Linear and cubic dynamic susceptibilities of superparamagnetic fine particles Yuri L. Raikher and Victor I. Stepanov Institute of Continuous Media Mechanics, Urals Branch of RAS, 614013, Perm, Russia Received 21 February 1997 A consistent theory of linear and nonlinear cubicinitial susceptibilities of an assembly of uniaxially anisotropic noninteracting fine magnetic particles is presented. The expressions for the static equilibrium susceptibilities are obtained directly from the pertinent statistical thermodynamics. The contributions of an- isotropy emerge yet in the first order and are analyzed for random and axes-aligned distributions. The ac susceptibilities are studied on the basis of the micromagnetic Fokker-Planck equation. Both a numerically exact solution for arbitrary frequency and a reliable low-frequency approximation are given. The obtained description proves to be more accurate as compared to the one based on the customary superparamagnetic blocking model. The results are used for a quantitative interpretation of recently published set of data on Co-Cu precipitating alloys. In this connection the choice of the particle size-distribution function is discussed. S0163-18299704722-X INTRODUCTION Since the very first studies of fine-particle systems, 1 the development of the micromagnetic science was inspired mainly by the necessity to predict the magnetic properties and response of a ferromagnetic particulate media. Beyond argument, in this objective the fundamental and applicational aspects are tied up very closely, if not inseparably. The problem of prime interest while performing experi- ments on or manufacturing fine-particle magnetic systems is to characterize the magnetic content of the sample with as few measurements as possible. Magnetic granulometry by means of a quasistatic magnetization curve is very well known and widely used. 1–3 The dynamic approach, where simultaneously linear and nonlinear susceptibilities are taken into account is more new, being most probably inspired by its use in the spin-glass science. To justify the method, one should process a good deal of experimental data with the aid of an appropriate theory. Such a work has been attempted recently in Refs. 4,5 with a precipitating Cu-Co alloy as a test object. The authors had no difficulties in fitting the linear susceptibility measurements with the aid of superparamag- netic blocking model assuming that: ithe particles are single domain and their magnetization does not depend on temperature, iithe magnetic anisotropy is uniaxial and has one and the same value for all the particles, and iiithe magnetic dipole-dipole interaction is negligible. It was fitting the nonlinear cubicsusceptibility data where a problem arose, since there was no theory for it insofar, consistent with the aforementioned assumptions. To fill the place, in Refs. 4,5 were employed the formulas originally derived for an isotropic superparamagnet. They were adjusted by replacing the pertinent relaxation time with a one exponential in the magnetic anisotropy constant K . However, the resulting agreement turned out to be poor. From that the authors of Refs. 4,5 concluded to that some of the basic assumptions iiiiare wrong. From our viewpoint, in the first place this reproach should be addressed not to the classic superpara- magnetic theory as itself but to a rather ‘‘intuitive’’ manner of its usage. The incentive and the main goal of our paper is to con- sistently extend the conventional theory on the case of a nonlinear response and by that to confirm its validity. While doing that we propose practical schemes both exact and ap- proximateto handle linear and cubic dynamic responses in the framework of classical superparamagnetism. Applying our results to the reported data on the nonlinear susceptibility of Cu-Co precipitates, we demonstrate that a fairly good agreement may be achieved easily. I. STATIC SUSCEPTIBILITIES As a starting point we take an isolated single-domain par- ticle of a ferro- or ferrimagnetic material rigidly trapped in the bulk of a solid nonmagnetic matrix. Single domain has a spatial uniformity of the spin alignment over the grain that enables us to describe it by the net magnetic moment =e, whose direction is given by a unit vector e. The magnetic moment magnitude is =I v with I the saturation magnetization of the material at given temperature and v being the particle volume. Besides that, we assume the par- ticle to possess a uniaxial magnetic anisotropy with an en- ergy density K and a direction defined by a unit vector n. If the external magnetic field H is not too high as to affect the atomic magnetic structure, its only effect on a single- domain grain is the magnetic moment rotation. Then the cor- responding orientation-dependent part of the particle energy U may be written as U =-K v en 2 -eH. 1 The stationary distribution function of the particle magnetic moment or if we neglect interactionsof an assembly of magnetic moments is determined by the Gibbs formula We=Z -1 expen 2 +eh, Z , = expen 2 +ehd e, 2 where PHYSICAL REVIEW B 1 JUNE 1997-II VOLUME 55, NUMBER 22 55 0163-1829/97/5522/1500513/$10.00 15 005 © 1997 The American Physical Society