Abstract
Plants, algae, and photosynthetic bacteria use surprisingly sophisticated optimizations at the quantum mechanical level to harvest the sun's energy. The observation of coherence phenomena within light-harvesting complexes after short laser-pulse excitation has inspired advances in our understanding of light-harvesting optimization, highlighting the interplay of electronic excitations and vibrations. However, it remains unclear how these vibronic effects change or optimize the function of light-harvesting complexes—in other words, what is the design principle we could learn? Here, we use two-dimensional electronic spectroscopy to quantify the vibronic mixing among the light-absorbing molecules of a light-harvesting complex from cryptophyte algae. These data reveal a striking reallocation of absorption strength that, in turn, provides a robust increase in the rate of energy transfer of up to 3.5-fold. The realization of how absorption-strength redistribution, induced by vibronic coupling, provides a multiplicative increase in the rate of energy funneling establishes a bioinspired design principle for optimal light-harvesting systems.
Original language | English (US) |
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Pages (from-to) | 858-872 |
Number of pages | 15 |
Journal | Chem |
Volume | 1 |
Issue number | 6 |
DOIs | |
State | Published - Dec 8 2016 |
All Science Journal Classification (ASJC) codes
- General Chemistry
- Biochemistry
- Environmental Chemistry
- General Chemical Engineering
- Biochemistry, medical
- Materials Chemistry
Keywords
- cryptophyte algae
- light-harvesting complexes
- photosynthesis
- two-dimensional electronic spectroscopy
- ultrafast spectroscopy