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The transport and capture of photo-induced electronic excitations is of fundamental interest to the design of energy efficient quantum technologies and to the study of potential quantum effects in biology. Using a simple quantum optical model, we examine the influence of coherence, entanglement, and cooperative dissipation on the transport and capture of excitation energy. We demonstrate that the rate of energy extraction is optimized under conditions that minimize the quantum coherence and entanglement of the system, which is a consequence of spontaneous parity time-reversal symmetry breaking. We then examine the effects of vibrational disorder and show that dephasing can be used to enhance the transport of delocalized excitations in settings relevant to biological photosynthesis. Our results highlight the rich, emergent behavior associated with the quantum-to-classical transition with relevance to the design of room-temperature quantum devices. Published by the American Physical Society2024
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Exciton-Condensate-Like Energy Transport in Light-Harvesting Complex 2
Bose-Einstein condensation of excitons, with its potential for frictionless energy transport, has recently been observed in materials at low temperatures. Here, we show that partial exciton condensation plays a significant role in the 18-chromophore B850 ring of the light-harvesting complex 2 (LH2) in purple bacteria. Even in the single-excitation regime, we observe that excitonic entanglement across multiple sites exhibits signatures of exciton condensation in the particle-hole reduced density matrix—a partial exciton condensate. Crucially, we find that, by distributing the exciton across multiple sites of the ring, the exciton-condensate-like state sets favorable conditions for enhanced energy transfer, both before and after decoherence. Surprisingly, this discovery reveals that excitonic condensation, previously thought to require extreme conditions, can occur in a partial form in biological systems under ambient conditions, providing new insight into energy transport. These results additionally bring new insight into the long-standing debate on quantum versus classical mechanisms in photosynthetic light harvesting by showing that quantum coherence, in the form of a partial exciton condensate, indirectly initializes subsequent classical transfer. Our findings not only deepen our understanding of quantum coherence in light harvesting but also suggest design principles for materials capable of leveraging excitonic entanglement for efficient energy transport. Published by the American Physical Society2025
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- PAR ID:
- 10591585
- Publisher / Repository:
- Knowledge @ UChicago
- Date Published:
- Journal Name:
- PRX Energy
- Volume:
- 4
- Issue:
- 1
- ISSN:
- 2768-5608
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1103/PRXEnergy.4.013004
