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Ultrafast screening and carrier dynamics in ZnO: Theory and experiment

At carrier densities above the Mott density Coulomb screening destroys the exciton resonance. This, together with band-gap renormalization and band filling, severely affects the optical spectra. We have experimentally studied these effects by ultrafast pump-probe reflectivity measurements on a ZnO single crystal at various wavelengths around the exciton resonance and in a broad carrier-density range. Theoretically we determined the Mott density in ZnO to be $1.5\times10^{24}$ m$^{-3}$ at 300 K. Taking a field-theoretical approach, we derived and solved the Bethe-Salpeter ladder equation and we computed the density-dependent reflectivity and absorption spectra. A carrier dynamics model has been developed, containing three-photon absorption, carrier cooling, and carrier trapping near the surface. The agreement between the theoretical reflectivity based on our model and the experimental data is excellent.