Few-photon coherent nonlinear optics with a single molecule

We model single photon nonlinearities resulting from the dipole-dipole interactions of cold polar molecules. We propose utilizing ``dark state polaritons'' to effectively couple photon and molecular states; through this framework, coherent control of the nonlinearity can be expressed and potentially used in an optical quantum computation architecture. Due to the dipole-dipole interaction the photons pick up a measurable nonlinear phase even in the single photon regime. A mani...

We investigate a nonlinear localization microscopy method based on Rabi oscillations of single emitters. We demonstrate the fundamental working principle of this new technique using a cryogenic far-field experiment in which subwavelength features smaller than $\lambda$/10 are obtained. Using Monte Carlo simulations, we show the superior localization accuracy of this method under realistic conditions and a potential for higher acquisition speed or a lower number of required ph...

We present a new scheme for performing optical spectroscopy on single molecules. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor ($\beta$) of 18% for the dye molecules doped in the organic crystal. Combination of extinction, fluorescence excitation and resonance fluorescence spectroscopy with microscopy provides high-resolution spatio-spectral access to a...

An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning....

Echo is a ubiquitous phenomenon found in many physical systems, ranging from spins in magnetic fields to particle beams in hadron accelerators. It is typically observed in inhomogeneously broadened ensembles of nonlinear objects, and is used to eliminate the effects of environmental-induced dephasing, enabling observation of proper, inherent object properties. Here, we report experimental observation of quantum wave packet echoes in a single isolated molecule. In contrast to ...

The unusual features of quantum mechanics are enabling the development of technologies not possible with classical physics. These devices utilize nonclassical phenomena in the states of atoms, ions, and solid-state media as the basis for many prototypes. Here we investigate molecular states as a distinct alternative. We demonstrate a memory for light based on storing photons in the vibrations of hydrogen molecules. The THz-bandwidth molecular memory is used to store 100-fs pu...

Realizing nonlinear coupling across space can enable new scientific and technological advances, including ultrafast operation and propagation of information in IR photonic circuitry, remote triggering or catalyzing of chemical reactions, and new platforms for quantum simulations with increased complexities. In this report, we show that ultrafast nonlinear couplings are achieved between polaritons residing in different cavities, in the mid-infrared (IR) regime, e.g. by pumping...

An outstanding goal in quantum optics is the realization of fast optical non-linearities at the single-photon level. Such non-linearities would allow for the realization of optical devices with new functionalities such as a single-photon switch/transistor or a controlled-phase gate, which could form the basis of future quantum optical technologies. While non-linear optics effects at the single-emitter level have been demonstrated in different systems, including atoms coupled ...

We present an experiment where a single molecule strongly affects the amplitude and phase of a laser field emerging from a subwavelength aperture. We achieve a visibility of -6% in direct and +10% in cross-polarized detection schemes. Our analysis shows that a close to full extinction should be possible using near-field excitation.

In the last decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction of polaritonic phenomena emerging in this light-matter interaction regime have proven to be difficult tasks. The challenge originates from the enormous number of degrees of freedom that need to be taken into account, both in the organic molecules and in their photonic environment. ...