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Orbiting orbitals: visualization of vibronic motion at a conical intersection.

Joonhee Lee1, Shawn M Perdue, Alejandro Rodriguez Perez

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Summary

Scanning tunneling microscopy visualizes Jahn-Teller active electrons in metalloporphyrins. Vibronic motion dictates electron delocalization and molecular function, revealing Berry phase characteristics.

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Area of Science:

  • Surface Science
  • Quantum Chemistry
  • Molecular Imaging

Background:

  • Jahn-Teller (JT) distortions are crucial in molecules with degenerate electronic states.
  • Understanding electron delocalization in metalloporphyrins is key to their electronic properties.
  • Vibronic coupling influences molecular geometry and electronic behavior.

Purpose of the Study:

  • To image the Jahn-Teller active unpaired electron in single metalloporphyrin radical anions.
  • To elucidate the role of vibronic motion in electron delocalization and molecular shape.
  • To visualize the vibronic potential and reveal quantum mechanical phenomena like the Berry phase.

Main Methods:

  • High-resolution scanning tunneling microscopy (STM) was employed to image individual metalloporphyrin radical anions.
  • Analysis of topographic images and transformation of polar graphs were used to visualize electron coupling.
  • Quantum chemical calculations likely complemented the experimental imaging to interpret vibronic dynamics.

Main Results:

  • The unpaired electron was observed to be delocalized over the porphyrin macrocycle.
  • The electron's topographic image directly reflects vibronic motion, specifically the zero-point pseudorotation.
  • Visualization of the vibronic potential at the conical intersection revealed the Berry phase and half-integer angular momentum.

Conclusions:

  • Jahn-Teller dynamics exhibit remarkable economy, with small atomic displacements controlling electron motion and molecular function.
  • The electron's orbital adiabatically follows skeletal deformations, linking electronic structure to molecular geometry.
  • This study provides unprecedented visualization of electron-vibration coupling and its fundamental quantum mechanical consequences.