Effects of Different Quantum Coherence on the Pump–Probe Polarization Anisotropy of Photosynthetic Light-Harvesting Complexes: A Computational Study

2015 ◽  
Vol 6 (10) ◽  
pp. 1954-1960 ◽  
Author(s):  
Shuming Bai ◽  
Kai Song ◽  
Qiang Shi
Keyword(s):  
Quantum Coherence ◽  
Light Harvesting ◽  
Computational Study ◽  
Polarization Anisotropy ◽  
Light Harvesting Complexes ◽  
Pump Probe

scholarly journals Local quantum uncertainty as a robust metric to characterize discord-like quantum correlations in subsets of the chromophores in photosynthetic light-harvesting complexes

2020 ◽  
Vol 66 (4 Jul-Aug) ◽  
pp. 525
Author(s):  
M. Chávez-Huerta ◽  
F. Rojas
Keyword(s):  
Quantum Coherence ◽  
Light Harvesting ◽  
Green Sulfur Bacteria ◽  
Quantum Correlations ◽  
Light Harvesting Complexes ◽  
Thermal Equilibrium State ◽  
Light Harvesting Complex ◽  
Quantum Uncertainty ◽  
Local Quantum Uncertainty ◽  
Local Quantum

Green sulfur bacteria is a photosynthetic organism whose light-harvesting complex accommodates a pigment-protein complex called Fenna-Matthews-Olson (FMO). The FMO complex sustains quantum coherence and quantum correlations between the electronic states of spatially separated pigment molecules as energy moves with nearly a 100% quantum efficiency to the reaction center. We present a method based on the quantum uncertainty associated to local measurements to quantify discord-like quantum correlations between two subsystems where one is a qubit and the other is a qudit. We implement the method by calculating local quantum uncertainty (LQU), concurrence, and coherence between subsystems of pure and mixed states represented by the eigenstates and by the thermal equilibrium state determined by the FMO Hamiltonian. Three partitions of the seven chromophores network define the subsystems: one chromophore with six chromophores, pairs of chromophores, and one chromophore with two chromophores. Implementation of the LQU approach allows us to characterize quantum correlations that had not been studied before, identify the most quantum correlated subsets of chromophores, and determine that, in the strongest associations of chromophores, the LQU is a monotonically increasing function of the coherence.

scholarly journals Analysis of Photosynthetic Systems and Their Applications with Mathematical and Computational Models

2020 ◽  
Vol 10 (19) ◽  
pp. 6821
Author(s):  
Shyam Badu ◽  
Roderick Melnik ◽  
Sundeep Singh
Keyword(s):  
Quantum Coherence ◽  
Density Functional ◽  
Computational Models ◽  
Environmental Science ◽  
Light Harvesting ◽  
Green Sulfur Bacteria ◽  
Theoretical Background ◽  
Light Harvesting Complexes ◽  
Chlorophyll Pigments ◽  
Potential Applications

In biological and life science applications, photosynthesis is an important process that involves the absorption and transformation of sunlight into chemical energy. During the photosynthesis process, the light photons are captured by the green chlorophyll pigments in their photosynthetic antennae and further funneled to the reaction center. One of the most important light harvesting complexes that are highly important in the study of photosynthesis is the membrane-attached Fenna–Matthews–Olson (FMO) complex found in the green sulfur bacteria. In this review, we discuss the mathematical formulations and computational modeling of some of the light harvesting complexes including FMO. The most recent research developments in the photosynthetic light harvesting complexes are thoroughly discussed. The theoretical background related to the spectral density, quantum coherence and density functional theory has been elaborated. Furthermore, details about the transfer and excitation of energy in different sites of the FMO complex along with other vital photosynthetic light harvesting complexes have also been provided. Finally, we conclude this review by providing the current and potential applications in environmental science, energy, health and medicine, where such mathematical and computational studies of the photosynthesis and the light harvesting complexes can be readily integrated.

scholarly journals Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

2017 ◽  
Vol 114 (32) ◽  
pp. 8493-8498 ◽  
Author(s):  
Hong-Guang Duan ◽  
Valentyn I. Prokhorenko ◽  
Richard J. Cogdell ◽  
Khuram Ashraf ◽  
Amy L. Stevens ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Quantum Coherence ◽  
Light Harvesting ◽  
Electronic Excitation Energy ◽  
Light Harvesting Complexes ◽  
Ultrafast Optical ◽  
Ultrafast Optical Spectroscopy ◽  
Biomolecular Complexes ◽  
Orthodox View

During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is commonly rationalized in terms of excitons moving on a grid of biomolecular chromophores on typical timescales <100 fs. Today’s understanding of the energy transfer includes the fact that the excitons are delocalized over a few neighboring sites, but the role of quantum coherence is considered as irrelevant for the transfer dynamics because it typically decays within a few tens of femtoseconds. This orthodox picture of incoherent energy transfer between clusters of a few pigments sharing delocalized excitons has been challenged by ultrafast optical spectroscopy experiments with the Fenna–Matthews–Olson protein, in which interference oscillatory signals up to 1.5 ps were reported and interpreted as direct evidence of exceptionally long-lived electronic quantum coherence. Here, we show that the optical 2D photon echo spectra of this complex at ambient temperature in aqueous solution do not provide evidence of any long-lived electronic quantum coherence, but confirm the orthodox view of rapidly decaying electronic quantum coherence on a timescale of 60 fs. Our results can be considered as generic and give no hint that electronic quantum coherence plays any biofunctional role in real photoactive biomolecular complexes. Because in this structurally well-defined protein the distances between bacteriochlorophylls are comparable to those of other light-harvesting complexes, we anticipate that this finding is general and directly applies to even larger photoactive biomolecular complexes.

scholarly journals Artificial quantum photosynthetic materials

2021 ◽  
Author(s):  
James Quach ◽  
Sabrina L. Slimani ◽  
Roman Kostecki ◽  
Ahmed Nuri Kursunlu ◽  
Tak W. Kee ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Quantum Coherence ◽  
Transient Absorption ◽  
Light Harvesting ◽  
Resonance Energy Transfer ◽  
Resonance Energy ◽  
Photon Absorption ◽  
Light Harvesting Complexes ◽  
Classical Energy ◽  
Artificial Photosynthetic

Photosynthesis has been shown to be a highly efficient process for energy transfer in plants and bacteria. It has been proposed that quantum mechanics plays a key role in this energy transfer process. There has been evidence that photosynthetic systems may exhibit quantum coherence. As artificial light-harvesting complexes have been proposed to mimic photosynthesis, it is prudent that artificial photosynthetic materials should also be tested for quantum coherence. To date, such studies have not been reported. In this work, we examine one such system, the BODIPY light harvesting complex (LHC), which has been shown to exhibit classical energy transfer via Förster resonance energy transfer. We compare the photon absorption of the LHC with the BODIPY chromophore by performing UV-visible, transient absorption, broadband pump-probe (BBPP) and two-dimensional electronic (2DES) spectroscopy. The 2DES and BBPP show evidence for quantum coherence, with oscillation frequencies of 100 cm-1 and 600 cm-1, which are attributable to vibronic, or exciton-phonon type coupling. Further computational analysis suggests strong couplings of the molecular orbitals of the LHC resulting from the stacking of neighbouring BODIPY chromophore units may contribute to undesirable hypochromic effects .

scholarly journals How Static Disorder Mimics Decoherence in Anisotropy Pump–Probe Experiments on Purple-Bacteria Light Harvesting Complexes

2016 ◽  
Vol 120 (44) ◽  
pp. 11449-11463 ◽  
Author(s):  
Clement Stross ◽  
Marc W. Van der Kamp ◽  
Thomas A. A. Oliver ◽  
Jeremy N. Harvey ◽  
Noah Linden ◽  
...  
Keyword(s):  
Light Harvesting ◽  
Purple Bacteria ◽  
Static Disorder ◽  
Light Harvesting Complexes ◽  
Pump Probe
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