Excitation-density and excess-energy dependence of ultrafast dynamics of photoexcited carriers in intrinsic bulk CdTe

In this study, ultrafast dynamics of photoexcited carriers in an intrinsic CdTe film are investigated deeply and systematically as a function of carrier density and excess energy using femtosecond-resolved pump-probe transient differential transmission spectroscopy. A dynamic model is developed based on an interband transition absorption model in direct bandgap semiconductors by introducing the dynamics of thermalization, cooling and recombination of photoexcited carriers into the interband transition absorption model. Then, the model is used to best fit the measured ultrafast dynamics to retrieve the initial temperature of thermalized electrons and time constants of the thermalization, cooling and recombination dynamic processes as a function of carrier density and excess energy. The increase with carrier density and the decrease with excess energy of thermalization time constant reveal that thermalization process of photoexcited carriers is dominated by carrier-phonon scatterings. We find for the first time that cooling of thermalized carriers depend strongly on carrier density and excess energy, and cooling time constant varies in a wide range from 0.2 to 5 ps. It is also found that carrier recombination in the intrinsic CdTe film is dominated by the radiative recombination of electron-hole pairs, rather than Auger recombination as reported in doped CdTe films. These new results are very important to understanding of microscopic mechanism of relaxation processes of photoexcited carriers and applications of CdTe-based optoelectronic devices.

Automated summary

This study examined the ultrafast dynamics of photoexcited carriers in an intrinsic CdTe film using femtosecond-resolved pump-probe transient differential transmission spectroscopy. A dynamic model was developed to analyze the thermalization, cooling, and recombination processes of the photoexcited carriers. The results showed that carrier thermalization time increased with carrier density and decreased with excess energy, while carrier cooling strongly depended on carrier density and excess energy, with cooling time varying from 0.2 to 5 ps. Furthermore, carrier recombination in the intrinsic CdTe film was dominated by radiative recombination of electron-hole pairs.