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The lifetime Ts of a long‐lived nuclear spin state (LLS) could be much longer than the longitudinal order T1. Many spin systems were used to produce long‐lived states, including two or more homonuclear spins that couple to each other. For multiple homonuclear spins with rather small chemical shift difference, normally it is difficult to selectively control the spins and then to prepare a LLS. Herein, we present a scheme that prepares different spin orders in a multi‐spin system by using optimal control and numerical calculation. By experimentally measuring the lifetime of the states, we find that for a three‐spin physical system, although there are many forms of state combinations with different spin orders, each component has its own lifetime.

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