Beating the macroscopic quantum tunneling limit by man-made magnetic dead layers

Magnetic dead layers (MDLs) are always undesirable in practical applications due to their highly frustrated spin configurations and severe degradation of host magnetism. Here we provide new insights in MDLs and unravel their attractive prospect for ferrimagnetic hybrid of Fe3O4 and γ-Fe2O3 (denoted as Fe3O4@γ-Fe2O3 in the main text) to exhibit macroscopic quantum tunneling (MQT) phenomena in measureable kelvin range. The 3 nm-sized negatively-charged Fe3O4@γ-Fe2O3 nanoparticles were immersed in various metal chloride solutions containing Mn2+, Co2+, Ni2+, Fe3+, and Fe2+ cations to form cationic MDLs via electrostatic attraction. These man-made MDLs, if being of positive enough zeta potentials, greatly disordered the magnetic dipole interactions among Fe3O4@γ-Fe2O3 nanoparticles and induce extra energy barrier to yield pronounced MQT effect in Fe3O4@γ-Fe2O3 nanoparticles even though they were dispersed neither in water nor in oil. Their crossover temperatures dividing MQT and purely thermal relaxation were found to be one order of magnitude higher than reported values in other MQT systems, and more strikingly, they could be tailored by altering the soak period in our facile and scalable route.