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We demonstrate optical control of the LO phonon-plasmon coupled (LOPC) modes in GaAs by using a femtosecond pump-pulse pair. The relaxation time of the plasmon-like LOPC mode significantly depends on the separation time (\Delta t) of the pump-pulse pair. Especially it is maximized when \Delta t becomes simultaneously comparable to the half period of the longitudinal optical (LO) phonon oscillation and resonant to the 3/4 period of the plasmon-like LOPC oscillation. We attribute these observations to the modification of carrier-LO phonon scattering and ballistic motion of the plasmon-like LOPC mode.

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