Laser-Induced Frequency Tuning of Fourier-Limited Single-Molecule Emitters

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 of times their natural line width and, in a persistent way, the transition frequency of organic chromophores cooled at liquid helium temperature in different host matrices. Supported by quantum chemistry calculations, the results can be interpreted as effects of a photoionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental observation 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 multiphoton experiments. Five molecules that are spatially separated by about 50 μm and originally 20 GHz apart are brought into resonance within twice their line width. This tuning method, which does not require additional fabrication steps, is here independently applied to multiple emitters, with an emission line width that is only limited by the spontaneous decay and an inhomogeneous broadening limited to 1 nm. The system hence shows promise for photonic quantum technologies.