Ultrafast dynamics of hot charge carriers in an oxide semiconductor probed by femtosecond spectroscopic ellipsometry

Steffen Richter, Oliver Herrfurth, Shirly Espinoza, Mateusz Rebarz, Miroslav Kloz, Joshua A. Leveillee, André Schleife, Stefan Zollner, Marius Grundmann, Jakob Andreasson, Rüdiger Schmidt-Grund

Research output: Contribution to journalArticlepeer-review

Abstract

Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorption partially blocked and screened by the photo-excited electron occupation of the conduction band and hole occupation of the valence band (absorption bleaching). Exciton absorption turns spectrally narrower upon pumping and sustains the Mott transition, indicating Mahan excitons. Simultaneously, intra-valence-band transitions occur at sub-picosecond time scales after holes scatter to the edge of the Brillouin zone. Our results pave new ways for the understanding of non-equilibrium charge-carrier dynamics in materials by reliably distinguishing between changes in absorption coefficient and refractive index, thereby separating competing processes. This information will help to overcome the limitations of materials for high-power optical devices that owe their properties from dynamics in the ultrafast regime.

Original languageEnglish (US)
Article number083066
JournalNew Journal of Physics
Volume22
Issue number8
DOIs
StatePublished - Aug 2020

Keywords

  • Mahan exciton
  • ZnO
  • ellipsometry
  • exciton-phonon interaction
  • high excitation
  • transient spectroscopy

ASJC Scopus subject areas

  • Physics and Astronomy(all)

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