A method for estimating quantitative parameters of a subject using a magnetic resonance imaging system comprising a programmed computer system, the steps of the method comprising: (a) providing MR data acquired with the MRI system to the programmed computer system, the provided MR data representing a plurality of different signal evolutions acquired using different acquisition parameter settings by performing a magnetic resonance fingerprinting data acquisition; (b) generating, using the programmed computer system, an initial dictionary comprising a plurality of signal templates that are generated based on coarsely sampling the acquisition parameter settings used when acquiring the provided MR data; (c) using the programmed computer system to compare the provided MR data with the initial dictionary and: (i) to store the quantitative parameters associated with an entry in the initial dictionary as the estimated quantitative parameters when the comparison satisfies a threshold criterion; (ii) to update the initial dictionary when the comparison does not satisfy the threshold criterion, wherein updating the initial dictionary includes performing a global optimization that searches a parameter space encompassing potential quantitative parameters, identifying the potential quantitative parameters that satisfy the threshold criterion, and adding the potential quantitative parameters that satisfy the threshold criterion to the initial dictionary to generate an updated dictionary, and wherein step (c) is repeated using the updated dictionary; and wherein the global optimization is initiated by identifying a seed entry based on the comparison performed in step (c), and wherein the seed entry is identified as an entry in the initial dictionary that when compared to the provided MR data yields a similarity value closest to the threshold criterion. (a) providing MR data acquired with the MRI system to the programmed computer system, the provided MR data representing a plurality of different signal evolutions acquired using different acquisition parameter settings by performing a magnetic resonance fingerprinting data acquisition; (b) generating, using the programmed computer system, an initial dictionary comprising a plurality of signal templates that are generated based on coarsely sampling the acquisition parameter settings used when acquiring the provided MR data; (c) using the programmed computer system to compare the provided MR data with the initial dictionary and: (i) to store the quantitative parameters associated with an entry in the initial dictionary as the estimated quantitative parameters when the comparison satisfies a threshold criterion; (ii) to update the initial dictionary when the comparison does not satisfy the threshold criterion, wherein updating the initial dictionary includes performing a global optimization that searches a parameter space encompassing potential quantitative parameters, identifying the potential quantitative parameters that satisfy the threshold criterion, and adding the potential quantitative parameters that satisfy the threshold criterion to the initial dictionary to generate an updated dictionary, and wherein step (c) is repeated using the updated dictionary; and (i) to store the quantitative parameters associated with an entry in the initial dictionary as the estimated quantitative parameters when the comparison satisfies a threshold criterion; (ii) to update the initial dictionary when the comparison does not satisfy the threshold criterion, wherein updating the initial dictionary includes performing a global optimization that searches a parameter space encompassing potential quantitative parameters, identifying the potential quantitative parameters that satisfy the threshold criterion, and adding the potential quantitative parameters that satisfy the threshold criterion to the initial dictionary to generate an updated dictionary, and wherein step (c) is repeated using the updated dictionary; and