September 2011

Journal

Size-dependent magnetic ordering and spin-dynamics in DyPO4 and GdPO4 nanoparticles

By:
Evangelisti, Marco; Sorop, Tibi; Bakharev, Oleg; Visser, Dirk; Hillier, Adrian; Alonso, Juan; Haase, Markus; Boatner, Lynn A; De Jongh, L.
Journal Name:
Physical Review B
Page Number:
094408
Volume:
94
Issue Number:
9
Publication Date:
September 2011
View DOI Listing:
https://doi.org/10.1103/PhysRevB.84.094408

Abstract

Low-temperature magnetic susceptibility and heat capacity measurements on nanoparticles (d ≈ 2.6 nm) of the antiferromagnetic compounds DyPO4 (TN = 3:4 K) and GdPO4 (TN = 0:77 K) provide clear demonstrations of finite-size effects, which limit the divergence of the magnetic correlation lengths, thereby suppressing the bulk long-range magnetic ordering transitions. Instead, the incomplete antiferromagnetic order inside the particles leads to the formation of net magnetic moments on the particles. For the nanoparticles of Ising-type DyPO4 superparamagnetic blocking is found in the ac-susceptibility at ≃ 1 K, those of the XY-type GdPO4 analogue show a dipolar spin-glass transition at ≃ 0:2 K. Monte Carlo simulations for the magnetic heat capacities of both bulk and nanoparticle samples are in agreement with the experimental data. Strong size effects are also apparent in the Dy3+ and Gd3+ spin-dynamics, which were studied by zero-field SR relaxation and high-field 31P-NMR nuclear relaxation measurements. The freezing transitions observed in the ac-susceptibility of the nanoparticles also appear as peaks in the temperature dependence of the zero-field SR rates, but at slightly higher temperatures - as to be expected from the higher frequency of the muon probe. For both bulk and nanoparticles of GdPO4, the muon and 31P-NMR rates are for T ≥ 5 K dominated by exchange-narrowed hyperfine broadening arising from the electron spin-spin interactions inside the particles. The dipolar hyperfine interactions acting on the muons and the 31P are, however, much reduced in the nanoparticles. For the DyPO4 analogues the high-temperature rates appear to be fully determined by electron spin-lattice relaxation processes.