The pioneering experiments in linear spectroscopy were performed using flames in the 1800s, but nonlinear optical measurements had to wait until lasers became available in the twentieth century. Because the nonlinear cross-section of materials is very small(1,2), macroscopic bulk samples and pulsed lasers are usually used. Numerous efforts have explored coherent nonlinear signal generation from individual nanoparticles(3-5) or small atomic ensembles(6-8) with millions of atoms. Experiments on a single semiconductor quantum dot have also been reported, albeit with a very small yield(9). Here, we report the coherent nonlinear spectroscopy of a single molecule under continuous-wave single-pass illumination and the switching of a laser beam by on the order of ten pump photons. The sharp molecular transitions and efficient photon-molecule coupling at a tight focus(10) allow for optical switching with less than a handful of pump photons and are thus promising for applications in quantum engineering(11)

We propose a scheme enabling the universal coupling of angular momentum of N remote noninteracting qubits using linear optical tools only. Our system consists of N single-photon emitters in a Λ-configuration that are entangled among their long-lived ground-state qubits through suitably designed measurements of the emitted photons. In this manner, we present an experimentally feasible algorithm that is able to generate any of the 2 N symmetric and nonsymmetric total angular momentum eigenstates spanning the Hilbert space of the N -qubit compound.

We perform high-resolution spectroscopy and localization microscopy to study single dye molecules confined to nanoscopic dimensions in one direction. We provide the fabrication details of our nanoscopic glass channels and the procedure for filling them with organic matrices. Optical data on hundreds of molecules in different channel depths show a clear trend from narrow stable lines in deep channels to broader linewidths in ultrathin matrices. In addition, we observe a steady blue shift of the center of the inhomogeneous band as the channels become thinner. Furthermore, we use super-resolution localization microscopy to correlate the positions and orientations of the individual dye molecules with the lateral landscape of the organic matrix, including cracks and strain-induced dislocations. Our results and methodology are useful for a number of studies in various fields such as physical chemistry, solid-state spectroscopy, and quantum nano-optics.