We demonstrate, numerically, the possibility of manipulating the spin states of molecular nanomagnets with shaped microwave pulses designed with quantum optimal control theory techniques. The state-to-state or full gate transformations can be performed in this way in shorter times than using simple monochromatic resonant pulses. This enhancement in the operation rates can therefore mitigate the effect of decoherence. The optimization protocols and their potential for practical implementations are illustrated by simulations performed for a simple molecular cluster hosting a single ${\mathrm{Gd}}^{3+}$ ion. Its eight accessible levels (corresponding to a total spin $S=7/2$) allow encoding an eight-level qudit or a system of three coupled qubits. All necessary gates required for universal operation can be obtained with optimal pulses using the intrinsic couplings present in this system. The application of optimal control techniques can facilitate the implementation of quantum technologies based on molecular spin qudits.

• Received 2 December 2021
• Revised 31 March 2022
• Accepted 2 May 2022

DOI:https://doi.org/10.1103/PhysRevApplied.17.064028