Cooperative quantum tunneling of the magnetization in Fe-doped Li${}_3$N

Abstract

The spin-reversal in dilute Li${}_2$(Li${}_{1-x}$Fe${}_x$)N with $x<1$ % is dominated by resonant quantum tunneling of spatially well-separated states. We report on the effect of finite couplings between those states that give rise to cooperative, simultaneous quantum tunneling of two spins. This phenomenon, known as spin-spin cross relaxation, effectively elucidates the fine-structure observed in isothermal magnetization loops, a previously unresolved aspect. Temperature and field-dependent magnetization measurements were conducted over a range from T = 2 K to 300 K in applied fields of up to ${\mu }_{0}H$ = 7 T. Magnetic dipole fields are computed numerically. Our findings affirm the absence of stoichiometric defects in Li${}_2$(Li${}_{1-x}$Fe${}_x$)N and underscore its exemplary suitability as a model system for investigating spin-reversal processes at the microscopic level. This is attributed to its comparatively simple crystal structure, the availability of large single crystals, elevated characteristic energies, and well-defined energy levels

arXiv comment9 pages, 7 figures

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