Abstract: Finely manipulating a large population of interacting nuclear spins is an extremely challenging problem arising in wide-ranging applications in quantum science and technology. Prominent examples include the design of robust excitation and inversion pulses for nuclear magnetic resonance spectroscopy and imaging, coordination of spin networks for coherence transfer, and control of superposition and entanglement for quantum computation. In this paper, by integrating the technique of small angle approximation with non-harmonic Fourier analysis, we establish a systematic method to construct robust pulse sequences that neutralize the effect of coupling variations in a spin network. In addition, we explore an alternating optimization procedure for tailoring the constructed pulses to satisfy practical design criteria. We also provide numerical examples to demonstrate the efficacy of the proposed methodology.
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