In a dynamic environment, we seek to enhance behavioral responses by anticipating future events. Previous studies have shown that the probability distribution of the timing of future events could shape our expectation of event timing; furthermore, the modulation of alpha oscillation is known to be a critical neural factor. However, a link between the modulation of alpha oscillation by temporal expectation and single neural activity is missing. In this study, we investigated how temporal expectation modulated frontal neural activities and behavioral reaction time by recording neural activity from the frontal eye field smooth pursuit eye movement region of monkeys while they performed a smooth pursuit eye movement task. We found that the temporal expectation reduced the coherence between the neural spiking and alpha frequency of the local field potential, along with the trial-by-trial correlation between the neural spiking activity and pursuit latency. This result suggests that the desynchronization of alpha oscillation by temporal expectation would be related to the decorrelation of population neural activity, which could be the neural source of reaction time enhancement by temporal expectation.