A robust control over quantum dynamics is of paramount importance for quantum technologies. Many of the existing control techniques are based on smooth Hamiltonian modulations involving repeated calculations of basic unitaries resulting in time complexities scaling rapidly with the length of the control sequence. Here we show that bang-bang controls need one-time calculation of basic unitaries and hence scale much more efficiently. By employing a global optimization routine such as the genetic algorithm, it is possible to synthesize not only highly intricate unitaries, but also certain nonunitary operations. We demonstrate the unitary control through the implementation of the optimal fixed-point quantum search algorithm in a three-qubit nuclear magnetic resonance (NMR) system. Moreover, by combining the bang-bang pulses with the crusher gradients, we also demonstrate nonunitary transformations of thermal equilibrium states into effective pure states in three-as well as five-qubit NMR systems.
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