A theory of the quantum spin liquid in the hyper-honeycomb metal-organic framework [(C2H5)3NH]2Cu2(C2O4)3 from first principles

A. C. Jacko, B. J. Powell

What is a hyper-honeycomb lattice?

It is a three-dimensional version of the honeycomb lattice.

A simple tight-binding model on the lattice has Dirac cones, just like graphene.

The preprint is a nice example how one can start with a structure that is chemically and structurally complex and then use calculations based on Density Functional Theory (DFT) to derive a "simple" effective Hamiltonian (in this case an antiferrromagnetic Heisenberg model of coupled chains) to describe the low-energy physics of the material.

We construct a tight-binding model of [(C2H5)3NH]2Cu2(C2O4)3 from Wannier orbital overlaps. Including interactions within the Jahn-Teller distorted Cu-centered eg Wannier orbitals leads to an effective Heisenberg model. The hyper-honeycomb lattice contains two symmetry distinct sublattices of Cu atoms arranged in coupled chains. One sublattice is strongly dimerized, the other forms isotropic antiferromagnetic chains. Integrating out the strongest (intradimer) exchange interactions leaves extremely weakly coupled Heisenberg chains, consistent with the observed low temperature physics.There is some rather subtle physics involved in the superexchange processes that determine the magnitude of the antiferromagnetic interactions J between neighbouring spins. In particular, there are destructive quantum interference effects that reduce one of the J's by an order of magnitude and increases another by an order of magnitude. To illustrate this effect, the authors also evaluate the J's when one flips the sign of some of the matrix elements in the tight-binding model. Similar subtle physics has also been observed in different families of organic charge transfer salts.

As an aside, there is some similarity (albeit many differences) with the basic chemistry of the insulating phase of cuprates: the parent compound involves a lattice of copper ions (d9) where there are three electrons in eg orbitals that are split by a Jahn-Teller distortion. The differences here are first, that the interactions between the frontier orbitals on the Cu sites is not via virtual processes involving oxygen p-orbitals but rather via pi-orbitals on the oxalate bridging orbitals. Second, the lattice of Cu orbitals is not a square but the hyper-honeycomb lattice.

The preprint is motivated by a recent experimental paper in JACS

Quantum Spin Liquid from a Three-Dimensional Copper-Oxalate Framework

Bin Zhang, Peter J. Baker, Yan Zhang, Dongwei Wang, Zheming Wang, Shaokui Su, Daoben Zhu, and Francis L. Pratt

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