Fundamental limitation of ultrastrong coupling between light and atoms

In a recent work of ours [Phys. Rev. Lett. 112, 073601 (2014)], we generalized the Power-Zineau-Woolley gauge to describe the electrodynamics of atoms in an arbitrary confined geometry. Here we complement the theory by proposing a tractable form of the polarization field to represent atomic material with well-defined intra-atomic potential. The direct electrostatic dipole-dipole interaction between the atoms is canceled. This theory yields a suitable framework to determine limitations on the light-matter coupling in quantum optical models with discernible atoms. We find that the superradiant criticality is at the border of covalent molecule formation and crystallization.