contributions are evaluated in a semi-empirical tight-binding model. The shift resulting from a change in the chemical potential is found to be dominant.