Quantum control in large dimensional Hilbert spaces is essential for realizing the power of quantum information processing. For closed quantum systems the relevant input/output maps are unitary transformations, and the fundamental challenge becomes how to implement these with high fidelity in the presence of experimental imperfections and decoherence. For two-level systems (qubits) most aspects of unitary control are well understood, but for systems with Hilbert space dimension d>2 (qudits), many questions remain regarding the optimal design of control Hamiltonians and the feasibility of robust implementation. Here we show that arbitrary, randomly chosen unitary transformations can be efficiently designed and implemented in a large dimensional Hilbert space (d=16) associated with the electronic ground state of atomic 133Cs, achieving fidelities above 0.98 as measured by randomized benchmarking. Generalizing the concepts of inhomogeneous control and dynamical decoupling to d>2 systems, we further demonstrate that these qudit unitary maps can be made robust to both static and dynamic perturbations. Potential applications include improved fault-tolerance in universal quantum computation, nonclassical state preparation for high-precision metrology, implementation of quantum simulations, and the study of fundamental physics related to open quantum systems and quantum chaos.
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