Antipolar and short and long-range magnetic ordering in quasi-two-dimensional AgCrP2S6

TL;DR

This study investigates multiple magnetic and polar phase transitions in quasi-2D AgCrP2S6 using Raman scattering and first-principles calculations, revealing complex ordering phenomena and symmetry changes at various temperatures.

Contribution

It provides the first detailed Raman and theoretical analysis of the temperature-dependent magnetic, polar, and lattice orderings in AgCrP2S6, uncovering quasi-antipolar and antipolar phases.

Findings

Identified spin ordering transitions at ~90 K and 20 K.

Discovered potential quasi-antipolar ordering at ~200 K.

Observed symmetry lowering and doubling of phonon modes below ~200 K.

Abstract

Within the Landau theoretical framework, the decreased entropy with decreasing the temperature is accompanied by the symmetry breaking and hence a corresponding phase transition. The broken symmetries leave its imprint on the underlying excitations and the same may be gauged using renormalization of these excitations. AgCrP2S6 provides a versatile playground to probe dynamics of the quasiparticle excitations as well as multiple phase transitions with lowering temperature linked with the polar, lattice and spin degrees of freedom. Here, we report an in-depth temperature- and polarization-dependent Raman scattering measurements on single crystals of quasi 2D zigzag antiferromagnet AgCrP2S6 along with the first principle based phonon calculations. We observed multiple phase transitions triggered by the short and long-range ordering of spins at ~ 90 K and 20 K, respectively; within the Cr sublattice where spins are arranged in a 1D chain, evident by the distinct anomalies in the phonon modes self-energy parameters as well as intensity. Contrary to the conventional belief, we uncovered potential quasi-antipolar ordering at ~ 200 K and with further lowering in temperature an antipolar ordering at ~ 140 K attributed to the Ag ions, which is conjectured to be forbidden owing to the heaviness of Ag ions. The quasi-antipolar and antipolar ordering is gauged via the distinct renormalization of the phonon parameters, which survives at all the temperatures. Additionally, large number of modes appears with decreasing the temperature, in the window of ~ 200-140 K, where antipolar ordering starts settling in. The emergence of large number of phonon modes below ~ 200 K, nearly double of those at room temperature, suggests the lowering of symmetry from high temperature C2h to the low temperature C2 or Cs and as a result doubling of the unit cell.