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Small perturbations of steady-state sequence parameters can induce very large spectral profile deviations that are localized to specific off-resonant frequencies, denoted critical frequencies. Although, a small number of studies have previously considered the use of these highly specific modulations for MR angiography and elastography, many potential applications still remain to be explored. An analysis of this phenomenon using a linear systems technique and a geometric magnetization trajectory technique shows that the critical frequencies correspond to singularities in the steady-state signal equation. An interleaved acquisition combined with a complex difference technique yields a spectral profile containing sharp peaks interleaved with wide stopbands, while a complex sum technique yields a spectral profile similar to that of balanced steady-state free precession. Simulations and phantom experiments are used to demonstrate a novel application of this technique for positive-contrast imaging of superparamagnetic iron-oxide nanoparticles. The technique is shown to yield images with high levels of positive contrast and good water and fat background suppression. The technique can also simultaneously yield images with contrast similar to balanced steady-state free precession.