Equilibrium susceptibilities of superparamagnets: longitudinal and transverse, quantum and classical.

The equilibrium susceptibility of uniaxial paramagnets is studied in a unified framework which permits us to connect traditional results of the theory of quantum paramagnets, S = 1/2,1,3/2,..., with molecular magnetic clusters, S∼5,10,20 all the way up (S = 30,50,100,...,) to the theory of classical superparamagnets. This is done using standard tools of quantum statistical mechanics and linear-response theory (the Kubo correlator formalism). Several features of the temperature dependence of the susceptibility curves (crossovers, peaks, deviations from Curie law) are studied and their scalings with S identified and characterized. Both the longitudinal and transverse susceptibilities are discussed, as well as the response of the ensemble with anisotropy axes oriented at random. For the latter case a simple approximate formula is derived too, and its range of validity assessed, which could be used in the modelization of experiments.

Low-field susceptibility of classical Heisenberg chains with arbitrary and different nearest-neighbour exchange.

Interest in molecular magnets continues to grow, offering a link between the atomic and nanoscale properties. The classical Heisenberg model has been effective in modelling exchange interactions in such systems. In this, the magnetization and susceptibility are calculated through the partition function, where the Hamiltonian contains both Zeeman and exchange energy. For an ensemble of N spins, this requires integrals in 2N dimensions. For two, three and four spin nearest-neighbour chains these integrals reduce to sums of known functions. For the case of the three and four spin chains, the sums are equivalent to results of Joyce. Expanding these sums, the effect of the exchange on the linear susceptibility appears as Langevin functions with exchange term arguments. These expressions are generalized here to describe an N spin nearest-neighbour chain, where the exchange between each pair of nearest neighbours is different and arbitrary. For a common exchange constant, this reduces to the result of Fisher. The high-temperature expansion of the Langevin functions for the different exchange constants leads to agreement with the appropriate high-temperature quantum formula of Schmidt et al, when the spin number is large. Simulations are presented for open linear chains of three, four and five spins with up to four different exchange constants, illustrating how the exchange constants can be retrieved successfully.

Spin dynamics in a dissipative environment: from quantal to classical.

We address the problem of spin dynamics in the presence of a thermal bath, by solving exactly the appropriate quantum master equations with continued-fraction methods. The crossover region between the quantum and classical domains is studied by increasing the spin value , and the asymptote for the classical absorption spectra is eventually recovered. Along with the recognized relevance of the coupling strength, we show the critical role played by the structure of the system-environment interaction in the emergence of classical phenomenology.

Large quantum nonlinear dynamic susceptibility of single-molecule magnets.

The nonlinear dynamical response of Mn12 single-molecule magnets is experimentally found to be very large, quite insensitive to the spin-lattice coupling constant, and displaying peaks reversed with respect to classical superparamagnets. It is shown that these features are caused by the strong field dependence of the relaxation rate due to the detuning of energy levels between which tunneling takes place. The nonlinear susceptibility technique, previously overlooked, is thus proposed as a privileged probe to ascertain the occurrence of quantum effects in mesoscopic magnetic systems.