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The spin state of an NMR-active nucleus can have a slight effect on its immediate electronic environment. This effect propagates through the intervening bonds and affects the electronic environments of NMR-active nuclei up to three bonds away; occasionally, even farther. This phenomenon is called spin–spin coupling or J-coupling. Coupling interactions are mutual and result in small changes in the absorption frequencies of both nuclei involved. While nuclei of the same element are involved...
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In Ultraviolet–Visible (UV–Vis) spectroscopy, the absorption of electromagnetic radiation is used to probe the electronic structure of molecules. This technique provides insights into molecular electronic transitions, particularly the movement of electrons between different molecular orbitals. Radiation is absorbed if the energy of the electromagnetic radiation passing through the molecule is precisely equal to the energy difference between the excited and ground states. During this...
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The coupling interactions of nuclei across four or more bonds are usually weak, with J values less than 1 Hz. While these are usually not observed in spectra, the presence of multiple bonds along the coupling pathway can result in observable long-range coupling.
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When Infrared (IR) radiation passes through a covalently bonded molecule, the bonds transition from lower to higher vibrational levels. The fundamental vibrational motions that result in infrared absorption can be classified as stretching or bending vibrations.
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Spin systems where the difference in chemical shifts of the coupled nuclei is greater than ten times J are called first-order spin systems. These nuclei are weakly coupled, and their chemical shifts and coupling constant can generally be estimated from the well-separated signals in the spectrum.
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Probing intramolecular vibronic coupling through vibronic-state imaging.

Fan-Fang Kong1, Xiao-Jun Tian1, Yang Zhang2,3

  • 1Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui, China.

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We visualized vibronic coupling in single pentacene molecules using electroluminescence. A 90° rotation in transition dipole orientation reveals strong Herzberg-Teller effects beyond the Franck-Condon model.

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Area of Science:

  • Molecular Spectroscopy
  • Quantum Chemistry
  • Surface Science

Background:

  • Vibronic coupling is fundamental to understanding molecular spectroscopy.
  • The Franck-Condon model is the conventional approach, but often insufficient.
  • Advanced imaging techniques are needed to probe these effects at the single-molecule level.

Purpose of the Study:

  • To investigate vibronic coupling in a single pentacene molecule in real space.
  • To visualize the spatial distribution of single-molecule electroluminescence.
  • To explore beyond the conventional Franck-Condon picture.

Main Methods:

  • Highly localized excitation of tunneling electrons.
  • Controlled plasmonic junction.
  • Imaging of single-molecule electroluminescence.

Main Results:

  • Observed a two-spot orientation for certain vibronic-state imaging, rotated 90° from the electronic transition.
  • This rotation indicates a change in transition dipole orientation from the short to the long molecular axis.
  • Demonstrated strong vibronic coupling with significant Herzberg-Teller contributions.

Conclusions:

  • The findings reveal strong vibronic coupling beyond the Franck-Condon approximation.
  • Vibration-induced transition charges along the long axis originate from dynamic perturbation of anti-symmetric vibrations.
  • This study provides new insights into electron-vibration interactions in organic molecules.