We study the generation of two-qudit entangling quantum logic gates using two techniques in quantum optimal control. We take advantage of both continuous, Lie-algebraic control and digital, Lie-group control. In both cases, the key is access to a time-dependent Hamiltonian which can generate an arbitrary unitary matrix in the group SU($d^2$). We find efficient protocols for creating high-fidelity entangling gates. As a test of our theory, we study the case of qudits robustly encoded in nuclear spins of alkaline earth atoms and manipulated with magnetic and optical fields, with entangling interactions arising from the well-known Rydberg blockade. We applied this in a case study based on a $d=10$ dimensional qudit encoded in the $I=9/2$ nuclear spin in $^{87}$Sr, controlled through a combination of nuclear spin-resonance, a tensor AC-Stark shift, and Rydberg dressing, which allows us to generate an arbitrary symmetric entangling two-qudit gate such as CPhase. Our techniques can be used to implement qudit entangling gates for any $2\le d \le10$ encoded in the nuclear spin. We also studied how decoherence due to the finite lifetime of the Rydberg states affects the creation of the CPhase gate and found, through numerical optimization, a fidelity of $0.9985$, $0.9980$, $0.9942$, and $0.9800$ for $d=2$, $d=3$, $d=5$, and $d=7$ respectively. This provides a powerful platform to explore the various applications of quantum information processing of qudits including metrological enhancement with qudits, quantum simulation, universal quantum computation, and quantum error correction.

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