Orbital Order Effect of Two-Dimensional Spin Gap System for CaV4O9

TL;DR

This paper investigates how orbital order influences the magnetic properties of CaV4O9, revealing that considering multiple orbitals improves agreement with experimental data but some discrepancies remain.

Contribution

It introduces a multi-orbital model for CaV4O9 that better explains experimental magnetic properties than previous single-orbital models.

Findings

Multi-orbital configurations better reproduce experimental data.

Some discrepancies suggest the importance of the $d_{xy}$ orbital.

Calculated susceptibilities and correlations depend on orbital order configurations.

Abstract

Effects of possible orbital order in magnetic properties of two-dimensional spin gap system for CaV$_4$O$_9$ are investigated theoretically. After analyzing experimental data, we show that single orbital models assumed in the literature are insufficient to reproduce the data. To understand the origin of the discrepancy, we assume that in $d^1$ state of V, $d_{xz}$ and $d_{yz}$ orbitals have substantial contributions in the lowest-energy atomic level which leads to a double-degeneracy. We study possible configurations of the orbital order. By exact diagonalization and perturbation expansion, we calculate the susceptibility, wavenumber dependence of low-lying excitations and equal-time spin-spin correlations which is related to integrated intensity of the neutron inelastic scattering. These quantities sensitively depend on the configuration of the orbital order. The calculated results for some configurations of the orbital order reproduce many experimental results much better than the previous single-orbital models. However some discrepancy still remains to completely reproduce all of the reported experimental results. To understand the origin of these discrepancies, we point out the possible importance of the partially occupied $d_{xy}$ orbital in addition to orbital order of partially filled $d_{xz}$ and $d_{yz}$ orbitals.