High spin magnetic molecules are promising candidates for quantum information processing because they intrinsically have multiple sublevels for information storage and computational operations. However, due to their susceptibility to the environment and limitation from the selection rule, the arbitrary control of the quantum state of a multilevel system on a molecular and electron spin basis has not been realized. Here we exploit the photoexcited triplet of C70 as a molecular electron spin qutrit. After the system was initialized by photoexcitation, we prepared it into representative three-level superposition states characteristic of the qutrit, measured their density matrices, and showed the interference of the quantum phases in the superposition. The interference pattern is further interpreted as a map of evolution through time under different conditions.
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