A novel procedure is described for processing the second-order data matrices with multivariate curve resolution-alternating least-squares; while the data set is nontrilinear and severe profile overlapping occurs in the instrumental data modes. The area of feasible solutions can be reduced to a unique solution by including/considering the area correlation constraint, besides the traditional constraints (i.e., non-negativity, unimodality, species correspondence, etc.). The latter is implemented not only for the unknown samples but also for all calibration samples, regardless of their interferent content. The area of correlation constraint was specially designed to remove rotational ambiguity in the chemical data sets when information about calibration samples is at hand. In this contribution a comprehensive strategy is developed to uniquely unravel nontrilinear data sets or data sets with severely overlapped profiles in the instrumental data modes. The approach is illustrated with simulated and experimental data sets. Borgen plots are employed to adequately visualize the extent of rotational ambiguity under non-negativity constraint.