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Internal Stark effect of single-molecule fluorescence.

Kirill Vasilev¹, Benjamin Doppagne¹, Tomáš Neuman¹

¹Université de Strasbourg, CNRS, IPCMS, UMR 7504, F-67000, Strasbourg, France.

Nature Communications

|February 4, 2022

Summary

Researchers tuned chromophore optical properties using electrostatic fields at the single-molecule level. This study observed the internal Stark effect (ISE) by removing protons from phthalocyanine using a scanning tunneling microscope.

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Area of Science:

Physical Chemistry
Molecular Spectroscopy
Surface Science

Background:

Optical properties of chromophores are tunable via local electrostatic fields.
The internal Stark effect (ISE) is crucial for biological functions.
Previous studies lacked single-molecule resolution for ISE.

Purpose of the Study:

To investigate the internal Stark effect (ISE) at the single-molecule level.
To monitor Stark shifts induced by confined charges within a single chromophore.
To understand the influence of deprotonation on chromophore emission energy.

Main Methods:

Utilized a scanning tunneling microscope (STM) at cryogenic temperatures.
Deprotonated a single free-base phthalocyanine molecule on a Ag(111) surface with NaCl.
Measured STM-induced fluorescence spectra to detect spectral shifts.

Main Results:

Observed spectral shifts in fluorescence emission upon sequential proton removal.
Correlated these shifts with the electrostatic field generated by remaining charges.
Demonstrated single-molecule control over chromophore optical properties.

Conclusions:

Confirmed the feasibility of ISE experiments at the ultimate single-molecule scale.
Established a method for probing charge-induced optical property tuning.
Provided insights into electrostatic field effects on molecular emission.