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International Journal of Quantum Chemistry

Quantum nonlocality in the excitation energy transfer in the F enna– M atthews– O lson complex

Charlotta Bengtson, Michael Stenrup, Erik Sjöqvist

Published Sep 8, 2016• 5 citations
Publisher

Abstract

Abstract The Fenna–Matthews–Olson (FMO) complex—a pigment protein complex involved in photosynthesis in green sulfur bacteria—is remarkably efficient in transferring excitation energy from light harvesting antenna molecules to a reaction center. Recent experimental and theoretical studies suggest that quantum coherence and entanglement may play a role in this excitation energy transfer (EET). We examine whether bipartite quantum nonlocality, a property that expresses a stronger‐than‐entanglement form of correlation, exists between different pairs of chromophores in the FMO complex when modeling the EET by the hierarchically coupled equations of motion method. We compare the results for nonlocality with the amount of bipartite entanglement in the system. In particular, we analyze in what way these correlation properties are affected by different initial conditions. It is found that bipartite nonlocality only exists when the initial conditions are chosen in an unphysiological manner and probably is absent when considering the EET in the FMO complex in its natural habitat. It is also seen that nonlocality and entanglement behave quite differently in this system. In particular, for localized initial states, nonlocality only exists on a very short time scale and then drops to zero in an abrupt manner. As already known from previous studies, quantum entanglement between chromophore pairs, on the other hand, is oscillating and exponentially decaying and follow thereby a pattern more similar to the chromophore population dynamics. The abrupt disappearance of nonlocality in the presence of nonvanishing entanglement is a phenomenon we call nonlocality sudden death; a striking manifestation of the difference between these two types of correlations in quantum systems.

DOI
10.1002/qua.25221

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The Fenna-Matthews-Olson (FMO) complex - a pigment protein complex involved in photosynthesis in green sulfur bacteria - is remarkably efficient in transferring excitation energy from light harvesting antenna molecules to a reaction center. Recent experimental and theoretical studies suggest that quantum coherence and entanglement may play a role in this excitation energy transfer (EET). We examine whether bipartite quantum nonlocality, a property that expresses a stronger-than-entanglement form of correlation, exists between different pairs of chromophores in the FMO complex when modeling the EET by the hierarchically coupled equations of motion method. We compare the results for nonlocality with the amount of bipartite entanglement in the system. In particular, we analyze in what way these correlation properties are affected by different initial conditions. It is found that bipartite nonlocality only exists when the initial conditions are chosen in an unphysiological manner and probably is absent when considering the EET in the FMO complex in its natural habitat. It is also seen that nonlocality and entanglement behave quite differently in this system. In particular, for localized initial states, nonlocality only exists on a very short time scale and then drops to zero in an abrupt manner. As already known from previous studies, quantum entanglement between chromophore pairs on the other hand is oscillating and exponentially decaying and follow thereby a pattern more similar to the chromophore population dynamics. The abrupt disappearance of nonlocality in the presence of nonvanishing entanglement is a phenomenon we call nonlocality sudden death; a striking manifestation of the difference between these two types of correlations in quantum systems.

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A study published on arXiv has strictly demonstrated the existence of true multipartite quantum entanglement between bacteriochlorophyll-a (BChl a) molecules within the Fenna-Matthews-Olson (FMO) light-harvesting complex of green sulfur bacteria. Using entanglement measures in the single-excitation subspace (bipartite concurrence and a global entanglement measure), the study proved for the first time in a biological system that these entanglement states persist for approximately 2 picoseconds (ps) not only at cryogenic temperatures but also at physiological temperatures (300 K, room temperature), surviving macroscopically. The findings suggest that strong quantum entanglement between distant molecules can enhance the robustness and efficiency of the energy transfer network as the exciton moves toward the reaction center, even amidst environmental noise (decohering effects). [Quantum Biology Society] Photosynthesis, known as one of the most efficient energy conversion processes in nature, has long been a subject of wonder for scientists. While previous research focused on quantum coherence at the single-particle level, a groundbreaking study has recently been published mathematically proving that "true quantum entanglement"—the non-local correlation between multiple pigment molecules—actually operates within living organisms, drawing global attention. The paper titled "Quantum entanglement in photosynthetic light harvesting complexes," published in the preprint repository arXiv, is evaluated as a monumental achievement in elucidating macroscopic quantum phenomena in biological systems. An international joint research team led by Mohan Sarovar, Akihito Ishizaki, Graham R. Fleming, and K. Birgitta Whaley from UC Berkeley and Lawrence Berkeley National Laboratory (LBNL) in the USA spearheaded this innovative research. ■ Demonstration of Multipartite Quantum Entanglement within the FMO Complex The researchers focused on the FMO (Fenna-Matthews-Olson) light-harvesting complex of green sulfur bacteria (Chlorobium tepidum). By precisely analyzing the exciton dynamics between the pigment molecules within the complex using a non-Markovian quantum master equation, they proved through bipartite concurrence and a measure of global entanglement that true multipartite quantum entanglement is formed, going beyond simple individual coherence. This marks the first rigorous instance of quantifying quantum entanglement in a biological system. ■ Quantum Information Maintained Through Room-Temperature Noise The most surprising discovery is that these delicate quantum entanglement states survive meaningfully even at warm and wet physiological temperatures. While it was generally thought that quantum states are instantly destroyed by the thermal fluctuations of the surrounding proteins and solvent (decohering effects), the study's results confirmed that the natural FMO complex maintains bipartite entanglement between dimerized pigments and even a small amount of long-range and multipartite entanglement at 300 K. This entanglement plays a crucial role in enhancing the efficiency and robustness of the energy transfer network as the exciton travels to the reaction center. ■ Living Organisms as Optimized Quantum Machines This study suggests that living organisms are not merely losing quantum phenomena in harsh environmental noise but are rather highly designed, optimized quantum machines that endure and actively utilize them. Mimicking these perfect energy transfer mechanisms of nature is expected to provide key physical clues for maximizing the efficiency of next-generation solar cells or developing innovative quantum communication and metrology devices that operate robustly even at room temperature. https://arxiv.org/abs/0905.3787

•Jul 13, 2026•0 citations
Abstract The Fenna–Matthews–Olson (FMO) complex—a pigment protein complex involved in photosynthesis in green sulfur bacteria—is remarkably efficient in transferring excitation energy from light harvesting antenna molecules to a reaction center. Recent experimental and theoretical studies suggest that quantum coherence and entanglement may play a role in this excitation energy transfer (EET). We examine whether bipartite quantum nonlocality, a property that expresses a stronger‐than‐entanglement form of correlation, exists between different pairs of chromophores in the FMO complex when modeling the EET by the hierarchically coupled equations of motion method. We compare the results for nonlocality with the amount of bipartite entanglement in the system. In particular, we analyze in what way these correlation properties are affected by different initial conditions. It is found that bipartite nonlocality only exists when the initial conditions are chosen in an unphysiological manner and probably is absent when considering the EET in the FMO complex in its natural habitat. It is also seen that nonlocality and entanglement behave quite differently in this system. In particular, for localized initial states, nonlocality only exists on a very short time scale and then drops to zero in an abrupt manner. As already known from previous studies, quantum entanglement between chromophore pairs, on the other hand, is oscillating and exponentially decaying and follow thereby a pattern more similar to the chromophore population dynamics. The abrupt disappearance of nonlocality in the presence of nonvanishing entanglement is a phenomenon we call nonlocality sudden death; a striking manifestation of the difference between these two types of correlations in quantum systems.
The Fenna-Matthews-Olson (FMO) complex - a pigment protein complex involved in photosynthesis in green sulfur bacteria - is remarkably efficient in transferring excitation energy from light harvesting antenna molecules to a reaction center. Recent experimental and theoretical studies suggest that quantum coherence and entanglement may play a role in this excitation energy transfer (EET). We examine whether bipartite quantum nonlocality, a property that expresses a stronger-than-entanglement form of correlation, exists between different pairs of chromophores in the FMO complex when modeling the EET by the hierarchically coupled equations of motion method. We compare the results for nonlocality with the amount of bipartite entanglement in the system. In particular, we analyze in what way these correlation properties are affected by different initial conditions. It is found that bipartite nonlocality only exists when the initial conditions are chosen in an unphysiological manner and probably is absent when considering the EET in the FMO complex in its natural habitat. It is also seen that nonlocality and entanglement behave quite differently in this system. In particular, for localized initial states, nonlocality only exists on a very short time scale and then drops to zero in an abrupt manner. As already known from previous studies, quantum entanglement between chromophore pairs on the other hand is oscillating and exponentially decaying and follow thereby a pattern more similar to the chromophore population dynamics. The abrupt disappearance of nonlocality in the presence of nonvanishing entanglement is a phenomenon we call nonlocality sudden death; a striking manifestation of the difference between these two types of correlations in quantum systems.
The Fenna-Matthews-Olson (FMO) complex - a pigment protein complex involved in photosynthesis in green sulfur bacteria - is remarkably efficient in transferring excitation energy from light harvesting antenna molecules to a reaction center. Recent experimental and theoretical studies suggest that quantum coherence and entanglement may play a role in this excitation energy transfer (EET). We examine whether bipartite quantum nonlocality, a property that expresses a stronger-than-entanglement form of correlation, exists between different pairs of chromophores in the FMO complex when modeling the EET by the hierarchically coupled equations of motion method. We compare the results for nonlocality with the amount of bipartite entanglement in the system. In particular, we analyze in what way these correlation properties are affected by different initial conditions. It is found that bipartite nonlocality only exists when the initial conditions are chosen in an unphysiological manner and probably is absent when considering the EET in the FMO complex in its natural habitat. It is also seen that nonlocality and entanglement behave quite differently in this system. In particular, for localized initial states, nonlocality only exists on a very short time scale and then drops to zero in an abrupt manner. As already known from previous studies, quantum entanglement between chromophore pairs on the other hand is oscillating and exponentially decaying and follow thereby a pattern more similar to the chromophore population dynamics. The abrupt disappearance of nonlocality in the presence of nonvanishing entanglement is a phenomenon we call nonlocality sudden death; a striking manifestation of the difference between these two types of correlations in quantum systems.
We study the evolution of quantum entanglement during exciton energy transfer (EET) in a network model of the Fenna-Matthews-Olson (FMO) complex, a biological pigment-protein complex involved in the early steps of photosynthesis in sulfur bacteria. The influence of Markovian as well as spatially and temporally correlated (non-Markovian) noise on the generation of entanglement across distinct chromophores (site entanglement) and different excitonic eigenstates (mode entanglement) is studied for different injection mechanisms, including thermal and coherent laser excitation. Additionally, we study the entangling power of the FMO complex under natural operating conditions. While quantum information processing tends to favor maximal entanglement, near unit EET is achieved as the result of an intricate interplay between coherent and noisy processes where the initial part of the evolution displays intermediate values of both forms of entanglement.
Abstract The Fenna-Matthews-Olson light-harvesting complexes have become a center of attention due to their high excitation energy transfer efficiency, which may surpass 98%. Experimental results reveal the presence of quantum entanglement in the protein structure, which seems to be associated to such a remarkably high efficiency. Notably, Redfield and Lindblad master equations have been already used to model the chromophore excitation in the protein complex as well as its interactions with the environment. The entanglement arising during the process has been quantified through several measures. This work provides a short review of methods used to model the above described system. It is also discussed the introduction of two nonconventional measures addresed to quantify the emergent entanglement.
Recent evidence of electronic coherence during energy transfer in photosynthetic antenna complexes has reinvigorated the discussion about whether coherence and/or entanglement have any practical functionality for these molecular systems. Here we investigate quantitative relationships between the quantum yield of a light-harvesting complex and the distribution of entanglement among its components. Our study focuses on the entanglement yield or average entanglement surviving a time scale comparable to the average excitation trapping time. We consider the Fenna–Matthews–Olson (FMO) protein of green sulfur bacteria as a prototype system and show that there is an inverse relationship between the quantum efficiency and the average entanglement between distant donor sites. Our results suggest that long-lasting electronic coherence among distant donors might help in the modulation of the light-harvesting function.
A study published on arXiv has strictly demonstrated the existence of true multipartite quantum entanglement between bacteriochlorophyll-a (BChl a) molecules within the Fenna-Matthews-Olson (FMO) light-harvesting complex of green sulfur bacteria. Using entanglement measures in the single-excitation subspace (bipartite concurrence and a global entanglement measure), the study proved for the first time in a biological system that these entanglement states persist for approximately 2 picoseconds (ps) not only at cryogenic temperatures but also at physiological temperatures (300 K, room temperature), surviving macroscopically. The findings suggest that strong quantum entanglement between distant molecules can enhance the robustness and efficiency of the energy transfer network as the exciton moves toward the reaction center, even amidst environmental noise (decohering effects). [Quantum Biology Society] Photosynthesis, known as one of the most efficient energy conversion processes in nature, has long been a subject of wonder for scientists. While previous research focused on quantum coherence at the single-particle level, a groundbreaking study has recently been published mathematically proving that "true quantum entanglement"—the non-local correlation between multiple pigment molecules—actually operates within living organisms, drawing global attention. The paper titled "Quantum entanglement in photosynthetic light harvesting complexes," published in the preprint repository arXiv, is evaluated as a monumental achievement in elucidating macroscopic quantum phenomena in biological systems. An international joint research team led by Mohan Sarovar, Akihito Ishizaki, Graham R. Fleming, and K. Birgitta Whaley from UC Berkeley and Lawrence Berkeley National Laboratory (LBNL) in the USA spearheaded this innovative research. ■ Demonstration of Multipartite Quantum Entanglement within the FMO Complex The researchers focused on the FMO (Fenna-Matthews-Olson) light-harvesting complex of green sulfur bacteria (Chlorobium tepidum). By precisely analyzing the exciton dynamics between the pigment molecules within the complex using a non-Markovian quantum master equation, they proved through bipartite concurrence and a measure of global entanglement that true multipartite quantum entanglement is formed, going beyond simple individual coherence. This marks the first rigorous instance of quantifying quantum entanglement in a biological system. ■ Quantum Information Maintained Through Room-Temperature Noise The most surprising discovery is that these delicate quantum entanglement states survive meaningfully even at warm and wet physiological temperatures. While it was generally thought that quantum states are instantly destroyed by the thermal fluctuations of the surrounding proteins and solvent (decohering effects), the study's results confirmed that the natural FMO complex maintains bipartite entanglement between dimerized pigments and even a small amount of long-range and multipartite entanglement at 300 K. This entanglement plays a crucial role in enhancing the efficiency and robustness of the energy transfer network as the exciton travels to the reaction center. ■ Living Organisms as Optimized Quantum Machines This study suggests that living organisms are not merely losing quantum phenomena in harsh environmental noise but are rather highly designed, optimized quantum machines that endure and actively utilize them. Mimicking these perfect energy transfer mechanisms of nature is expected to provide key physical clues for maximizing the efficiency of next-generation solar cells or developing innovative quantum communication and metrology devices that operate robustly even at room temperature. https://arxiv.org/abs/0905.3787