摘要：SummaryLong decoherence time is a key consideration for molecular magnets in the application of the quantum computation. Although previous studies have shown that the local symmetry of spin carriers plays a crucial part in the spin-lattice relaxation process, its role in the spin decoherence is still unclear. Herein, two nine-coordinated capped square antiprism neodymium moieties [Nd(CO3)4H2O]5–with slightly different local symmetries,C1versusC4(1and2), are reported, which feature in the easy-plane magnetic anisotropy as shown by the high-frequency electron paramagnetic resonance (HF-EPR) studies. Detailed analysis of the relaxation time suggests that the phonon bottleneck effect is essential to the magnetic relaxation in the crystalline samples of1and2. The 240 GHz Pulsed EPR studies show that the higher symmetry results in longer decoherence times, which is supported by the first principle calculations.Graphical AbstractDisplay OmittedHighlights•Neodymium-based complexes show the spin decoherence without the magnetic dilution•The higher structural symmetry results in longer spin decoherence times•The phonon bottleneck effect induces the slow magnetization relaxation behaviorsMaterials Property; Molecules; Quantum Chemical Calculations
