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Updated: Jul 6, 2025
06:08
Time-resolved Photophysical Characterization of Triplet-harvesting Organic Compounds at an Oxygen-free Environment Using an iCCD Camera
Published on: December 27, 2018
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Light-Harvesting Efficiency Cannot Depend on Optical Coherence in the Absence of Orientational Order
Dominic M Rouse1,2, Adesh Kushwaha3, Stefano Tomasi3
1School of Physics and Astronomy, University of Glasgow, Glasgow G12 8QQ, United Kingdom.
The Journal of Physical Chemistry Letters
|January 2, 2024
Summary
Optical coherence cannot enhance light-harvesting efficiency in molecular systems under weak light conditions. Coherent control is lost due to time-averaging and molecular disorder, limiting practical applications.
Area of Science:
- Quantum mechanics
- Photochemistry
- Biophysics
Background:
- Light-harvesting efficiency is crucial for biological and artificial systems.
- Optical coherence has been proposed as a quantum control mechanism to enhance this efficiency.
- Manipulating polarization or spectral phase are key methods for optical coherence control.
Purpose of the Study:
- To investigate the feasibility of using optical coherence for light-harvesting efficiency control.
- To determine the conditions under which coherent optical control is effective or ineffective.
- To clarify the role of molecular disorder and time-averaging in coherent control.
Main Methods:
- Theoretical analysis of light-harvesting systems.
- Examination of weak light conditions.
- Consideration of molecular systems with orientationally disordered subunits.
- Analysis of time scales longer than ultrafast.
Main Results:
- Optical coherence does not enhance light-harvesting efficiency in molecular systems under weak light.
- Coherent control is lost in disordered samples or when molecules reorient during light harvesting.
- Spectral-phase control is ineffective when efficiency is time-averaged over periods longer than optical coherence time.
Conclusions:
- Coherent optical control of light-harvesting efficiency is not universally applicable.
- Practical limitations like time-averaging and molecular disorder negate the benefits of optical coherence.
- Effective coherent control is restricted to systems with orientational order and relies solely on polarization control.
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