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The tip-of-the-tongue (TOT) state is a spontaneously occurring metacognitive state that indicates that the answer to a query is almost, but not quite, at hand, i.e., that resolution is imminent. Since the time of William James, a distinctive feeling of nagging frustration has been observed to be associated with TOT states. On a more positive note, TOT states are also associated with intense goal-directed curiosity and with a strong desire to know that translates into successful mental action. The present study showed that prior to the presentation of resolving feedback to verbal queries—if the individual was in a TOT state—alpha suppression was in evidence in the EEG. This alpha suppression appears to be a marker of a spontaneously occurring, conscious, and highly motivating goal-directed internal metacognitive state. At the same time, alpha expression in the same time period was associated with the feeling of not knowing, indicating a more discursive state. Both alpha and alpha suppression were observed broadly across centro-parietal scalp electrodes and disappeared immediately upon presentation of the resolving feedback. Analyses indicated that the occurrence of alpha suppression was associated with participants’ verbal affirmations of being in a TOT state, which is also related to subsequent expression of a late positivity when feedback is provided, and to enhanced memory.