Enhanced Control of Single-Molecule Emission Frequency and Spectral Diffusion

Year: 2024

Authors: Duquennoy R., Landrieux S., De Bernardis D., Mony J., Colautti M., Jin L., Pernice W.H.P., Toninelli C.

Autors Affiliation: Natl Inst Opt CNR INO, I-50019 Sesto Fiorentino, Italy; European Lab Nonlinear Spect LENS, I-50019 Sesto Fiorentino, Italy; Univ Naples Federico II, Phys Dept, I-80126 Fuorigrotta, Italy; Univ Paris Saclay, Inst Opt, Lab Charles Fabry, CNRS,Grad Sch, F-91127 Palaiseau, France; Heidelberg Univ, Kirchhoff Inst Phys, D-69120 Heidelberg, Germany; Univ Munster, Inst Phys, D-48149 Munster, Germany.

Abstract: The Stark effect provides a powerful method to shift the spectra of molecules, atoms, and electronic transitions in general, becoming one of the simplest and most straightforward ways to tune the frequency of quantum emitters by means of a static electric field. At the same time, in order to reduce the emitter sensitivity to charge noise, inversion symmetric systems are typically designed, providing a stable emission frequency with a quadratic-only dependence on the applied field. However, such nonlinear behavior might be reflected in correlations between the tuning ability and unwanted spectral fluctuations. Here, we provide experimental evidence of this trend using molecular quantum emitters in the solid state cooled down to liquid helium temperatures. We finally combine the electric field generated by electrodes, which is parallel to the molecule’s induced dipole, with optically excite long-lived charge states acting in the perpendicular direction. Based on the anisotropy of the molecule’s polarizability, our two-dimensional control of the local electric field allows us not only to tune the emitter’s frequency but also to sensibly suppress the spectral instabilities associated with field fluctuations.

Journal/Review: ACS NANO

Volume: 18 (47)      Pages from: 32508  to: 32516

More Information: This work has been cofunded by the European Union – NextGeneration EU, Integrated infrastructure initiative in Photonic and Quantum Sciences – I-PHOQS [IR0000016, ID D2B8D520, CUP B53C22001750006]. The research has been cofunded by the EC under the F ET-OPEN- RIA project STORMYTUNE (G.A. 899587). It is also cofunded by the European Union (ERC, QUINTESSEnCE, 101088394). Views and opinions expressed are however those of the author(s) only and do not necessarily reflect those of the European Union or the European Research Council. Neither the European Union nor the granting authority can be held responsible for them. The authors wish to acknowledge Pietro Lombardi for advice on sample fabrication.
KeyWords: quantum emitters; spectral-diffusion control; Stark shift; singlemolecule; quantum technologies
DOI: 10.1021/acsnano.4c08382