Dynamical Monte Carlo investigation of spin reversals and nonequilibrium magnetization of single-molecule magnets

TL;DR

This study integrates thermal effects and Landau-Zener quantum tunneling within a dynamical Monte Carlo framework to accurately simulate magnetization behaviors of single-molecule magnets, revealing temperature-dependent reversal mechanisms and the influence of magnetic dipolar interactions.

Contribution

It introduces a combined thermal and quantum tunneling Monte Carlo method for modeling SMM magnetization, highlighting the roles of different reversal processes across temperatures.

Findings

Clear step structures in low-temperature magnetization curves.

Thermally activated barrier hurdling dominates near 3K.

Thermal-assisted tunneling is significant at intermediate temperatures.

Abstract

In this paper, we combine thermal effects with Landau-Zener (LZ) quantum tunneling effects in a dynamical Monte Carlo (DMC) framework to produce satisfactory magnetization curves of single-molecule magnet (SMM) systems. We use the giant spin approximation for SMM spins and consider regular lattices of SMMs with magnetic dipolar interactions (MDI). We calculate spin reversal probabilities from thermal-activated barrier hurdling, direct LZ tunneling, and thermal-assisted LZ tunnelings in the presence of sweeping magnetic fields. We do systematical DMC simulations for Mn$_{12}$ systems with various temperatures and sweeping rates. Our simulations produce clear step structures in low-temperature magnetization curves, and our results show that the thermally activated barrier hurdling becomes dominating at high temperature near 3K and the thermal-assisted tunnelings play important roles at intermediate temperature. These are consistent with corresponding experimental results on good Mn$_{12}$ samples (with less disorders) in the presence of little misalignments between the easy axis and applied magnetic fields, and therefore our magnetization curves are satisfactory. Furthermore, our DMC results show that the MDI, with the thermal effects, have important effects on the LZ tunneling processes, but both the MDI and the LZ tunneling give place to the thermal-activated barrier hurdling effect in determining the magnetization curves when the temperature is near 3K. This DMC approach can be applicable to other SMM systems, and could be used to study other properties of SMM systems.