Coherent ion dip spectroscopy (CIS) provides high sensitivity and high resolution for the investigation of vibrational overtones in molecular electronic ground states. For a special time sequence of two coherent narrow‐band Fourier transform limited nanosecond UV light pulses, with a modest delay of the pump pulse of 6.4 ns, a complete blocking of the population transfer to the upper state is achieved in the lambda‐type three‐level system ion dip experiment. This leads to ion dips with a depth as large as 95% and each dip represents an individual rovibronic transition. In this work, CIS is applied for the first time to a weakly bound van der Waals complex, benzene–Ar. We are able to observe six new van der Waals vibrational states up to an excess energy of 130 cm−1. The assignments are made by comparison with recent S1 excited state data of benzene–Ar and p‐difluorobenzene–Ar and by analysis of the positions and intensities of the observed individual rotational lines. The frequency positions of the intermolecular vibrational states display a regular pattern up to 130 cm−1.

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