Temporally delayed, phase-locked coherent pairs of near IR femtosecond laser pulses were employed to study electronic coherences in molecular Nd 3 + -complexes at room temperature. Dissolved and solid complexes were studied under a confocal microscope set-up with fluorescence detection. The observed electronic coherence on a few hundred femtoseconds time scale is modulated by additional coherent wave packet dynamics, which we attribute mainly to be vibrational in nature. In future, the complexes may serve as prototypes for possible applications in quantum information technology.

The Cover Feature illustrates the creation and probing of a long‐lived electronic coherence in molecular Nd‐complexes by IR femtosecond laser pulses. The electronic coherence is observed via the Δτ‐dependent modulation of the fluorescence signal and shows the influence of additional vibrational dynamics. The Nd‐complexes may serve as prototypes for possible future applications in quantum information technology. More information can be found in the Research Article by Hendrike Braun and co‐workers.