Singlet polaron theory of low-energy optical excitations in NiPS$_3$

Abstract

Light-matter interactions can be used as a tool to realize novel many-body states of matter and to study the interplay between electronic and magnetic degrees of freedom. In particular, tightly bound many-body states that behave as coherent quasi-particles are rare, and may lead to unconventional technological applications beyond the semi-conductor paradigm, particularly if these excitations are bosonic and can condense. Two-dimensional magnetic systems present a pristine platform to realize and study such states. We construct a theory that explains the low-energy optical excitations at 1.476 eV and 1.498 eV observed by photoluminiscence, optical absorption, and RIXS in the van der Waals antiferromagnet NiPS$_3$. Using \textit{ab initio} methods, we construct a two-band Hubbard model for two \textit{effective} Ni orbitals of the original lattice. The dominant effective hopping corresponds to third-nearest neighbours. This model exhibits two triplet-singlet excitations of energy near two times the Hund exchange. From perturbation theory, we obtain an effective model for the movement of the singlets in an antiferromagnetic background, that we solve using a generalized self-consistent Born approximation. These singlet excitations, dressed by a cloud of magnons, move coherently as polaronic-like quasi-particles, "singlet polarons". Our theory explains the main features of the observed spectra.