Generalized Optical Sum Rules for Light-Dressed Matter.

Light-driven matter can exhibit qualitatively distinct electronic and optical properties from those observed at equilibrium. We introduce generalized sum rules for the optical properties of light-driven molecules. Both classical and quantum light are considered. For classical light, the Floquet sum rules show that the sum of all Fourier components, indexed by n = - ∞ to ∞ , of the time-dependent dipole matrix elements between Floquet modes weighted by the corresponding quasienergy difference in the first Floquet Brillouin zone plus n driving frequency is a constant. Surprisingly, it is impossible to alter the energy exchange rate between matter and a perturbative external probe laser by a strong driving, even though the spectra can differ significantly from the bare ones. These developments provide guidance for the control of effective optical properties of matter by light fields.