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Gd3+ complexes have been shown to undergo unusual slow magnetic relaxation processes similar to those of single‐molecule magnets (SMMs), even though Gd3+ does not exhibit strong magnetic anisotropy. To reveal the origin of the slow magnetic relaxation of Gd3+ complexes, we have investigated the magnetic properties and heat capacities of two Gd3+‐phthalocyaninato triple‐decker complexes, one of which...
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