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Long-Lived Electronic Coherences in Molecules.

Brian Kaufman1, Philipp Marquetand2, Tamás Rozgonyi3

  • 1Department of Physics and Astronomy, Stony Brook University, Stony Brook, New York 11794-3800, USA.

Physical Review Letters
|January 12, 2024
PubMed
Summary
This summary is machine-generated.

We show that long-lived electronic coherences in molecules can be maintained using ultrafast laser pulses. These coherences persist even with complex molecular vibrations, impacting attosecond science and photochemistry.

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Area of Science:

  • Quantum dynamics
  • Molecular spectroscopy
  • Ultrafast laser science

Background:

  • Understanding electronic coherences is crucial for controlling molecular processes.
  • Vibrational motion often leads to rapid decoherence in molecules.

Purpose of the Study:

  • To demonstrate and characterize long-lived electronic coherences in molecules.
  • To investigate the survival of coherences between excited states.

Main Methods:

  • Utilizing shaped octave-spanning ultrafast laser pulses for pump-probe measurements.
  • Performing theoretical calculations of light-matter interactions.
  • Preparing and interrogating entangled nuclear-electronic wave packets.

Main Results:

  • Observed long-lived electronic coherences despite significant vibrational motion.
  • Demonstrated that coherences between excited states can persist after ground state coherence is lost.
  • Validated experimental findings with theoretical calculations.

Conclusions:

  • Long-lived electronic coherences are achievable and controllable in molecules.
  • Excited-state coherences offer a pathway for robust quantum phenomena in complex systems.
  • Findings have significant implications for attosecond science, photochemistry, and quantum information processing.