Pair binding and Hund's rule breaking in high-symmetry fullerenes

TL;DR

This study uses large-scale density-matrix renormalization group calculations to explore pair binding and Hund's rule breaking in high-symmetry fullerenes, revealing a lower Mott transition point and complex magnetic behaviors.

Contribution

It provides a computationally efficient analysis of Hund's rule breaking and pair binding in high-symmetry fullerenes, improving understanding of their electronic properties.

Findings

Mott transition at Uc~2.2t for C20, lower than previous estimates.

Pair-binding energy remains overall repulsive across U values.

Hund's rule is broken in C40 and C60, with doping affecting magnetic states.

Abstract

Highly-symmetric molecules often exhibit degenerate tight-binding states at the Fermi edge. This typically results in a magnetic ground state if small interactions are introduced in accordance with Hund's rule. In some cases, Hund's rule may be broken, which signals pair binding and goes hand-in-hand with an attractive pair-binding energy. We investigate pair binding and Hund's rule breaking for the Hubbard model on high-symmetry fullerenes C$_{20}$, C$_{28}$, C$_{40}$, and C$_{60}$ by using large-scale density-matrix renormalization group calculations. We exploit the SU(2) spin symmetry, the U(1) charge symmetry, and optionally the Z(N) spatial rotation symmetry of the problem. For C$_{20}$, our results agree well with available exact-diagonalization data, but our approach is numerically much cheaper. We find a Mott transition at $U_c\sim2.2t$, which is much smaller than the previously reported value of $U_c\sim4.1t$ that was extrapolated from a few datapoints. We compute the pair-binding energy for arbitrary values of $U$ and observe that it remains overall repulsive. For larger fullerenes, we are not able to evaluate the pair binding energy with sufficient precision, but we can still investigate Hund's rule breaking. For C$_{28}$, we find that Hund's rule is fulfilled with a magnetic spin-2 ground state that transitions to a spin-1 state at $U_{c,1}\sim5.4t$ before the eventual Mott transition to a spin singlet takes place at $U_{c,2}\sim 11.6t$. For C$_{40}$, Hund's rule is broken in the singlet ground state, but is restored if the system is doped with one electron. Hund's rule is also broken for C$_{60}$, and the doping with two or three electrons results in a minimum-spin state. Our results are consistent with an electronic mechanism of superconductivity for C$_{60}$ lattices. We speculate that the high geometric frustration of small fullerenes is detrimental to pair binding.