Nonlinear photon-atom coupling with 4Pi microscopy

Implementing nonlinear interactions between single photons and single atoms is at the forefront of optical physics. Motivated by the prospects of deterministic all-optical quantum logic, many efforts are currently underway to find suitable experimental techniques. Focusing the incident photons onto the atom with a lens yielded promising results, but is limited by diffraction to moderate interaction strengths. However, techniques to exceed the diffraction limit are known from high-resolution imaging. Here we adapt a super-resolution imaging technique, 4Pi microscopy, to efficiently couple light to a single atom. We observe 36.6(3)% extinction of the incident field, and a modified photon statistics of the transmitted field-indicating nonlinear interaction at the single-photon level. Our results pave the way to few-photon nonlinear optics with individual atoms in free space.