scholarly journals Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Björn Kriete ◽  
Julian Lüttig ◽  
Tenzin Kunsel ◽  
Pavel Malý ◽  
Thomas L. C. Jansen ◽  
...  
Keyword(s):  
Energy Transport ◽  
Light Harvesting ◽  
Artificial Light ◽  
Light Harvesting Complex ◽  
Structural Hierarchy ◽  
Exciton Diffusion ◽  
Exciton Transfer ◽  
Exciton Transport ◽  
Photosynthetic Complexes ◽  
Shed Light

Abstract Unraveling the nature of energy transport in multi-chromophoric photosynthetic complexes is essential to extract valuable design blueprints for light-harvesting applications. Long-range exciton transport in such systems is facilitated by a combination of delocalized excitation wavefunctions (excitons) and exciton diffusion. The unambiguous identification of the exciton transport is intrinsically challenging due to the system’s sheer complexity. Here we address this challenge by employing a spectroscopic lab-on-a-chip approach: ultrafast coherent two-dimensional spectroscopy and microfluidics working in tandem with theoretical modeling. We show that at low excitation fluences, the outer layer acts as an exciton antenna supplying excitons to the inner tube, while under high excitation fluences the former converts its functionality into an exciton annihilator which depletes the exciton population prior to any exciton transfer. Our findings shed light on the excitonic trajectories across different sub-units of a multi-layered artificial light-harvesting complex and underpin their great potential for directional excitation energy transport.

scholarly journals Noise-Assisted Discord-Like Correlations in Light-Harvesting Photosynthetic Complexes

2021 ◽  
Vol 3 (2) ◽  
pp. 262-271
Author(s):  
Pablo Reséndiz-Vázquez ◽  
Ricardo Román-Ancheyta ◽  
Roberto León-Montiel
Keyword(s):  
Potential Role ◽  
Energy Transport ◽  
Light Harvesting ◽  
Quantum Correlations ◽  
Transport Processes ◽  
Quantum Evolution ◽  
Light Harvesting Complexes ◽  
Transport Efficiency ◽  
Photovoltaic Materials ◽  
Photosynthetic Complexes

Transport phenomena in photosynthetic systems have attracted a great deal of attention due to their potential role in devising novel photovoltaic materials. In particular, energy transport in light-harvesting complexes is considered quite efficient due to the balance between coherent quantum evolution and decoherence, a phenomenon coined Environment-Assisted Quantum Transport (ENAQT). Although this effect has been extensively studied, its behavior is typically described in terms of the decoherence’s strength, namely weak, moderate or strong. Here, we study the ENAQT in terms of quantum correlations that go beyond entanglement. Using a subsystem of the Fenna–Matthews–Olson complex, we find that discord-like correlations maximize when the subsystem’s transport efficiency increases, while the entanglement between sites vanishes. Our results suggest that quantum discord is a manifestation of the ENAQT and highlight the importance of beyond-entanglement correlations in photosynthetic energy transport processes.

Carotenoid deactivation in an artificial light-harvesting complex via a vibrationally hot ground state

2009 ◽  
Vol 357 (1-3) ◽  
pp. 181-187 ◽  
Author(s):  
Janne Savolainen ◽  
Tiago Buckup ◽  
Jürgen Hauer ◽  
Aliakbar Jafarpour ◽  
Carles Serrat ◽  
...  
Keyword(s):  
Ground State ◽  
Light Harvesting ◽  
Artificial Light ◽  
Light Harvesting Complex

scholarly journals Electronic coherence lifetimes of the Fenna–Matthews–Olson complex and light harvesting complex II

2019 ◽  
Vol 10 (45) ◽  
pp. 10503-10509 ◽  
Author(s):  
Shawn Irgen-Gioro ◽  
Karthik Gururangan ◽  
Rafael G. Saer ◽  
Robert E. Blankenship ◽  
Elad Harel
Keyword(s):  
Energy Transport ◽  
Light Harvesting ◽  
Light Harvesting Complex ◽  
Complex Ii ◽  
Efficient Energy ◽  
Naturally Occurring ◽  
Light Harvesting Complex Ii ◽  
Electronic Coherence ◽  
Excitonic States

The study of coherence between excitonic states in naturally occurring photosynthetic systems offers tantalizing prospects for uncovering mechanisms of efficient energy transport.

scholarly journals Controlling the efficiency of an artificial light-harvesting complex

2008 ◽  
Vol 105 (22) ◽  
pp. 7641-7646 ◽  
Author(s):  
J. Savolainen ◽  
R. Fanciulli ◽  
N. Dijkhuizen ◽  
A. L. Moore ◽  
J. Hauer ◽  
...  
Keyword(s):  
Light Harvesting ◽  
Artificial Light ◽  
Light Harvesting Complex

Research on Entanglement and Coherence in Light Harvesting Complex during Photosynthesis

2013 ◽  
Vol 641-642 ◽  
pp. 927-930
Author(s):  
Xing Yu Guan ◽  
J. Chee
Keyword(s):  
Energy Transport ◽  
Light Harvesting ◽  
Protein Complexes ◽  
Green Plant ◽  
Light Harvesting Complex ◽  
Transport Efficiency ◽  
The Past ◽  
Pigment Protein Complexes

Photosynthesis is a wonderful phenomenon which is present in green plant. In recent years, it has been discovered that there is entanglement in the biological pigment protein complexes, and that may be the reason of high transport efficiency. And coherence also plays an important role during the process of this efficiency energy transport. However, some scientists consider that it is not at all clear entanglement exists in the FMO complex, or unlike coherence, its role for the transport efficiency seems to be irrelevant. This paper mainly introduces what progress have scientists made during the past few years.

scholarly journals Fully Quantum Modeling of Exciton Diffusion in Mesoscale Light Harvesting Systems

Materials ◽  
2021 ◽  
Vol 14 (12) ◽  
pp. 3291
Author(s):  
Fulu Zheng ◽  
Lipeng Chen ◽  
Jianbo Gao ◽  
Yang Zhao
Keyword(s):  
Light Harvesting ◽  
Purple Bacteria ◽  
Time Dependent ◽  
Graphic Processing Units ◽  
Exciton Diffusion ◽  
Quantum Mechanical Treatment ◽  
Exciton Transfer ◽  
Harvesting Systems ◽  
Intractable Problem ◽  
Computational Resources

It has long been a challenge to accurately and efficiently simulate exciton–phonon dynamics in mesoscale photosynthetic systems with a fully quantum mechanical treatment due to extensive computational resources required. In this work, we tackle this seemingly intractable problem by combining the Dirac–Frenkel time-dependent variational method with Davydov trial states and implementing the algorithm in graphic processing units. The phonons are treated on the same footing as the exciton. Tested with toy models, which are nanoarrays of the B850 pigments from the light harvesting 2 complexes of purple bacteria, the methodology is adopted to describe exciton diffusion in huge systems containing more than 1600 molecules. The superradiance enhancement factor extracted from the simulations indicates an exciton delocalization over two to three pigments, in agreement with measurements of fluorescence quantum yield and lifetime in B850 systems. With fractal analysis of the exciton dynamics, it is found that exciton transfer in B850 nanoarrays exhibits a superdiffusion component for about 500 fs. Treating the B850 ring as an aggregate and modeling the inter-ring exciton transfer as incoherent hopping, we also apply the method of classical master equations to estimate exciton diffusion properties in one-dimensional (1D) and two-dimensional (2D) B850 nanoarrays using derived analytical expressions of time-dependent excitation probabilities. For both coherent and incoherent propagation, faster energy transfer is uncovered in 2D nanoarrays than 1D chains, owing to availability of more numerous propagating channels in the 2D arrangement.

Coherent control of the efficiency of an artificial light-harvesting complex

2009 ◽  
pp. 454-456
Author(s):  
Janne Savolainen ◽  
Riccardo Fanciulli ◽  
Niels Dijkhuizen ◽  
Ana L. Moore ◽  
Jürgen Hauer ◽  
...  
Keyword(s):  
Coherent Control ◽  
Light Harvesting ◽  
Artificial Light ◽  
Light Harvesting Complex

Macroorganisation and flexibility of thylakoid membranes

2019 ◽  
Vol 476 (20) ◽  
pp. 2981-3018 ◽  
Author(s):  
Petar H. Lambrev ◽  
Parveen Akhtar
Keyword(s):  
Light Harvesting ◽  
Current Knowledge ◽  
Three Dimensional ◽  
Photosynthetic Apparatus ◽  
Dynamic Responses ◽  
State Transitions ◽  
Photochemical Quenching ◽  
Light Harvesting Complex ◽  
Complex Ii ◽  
Light Harvesting Complex Ii

Abstract The light reactions of photosynthesis are hosted and regulated by the chloroplast thylakoid membrane (TM) — the central structural component of the photosynthetic apparatus of plants and algae. The two-dimensional and three-dimensional arrangement of the lipid–protein assemblies, aka macroorganisation, and its dynamic responses to the fluctuating physiological environment, aka flexibility, are the subject of this review. An emphasis is given on the information obtainable by spectroscopic approaches, especially circular dichroism (CD). We briefly summarise the current knowledge of the composition and three-dimensional architecture of the granal TMs in plants and the supramolecular organisation of Photosystem II and light-harvesting complex II therein. We next acquaint the non-specialist reader with the fundamentals of CD spectroscopy, recent advances such as anisotropic CD, and applications for studying the structure and macroorganisation of photosynthetic complexes and membranes. Special attention is given to the structural and functional flexibility of light-harvesting complex II in vitro as revealed by CD and fluorescence spectroscopy. We give an account of the dynamic changes in membrane macroorganisation associated with the light-adaptation of the photosynthetic apparatus and the regulation of the excitation energy flow by state transitions and non-photochemical quenching.

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