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Area of Science:

  • Quantum dynamics
  • Molecular spectroscopy
  • Physical chemistry

Background:

  • Electronic and vibrational correlations are crucial for molecular dynamics and structure.
  • Experimentally probing these correlations, especially with quantum coherence selectivity, is challenging.

Purpose of the Study:

  • To demonstrate a novel method for probing correlations within the vibrational and electronic manifold with quantum coherence selectivity.
  • To simultaneously encode and measure vibrational-vibrational, electronic-vibrational, and electronic-electronic interactions.

Main Methods:

  • Measurement of a fully coherent four-dimensional spectrum.
  • Utilizing a combination of near-impulsive resonant and non-resonant excitation.
  • Achieving electronic and vibrational frequency resolution to isolate coherence pathways.

Main Results:

  • Successfully measured a fifth-order signal of a complex organic molecule in solution, free from lower-order contamination.
  • Isolated and assigned individual quantum coherence pathways.
  • Revealed the vibronic structure within a featureless 2D electronic spectrum.

Conclusions:

  • The developed method enables detailed study of electronic and vibrational correlations.
  • It is suitable for investigating quantum effects in systems with strong electron-phonon-vibration coupling, like photosynthetic complexes.