Long range dipole-dipole interaction in low-density atomic vapors probed by double-quantum two-dimensional coherent spectroscopy

Optical double-quantum two-dimensional coherent spectroscopy (2DCS) was implemented to probe interatomic dipole-dipole interactions in both potassium and rubidium atomic vapors. The dipole-dipole interaction was detected at densities of 4.81 × 108 cm−3 and 8.40 × 109 cm−3 for potassium and rubidium, respectively, corresponding to a mean interatomic separation of 15.8 µm or 3.0 × 105a0 for potassium and 6.1 µm or 1.2 × 105a0 for rubidium, where a0 is the Bohr radius. The experimental results confirm the long range nature of the dipole-dipole interaction, which is critical for understanding many-body physics in atoms/molecules. The long range interaction also has implications in atom-based applications involving many-body interactions. Additionally, we demonstrated that double-quantum 2DCS is sufficiently sensitive to probe dipole-dipole interaction at densities that can be achieved with cold atom in a magneto-optical trap, paving the way for double-quantum 2DCS studies of cold atoms and molecules. The method can also open a new avenue to study long-range interactions in solid state systems such as quantum dots and color centers in diamonds.