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The anisotropy barrier of polynuclear single‐molecule magnets is expected to be higher with less tunneling the better stabilized the spin ground state is so that less MS mixing in the ground state and with excited spin states occur. We have realized this experimentally in two structurally related heptanuclear SMMs: the triplesalen‐based [MnIII6CrIII]3+ and the triplesalalen‐based *[MnIII6CrIII]3+...
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