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Qubits are the basic unit of quantum information and computation. To realize quantum computing and information processing, the decoherence times of qubits must be long enough. Among the studies of molecule‐based electron spin qubits, most of the work focused on the ions with the spin S=1/2, where only single‐bit gates can be constructed. However, quantum operations require the qubits to interact with each other, so people gradually carry out relevant research in ions or systems with S>1/2 and multilevel states. In this work, a two‐dimensional (2D) oxygen‐coordinated GdIIINaI‐based oxamato supramolecular coordination framework, Na[Gd(4‐HOpa)4(H2O)] ⋅ 2H2O (1, 4‐HOpa=N‐4‐hydroxyphenyloxamate), was selected as a possible carrier of qubit. The field‐induced slow magnetic relaxation shows this system has phonon bottleneck (PB) effect at low temperatures with a very weak magnetic anisotropy. The pulse electron paramagnetic resonance studies show the spin‐lattice and spin‐spin relaxation times are T1=1.66 ms at 4 K and Tm=4.25 μs at 8 K for its diamagnetically diluted sample (1Gd0.12 %). It suggested that the relatively long decoherence time is mainly ascribed to its near isotropic and the PB effect from resonance phonon trapped for pure sample, while the dilution further improves its qubit performance. [ABSTRACT FROM AUTHOR]

• A soft tripodal ligand was used to construct a high-spin Co(II) complex with weak ligand field. • HFEPR and magnetic data reveal easy-axis anisotropy and SMM's behavior for this complex. • This complex is the first instance of Co(II)-based single-ion magnet with an octahedral CoS 6 unit. The soft donor ligands are of great importance to the pursuit of 3d transition-metal complexes with large magnetic anisotropy. Herein, a soft tripodal ligand, hydrotris(mercaptobenzothiazolyl)borate (Tbz) was used to construct a high-spin mononuclear complex [CoII(Tbz) 2 ] (1), having an octahedral geometry in an S 6 donor set. The combination of direct-current (dc) magnetic susceptibility and Low-temperature high-field electron paramagnetic resonance (HFEPR) reveals the easy-axis magnetic anisotropy of 1. Complex 1 shows field-induced slow relaxation of magnetization at an applied magnetic field of 1000 Oe, indicating the behavior of single-molecule magnet. The foregoing result constitutes the first instance of Co(II)-based single-ion magnet containing a CoS 6 unit. [ABSTRACT FROM AUTHOR]