Spin dynamics and magnetic phase diagram of La1xCaxMnO3 (0<~x<~0.15)

Abstract
Spin dynamics of ceramic La1xCaxMnO3 with x=0, 0.05, and 0.15 and the relative Mn4+ concentration c=0.180.22 is investigated by measurements of the ac susceptibility and the relaxation of the thermoremanent magnetization (TRM). The χac(T) function exhibits a transition from the paramagnetic to a mixed spin-glass and ferromagnetic phase. Below that is found a steep decrease and onset of the frequency dependence of χac(T), providing evidence for existence of a reentrant spin glass (RSG) phase. The dependence of the spin-glass freezing temperature, Tf, on f satisfies the conventional critical slowing-down law, τ/τ0=(Tf/TG1)zv with τ=1/f, zv=12±2, τ01012s and the glass temperature, TG, decreasing from 93 to 70.5 K when x is increased from 0 to 0.15. The relaxation rate S(t) of TRM has a clear maximum near a wait time tw(24)×103s and the function S(T) shows a sharp maximum near TG. The plots of S(T) exhibit a substantial decrease at T>TG while for T<TG they collapse into a single curve, as typical for mixed (TG<T<TC) and RSG phases, respectively. The observed spin dynamics agrees completely with the magnetic phase diagram (paramagnetic, mixed, and RSG phases with decreasing T) predicted recently for a system containing lattice disorder and competing superexchange and double exchange interactions.