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Multicolor Quantum Control for Suppressing Ground State Coherences in Two-Dimensional Electronic Spectroscopy.

J Lim1, C M Bösen1, A D Somoza1

  • 1Institut für Theoretische Physik and IQST, Albert-Einstein-Allee 11, Universität Ulm, 89081 Ulm, Germany.

Physical Review Letters
|December 24, 2019
PubMed
Summary
This summary is machine-generated.

This study introduces a novel coherent control scheme to isolate excited-state coherences in light-harvesting complexes. This method enhances the analysis of energy transfer dynamics in complex biological systems.

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Area of Science:

  • Quantum Biology
  • Spectroscopy
  • Photochemistry

Background:

  • Light-harvesting complexes exhibit oscillatory spectral features suggesting coherent energy transfer.
  • Isolating excited-state coherences in congested spectra is a significant experimental challenge.

Purpose of the Study:

  • To develop a coherent control scheme for suppressing ground-state coherences.
  • To enable rephasing spectra dominated by excited-state coherences for clearer analysis.
  • To advance the understanding of energy transfer in complex biological systems.

Main Methods:

  • Implementation of a novel coherent control scheme.
  • Suppression of ground-state coherences.
  • Analysis using a model dimeric system and numerically exact methods.

Main Results:

  • Demonstrated suppression of ground-state coherences.
  • Achieved rephasing spectra dominated by excited-state coherences.
  • Provided a benchmark for the developed coherent control scheme.

Conclusions:

  • The developed scheme facilitates rigorous inference of coherent energy transfer.
  • Combining temporal and spectral control methods can lead to advanced experimental techniques.
  • Significant advancement in understanding complex open many-body structure and dynamics is anticipated.