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Single-molecule tautomerization tracking through space- and time-resolved fluorescence spectroscopy.

Benjamin Doppagne1, Tomáš Neuman2, Ruben Soria-Martinez1

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Summary

Hydrogen atom tautomerization in phthalocyanine molecules was studied using scanning tunneling microscopy and fluorescence spectroscopy. This research reveals the molecular switching mechanism and its dependence on the atomic environment.

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Area of Science:

  • Molecular Physics
  • Surface Science
  • Spectroscopy

Background:

  • Tautomerization is a fundamental process in nature and chemistry, crucial for molecular switches.
  • Studying tautomerization in molecules like phthalocyanines requires advanced techniques to understand its mechanism.
  • Previous methods like optical spectroscopies and scanning probe microscopes offered limited combined insights.

Purpose of the Study:

  • To investigate the NH tautomerization in individual free-base phthalocyanine (H2Pc) molecules.
  • To combine scanning tunneling microscopy (STM) and fluorescence spectroscopy for atomic-scale insights.
  • To elucidate the role of the molecular environment and excited states in the tautomerization process.

Main Methods:

  • Utilized scanning tunneling microscopy (STM) and fluorescence spectroscopy on H2Pc molecules on a NaCl-covered Ag(111) surface.
  • Employed STM-induced fluorescence (STM-F) and hyper-resolved fluorescence maps (HRFMs).
  • Performed time-correlated fluorescence measurements and compared experimental data with simulations.

Main Results:

  • Identified distinct spectral features corresponding to two molecular tautomers of H2Pc.
  • Determined the orientation of molecular optical dipoles and the vibronic fingerprint of tautomers.
  • Monitored tautomerization events, linking proton dynamics to a switching two-level system.
  • Observed that tautomerization can occur via remote excitation, suggesting excited-state involvement.

Conclusions:

  • The combined STM and fluorescence approach provides unprecedented atomic-scale understanding of molecular tautomerization.
  • Minute environmental changes significantly influence the tautomerization process.
  • The excited state of the molecule plays a critical role in the tautomerization reaction pathway.