Nontrivial Spin Dynamics Synergy in a Weakly Coupled Heteroanisotropic Dysprosium Chain-Based Array

Spin chains (SCs) are fascinating due to their exotic quantum effects and promising applications. Despite the significant challenges in chemically aligning heteroanisotropic spins into weakly coupled chains, it is essential for advancing molecular spin engineering and exploring novel quantum behaviors. As well-defined, highly anisotropic, and two-level quantum systems, single-molecule magnet (SMM) units provide an excellent platform for the bottom-up approach to constructing heteroanisotropic spin chains. Herein, we successfully linked Ising-like dysprosium into one-dimensional (1D) spin chains via coordination bonds, resulting in three novel 1D arrays of homo/heteroanisotropic dysprosium (SC-α, SC-β, and SC-αβ) built from two kinds of pro-SMM units (α and β) connected by hydroquinone along the easy axes. Unlike the homodysprosium chains (SC-α and SC-β) and traditional single-chain magnets (SCMs) with strong coupling, the weakly coupled hetero-SMM chain (SC-αβ) revealed nontrivial synergistic spin dynamics between magnetic anisotropy and temperature-dependent spin polarization, leading to a unique two-stage magnetic quantum tunneling phenomena occurring at high and low temperatures. Furthermore, we demonstrated unprecedented control of spin orientation between the heterodysprosium units by manipulating magnetizing paths. These findings highlight the significant potential of weakly coupled heteroanisotropic spin chains, with distinct relaxation lifetimes, for novel applications in quantum information storage and processing.