Dynamically coupled plasmon-phonon modes in GaP: An indirect-gap polar semiconductor

Abstract

The ultrafast coupling dynamics of coherent optical phonons and the photoexcited electron-hole plasma in the indirect gap semiconductor GaP are investigated by experiment and theory. For below-gap excitation and probing by 800-nm light, only the bare longitudinal optical (LO) phonons are observed. For above-gap excitation with 400-nm light, the photoexcitation creates a high density, nonequilibrium $e\text{\ensuremath{-}}h$ plasma, which introduces an additional, faster decaying oscillation due to an LO phonon-plasmon coupled (LOPC) mode. The LOPC mode frequency exhibits very similar behavior for both $n$- and $p$-doped GaP, downshifting from the LO to the transverse optical (TO) phonon frequency limits with increasing photoexcited carrier density. We assign the LOPC mode to the LO phonons coupled with the photoexcited multicomponent plasma. For the 400-nm excitation, the majority of the photoexcited electrons are scattered from the $\mathrm{\ensuremath{\Gamma}}$ valley into the satellite $X$ valley, while the light and spin-split holes are scattered into the heavy hole band, within 30 fs. The resulting mixed plasma is strongly damped, leading to the LOPC frequency appearing in the reststrahlen gap. Due to the large effective masses of the $X$ electrons and heavy holes, the coupled mode appears most distinctly at carrier densities $\ensuremath{\gtrsim}5\ifmmode\times\else\texttimes\fi{}{10}^{18}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$. We perform theoretical calculations of the nuclear motions and the electronic polarizations following an excitation with an ultrashort optical pulse to obtain the transient reflectivity responses of the coupled modes. We find that, while the longitudinal diffusion of photoexcited carriers is insignificant, the lateral inhomogeneity of the photoexcited carriers due to the laser intensity profile should be taken into account to reproduce the major features of the observed coupled mode dynamics.