Phonon-bottleneck enhanced magnetic hysteresis in a molecular paddle wheel complex of Ru25+

Abstract

The ruthenium based molecular magnet [Ru2(D(3,5-Cl2Ph)F)4Cl(0.5H2O)·C6H14] (hereafter Ru2) behaves as a two-level system at sufficiently low temperatures. The authors performed spin detection by means of single-crystal measurements and obtained magnetic hysteresis loops around zero bias as a function of field sweeping rate. Compared to other molecular systems, Ru2 presents an enhanced irreversibility as shown by "valleys" of negative differential susceptibility in the hysteresis curves. Simulations based on phonon bottleneck model are in good qualitative agreement and suggest an abrupt spin reversal combined with insufficient thermal coupling between sample and cryostat phonon bath.Molecular magnets have been explored intensively in the recent years for their potential application in information technology and as test beds for quantum mechanics at macroscopic scale. These systems are tunable, identical, two-or multilevel systems that can be produced in large numbers and therefore are potential candidates for qubit implementation in quantum computing algorithms [1]. In crystalline form, the molecules are relatively well isolated from each other and thus the quantum physics of their spin is not strongly affected by the collective nature of the sample. Large spin molecular magnets have demonstrated key quantum effects, such as quantum tunneling of the magnetization through an anisotropy barrier [2,3] and Berry phase interference [4]. Low spin molecules have shown interesting effects when tuning phonon dissipation [5] that provide increased relaxation and decoherence times for the molecular qubits.In the case of low-spin molecular systems, the anisotropy barrier against spin reversal is often very small. However, magnetic hysteresis has been recently measured for a series of low-spin molecules (V 15 S=1/2, Fe 10 S=1, V 6 S=1/2) [5,6,7,8] and explained in the frame of the phonon-bottleneck (PB) model [6,9]. In this model, the phonons' low heat capacity keeps the lattice and the spins at the same temperature T s , slightly different from cryostat temperature T , as a result of inherent limited sample thermalization in the experimental setup. Cycling of an external magnetic field induces a delay (hysteresis) in the dynamics of the spin temperature which is observed by measuring the magnetic moment of a single crystal. Other theoretical interpretations treat * Electronic email: ichiorescu@fsu.edu the lattice at equilibrium with the cryostat at a temperature T = T s [10]. Though magnetic hysteresis can be simulated for a given bath temperature, these models cannot explain the observed dependence on sample thermalization [5] and the picture of phonons having very low heat capacity at low temperatures [9]. On the other hand, the PB model presented in Ref. [6] gives a good quantitative agreement with the experiments. The present study introduces a particular aspect of the phonon-bottleneck phenomena as observed in the Ru 2 paddle wheel molecular system (structure in Fig. 1). Single crystal measurements reveal enhanced magnet...

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