Inducing Enantiosensitive Permanent Multipoles in Isotropic Samples with Two-Color Fields

Abstract

We find that two-color fields can induce field-free permanent dipoles in initially isotropic samples of chiral molecules via resonant electronic excitation in a one-$$3\omega $$ 3 ω -photon versus three-$$\omega $$ ω -photons scheme. These permanent dipoles are enantiosensitive and can be controlled via the relative phase between the two colors. When the two colors are linearly polarized perpendicular to each other, the interference between the two pathways induces excitation sensitive to the molecular handedness and orientation, leading to uniaxial orientation of the excited molecules and to an enantio-sensitive permanent dipole perpendicular to the polarization plane. We also find that although a corresponding one-$$2\omega $$ 2 ω -photon versus two-$$\omega $$ ω -photons scheme cannot produce enantiosensitive permanent dipoles, it can produce enantiosensitive permanent quadrupoles that are also controllable through the two-color relative phase.