We study control of electron-nuclear spin dynamics at magnetic field strengths where the Larmor frequency of the nucleus is comparable to the hyperfine coupling strength. The quantization axis for the nuclear spin differs from the static B₀ field direction and depends on the state of the electron spin. The quantization axis can be switched by flipping the state of electron spin, allowing for universal control of nuclear spin states. We show that by performing a sequence of flips (each followed by a suitable delay), we can perform any desired rotation of the nuclear spin, which can also be conditioned on the state of the electron spin. These operations, combined with electron spin rotations, can be used to synthesize any unitary transformation of the coupled electron-nuclear spin system. We discuss how these methods can be used for design of experiments for transfer of polarization from the electron to the nuclear spins.
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Navin Khaneja (2007) studied this question.
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