Laser-induced frequency tuning of Fourier-limited single-molecule emitters

Abstract

The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single molecule scale, how a focused laser beam can locally shift by hundreds-time their natural linewidth and in a persistent way the transition frequency of organic chromophores, cooled at liquid helium temperatures in different host matrices. Supported by quantum chemistry calculations, the results are interpreted as effects of a photo-ionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental method is then applied to a common challenge in quantum photonics, i.e. the independent tuning and synchronization of close-by quantum emitters, which is desirable for multi-photon experiments. Five molecules that are spatially separated by about 50 microns and originally 20 GHz apart are brought into resonance within twice their linewidth. Combining this ability with an emission linewidth that is only limited by the spontaneous decay, the system enables fabrication-free, independent tuning of multiple molecules integrated on the same photonic chip.

15 pages, 5 figures. Supplementary Informations 23 pages, 13 figures

References in corpus (8)

• On-line database of the spectral properties of polycyclic aromatic hydrocarbons
• Quantum Interference of Tunably Indistinguishable Photons from Remote Organic Molecules
• Turning a molecule into a coherent two-level quantum system
• Scalable in operando strain tuning in nanophotonic waveguides enabling three-quantum dot superradiance
• Controlling the phase of a light beam with a single molecule
• Electrical control of lifetime-limited quantum emitters using 2D materials
• Coherent coupling of single molecules to on-chip ring resonators
• In-situ tuning of individual position-controlled nanowire quantum dots via laser-induced intermixing