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Optimal Control Theory is a powerful mathematical tool, which has known a rapid development since the 1950s, mainly for engineering applications. More recently, it has become a widely used method to improve process performance in quantum technologies by means of highly efficient control of quantum dynamics. This tutorial aims at providing an introduction to key concepts of optimal control theory which is accessible to physicists and engineers working in quantum control or in related fields. The different mathematical results are introduced intuitively, before being rigorously stated. This tutorial describes modern aspects of optimal control theory, with a particular focus on the Pontryagin Maximum Principle, which is the main tool for determining open-loop control laws without experimental feedback. The different steps to solve an optimal control problem are discussed, before moving on to more advanced topics such as the existence of optimal solutions or the definition of the different types of extremals, namely normal, abnormal, and singular. The tutorial covers various quantum control issues and describes their mathematical formulation suitable for optimal control. The connection between the Pontryagin Maximum Principle and gradient-based optimization algorithms used for high-dimensional quantum systems is described. The optimal solution of different low-dimensional quantum systems is presented in detail, illustrating how the mathematical tools are applied in a practical way.