We report on the implementation of a quantum process tomography technique known as direct characterization of quantum dynamics applied on coherent and incoherent single-qubit processes in a system of trapped (40)Ca(+) ions. Using quantum correlations with an ancilla qubit, direct characterization of quantum dynamics reduces substantially the number of experimental configurations required for a full quantum process tomography and all diagonal elements of the process matrix can be estimated with a single setting. With this technique, the system's relaxation times T(1) and T(2) were measured with a single experimental configuration. We further show the first, complete characterization of single-qubit processes using a single generalized measurement realized through multibody correlations with three ancilla qubits.