Evidence for superferrimagnetic clusters and spin-glass transition involving 4f Dy3+ spins in h-DyMnO3: A new twist to 4f Re3+ spin ordering in hexagonal manganites

TL;DR

This study reveals that Dy3+ spins in h-DyMnO3 exhibit superferrimagnetic and spin-glass states due to geometrical frustration, challenging previous assumptions of long-range order and highlighting complex magnetic behavior in hexagonal manganites.

Contribution

It demonstrates that Dy3+ spins do not form long-range order but instead show superferrimagnetic and spin-glass states driven by geometrical frustration, with novel crossover behavior.

Findings

Dy3+ spins are in a superferrimagnetic state below 68K.

Dy3+ spins undergo a spin-glass transition below 7K.

The spin-glass state shows a crossover from de Almeida-Thouless to Gabay-Toulouse behavior.

Abstract

The ferroelectric phase of the multiferroic hexagonal manganites (h-ReMnO3) has been reported to undergo a series of magnetic transitions involving long-range ordering/reorientation of 4fRe3+ and/or 3dMn3+ spins below room temperature. These transitions have attracted a lot of attention in recent years due to the geometrically frustrated nature of magnetic interactions. We have revisited these transitions in high quality single crystals of h-DyMnO3 using dc and ac susceptibility measurements as a function of temperature (T), magnetic field (H) and frequency (w) supplemented by specific heat measurements. Taking h-DyMnO3 as an example, we show that the Dy3+ spins below TN~68K are in a superferrimagnetic (SFIM) state whereas they undergo spin-glass (SG) transition below TDy3+~7K. Our observations demonstrate that neither the N\'eel transition at TN~68K nor the transition at TDy3+~7K is associated with long-range ordered states of Dy3+ spins as believed so far in the literature. The SG state of h-DyMnO3 is quite exotic as it occurs in an ordered compound purely due to geometrical frustration without any random disorder. Further, it shows an interesting crossover from de Almeida-Thouless type exponent (m=2/3) to Gabay-Toulouse type (m=2) with increasing field which cannot be explained in terms of the existing mean field theories of SG transition in Ising or Heisenberg systems but is expected for a vector X-Y SG system. Our observations call for a systematic reinvestigation of the nature of magnetic transitions involving Re3+ ions in other h-ReMnO3 also.