Unveiling unique properties of icosahedral magnetic quasicrystals -- Multipole physics and frustration

Multipolar degrees of freedom and their hidden orders have been widely discussed in the context of heavy fermions, frustrated magnets and exotic Kondo effects. Although there has been extensive search for multipolar degrees of freedom in magnetic systems, there are few examples that allow pure multipolar degrees of freedom in the absence of magnetic dipoles. In this work, for the first time, we show that the magnetic behavior in an icosahedral quasicrystal is generally described by multipolar degrees of freedom, and in a specific case by the pure magnetic octupoles in the absence of dipoles, resulting from the interplay of spin orbit coupling and crystal field splitting. Importantly, we point out the non-crystallographic symmetries lead to multipolar degrees of freedom, only allowed in quasicrystals but forbidden in conventional crystals. For both Kramers and non-Kramers doublets, the characteristics of multipoles are classified and the effective spin Hamiltonian on symmetry grounds are derived. Based on the self-similar triangular structure of the icosahedron, we argue the long-range frustration in terms of the Ising model. We further classify the possible quantum phases including quantum fluctuations, in terms of the instantaneous entanglement generation of the ground state. Our study offers the magnetic icosahedral quasicrystal as a new platform to search for the novel multipolar degrees of freedom and their exotic phenomena.Comment: 17 pages, 10 figure