Enhanced Control of Single-Molecule Emission Frequency and Spectral Diffusion

Area of Science:

• Quantum Optics
• Solid-State Spectroscopy
• Molecular Physics

Background:

• The Stark effect is a key method for tuning quantum emitter frequencies using static electric fields.
• Inversion-symmetric systems offer stable emission but exhibit quadratic field dependence, potentially linking tuning to spectral fluctuations.

Purpose of the Study:

• To experimentally investigate the correlation between spectral tuning and fluctuations in molecular quantum emitters.
• To demonstrate a method for simultaneously tuning emitter frequency and suppressing spectral instabilities.

Main Methods:

• Utilized molecular quantum emitters in a solid-state matrix cooled to liquid helium temperatures.
• Applied a two-dimensional electric field using electrodes, with one component parallel to the molecular dipole and another exciting perpendicular charge states.
• Leveraged the anisotropy of molecular polarizability for precise field control.

Main Results:

• Provided experimental evidence of the correlation between Stark tuning and spectral instabilities in molecular systems.
• Demonstrated that two-dimensional electric field control can effectively tune the emitter's frequency.
• Showed significant suppression of spectral instabilities associated with electric field fluctuations.

Conclusions:

• Two-dimensional electric field control offers a powerful approach for managing quantum emitter properties.
• This technique allows for simultaneous spectral tuning and stabilization, overcoming limitations of traditional Stark effect applications.