A method for controlling a nuclear magnetic resonance (NMR) apparatus , comprising: controlling the NMR apparatus to apply radio frequency (RF) energy to a volume n an object, where the RF energy is applied in two or more coordinated series of nuclear magnetic resonance fingerprinting (NMRfp) variable sequence blocks, where a variable sequence block includes one or more excitation phases, one or more readout phases, and one or more waiting phases, where at least one sequence block in a series of variable sequence blocks differs from at least one other variable sequence block in the series in at least N sequence block parameters, N being an integer greater than one, where a first member of the coordinated series is configured to cause a first nuclei type in the volume to produce a first NMR signal, and where a second member of the coordinated series is configured to cause a second different nuclei type in the volume to produce a second NMR signal; controlling the NMR apparatus to repetitively and variably sample a (k, t, E, n) space associated with the volume to acquire a set of NMR signals associated with two or more types of nuclei in the space, where members of the set of NMR signals are associated with different points in the (k, t, E, n) space, where k is frequency space, t is time, where E includes at least one NMR parameter, and where n is nuclei, controlling the NMR apparatus to determine a signal evolution from the set of NMR signals where the signal evolution is a function of NMR excitation produced by applying the RF energy in the coordinated series of variable sequence blocks; and controlling the NMR apparatus to characterize the volume by comparing the signal evolution to one or more of, a reference signal evolution, and a combination of reference signal evolutions. controlling the NMR apparatus to apply radio frequency (RF) energy to a volume n an object, where the RF energy is applied in two or more coordinated series of nuclear magnetic resonance fingerprinting (NMRfp) variable sequence blocks, where a variable sequence block includes one or more excitation phases, one or more readout phases, and one or more waiting phases, where at least one sequence block in a series of variable sequence blocks differs from at least one other variable sequence block in the series in at least N sequence block parameters, N being an integer greater than one, where a first member of the coordinated series is configured to cause a first nuclei type in the volume to produce a first NMR signal, and where a second member of the coordinated series is configured to cause a second different nuclei type in the volume to produce a second NMR signal; controlling the NMR apparatus to repetitively and variably sample a (k, t, E, n) space associated with the volume to acquire a set of NMR signals associated with two or more types of nuclei in the space, where members of the set of NMR signals are associated with different points in the (k, t, E, n) space, where k is frequency space, t is time, where E includes at least one NMR parameter, and where n is nuclei, controlling the NMR apparatus to determine a signal evolution from the set of NMR signals where the signal evolution is a function of NMR excitation produced by applying the RF energy in the coordinated series of variable sequence blocks; and controlling the NMR apparatus to characterize the volume by comparing the signal evolution to one or more of, a reference signal evolution, and a combination of reference signal evolutions. <EOS>