Large-amplitude chirped coherent phonons in tellurium mediated by ultrafast photoexcited carrier diffusion

Abstract

We report femtosecond time-resolved reflectivity measurements of coherent phonons in tellurium performed over a wide range of temperatures (3K to 296K) and pump laser intensities. A totally symmetric A$_{1}$ coherent phonon at 3.6 THz responsible for the oscillations in the reflectivity data is observed to be strongly positively chirped (i.e, phonon time period decreases at longer pump-probe delay times) with increasing photoexcited carrier density, more so at lower temperatures. We show for the first time that the temperature dependence of the coherent phonon frequency is anomalous (i.e, increasing with increasing temperature) at high photoexcited carrier density due to electron-phonon interaction. At the highest photoexcited carrier density of $\sim$ 1.4 $\times$ 10$^{21}$cm$^{-3}$ and the sample temperature of 3K, the lattice displacement of the coherent phonon mode is estimated to be as high as $\sim$ 0.24 \AA. Numerical simulations based on coupled effects of optical absorption and carrier diffusion reveal that the diffusion of carriers dominates the non-oscillatory electronic part of the time-resolved reflectivity. Finally, using the pump-probe experiments at low carrier density of 6 $\times$ 10$^{18}$ cm$^{-3}$, we separate the phonon anharmonicity to obtain the electron-phonon coupling contribution to the phonon frequency and linewidth.Comment: 22 pages, 6 figures, submitted to PR