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Control structures and strategies have a critical influence on a power electronic converter’s behavior during disturbances. Most of the previous works in the field of pulsewidth modulation voltage-source converter (VSC) operation under unbalanced conditions propose dual vector controllers with dc bus voltage optimization strategies, which have been proven to be well adapted for rectifier applications. In this paper, two major contributions are made. On the one hand, a new optimized operation strategy based on exchanged power maximization is proposed for vector control structures, which permits the extension of optimized operation to other VSC applications (e.g., flexible alternating current transmission system and distributed generation interfaces). On the other hand, a scalar control structure is proposed based on resonant controllers, together with three adapted optimized operation strategies, namely: 1) dc bus voltage optimization; 2) power exchange maximization; and 3) a hybrid strategy (an intermediary mode between the other two strategies). Their main advantage is their simplicity and the lack of real-time symmetrical component extraction techniques. This scalar controller and the proposed optimized operation strategies are compared to conventional vector controllers. It is proven through experimental analysis that the proposed scalar controller offers very good performances with simpler structures and bigger flexibility in terms of operation modes.