Elemental chalcogens as a minimal model for chiral charge and orbital order

Abstract

Helices of increased electron density can spontaneously form in materials containing multiple, interacting density waves. Although a macroscopic order parameter theory describing this behaviour has been proposed and experimentally tested, a detailed microscopic understanding of spiral electronic order in any particular material is still lacking. Here, we present the elemental chalcogens Selenium and Tellurium as model materials for the development of chiral charge and orbital order. We formulate minimal models capturing the formation of spiral structures both in terms of a macroscopic Landau theory and a microscopic Hamiltonian. Both reproduce the known chiral crystal structure and are consistent with its observed thermal evolution and behaviour under applied pressure. The combination of microscopic and macroscopic frameworks allows us to distil the essential ingredients in the emergence of helical charge order, and may serve as a guide to understanding spontaneous chirality both in other specific materials and throughout materials classes.