Frustrated square lattice with spatial anisotropy: crystal structure and magnetic properties of PbZnVO(PO4)2

TL;DR

This study investigates the crystal structure and magnetic properties of PbZnVO(PO4)2, revealing spatial anisotropy in exchange interactions and its effects on magnetic ordering, supported by experimental measurements and band structure calculations.

Contribution

It provides the first detailed analysis of PbZnVO(PO4)2's magnetic interactions, highlighting spatial anisotropy and proposing a new approach to designing frustrated square lattice materials.

Findings

Nearest-neighbor coupling J(1) ~ -5.2 K

Next-nearest-neighbor coupling J(2) ~ 10.0 K

Magnetic ordering transition at 3.9 K

Abstract

Crystal structure and magnetic properties of the layered vanadium phosphate PbZnVO(PO4)2 are studied using x-ray powder diffraction, magnetization and specific heat measurements, as well as band structure calculations. The compound resembles AA'VO(PO4)2 vanadium phosphates and fits to the extended frustrated square lattice model with the couplings J(1), J(1)' between nearest-neighbors and J(2), J(2)' between next-nearest-neighbors. The temperature dependence of the magnetization yields estimates of averaged nearest-neighbor and next-nearest-neighbor couplings, J(1) ~ -5.2 K and J(2) ~ 10.0 K, respectively. The effective frustration ratio alpha=J(2)/J(1) amounts to -1.9 and suggests columnar antiferromagnetic ordering in PbZnVO(PO4)2. Specific heat data support the estimates of J(1) and J(2) and indicate a likely magnetic ordering transition at 3.9 K. However, the averaged couplings underestimate the saturation field, thus pointing to the spatial anisotropy of the nearest-neighbor interactions. Band structure calculations confirm the identification of ferromagnetic J(1), J(1)' and antiferromagnetic J(2), J(2)' in PbZnVO(PO4)2 and yield J(1)'-J(1) ~ 1.1 K in excellent agreement with the experimental value of 1.1 K, deduced from the difference between the expected and experimentally measured saturation fields. Based on the comparison of layered vanadium phosphates with different metal cations, we show that a moderate spatial anisotropy of the frustrated square lattice has minor influence on the thermodynamic properties of the model. We discuss relevant geometrical parameters, controlling the exchange interactions in these compounds, and propose a new route towards strongly frustrated square lattice materials.