Coherence and population dynamics of chlorophyll excitations in FCP complex: Two-dimensional spectroscopy study

Butkus, Vytautas; Gelžinis, Andrius; Augulis, Ramu̅nas; Gall, Andrew; Büchel, Claudia; Robert, Bruno; Zigmantas, Donatas; Valkūnas, Leonas; Abramavičius, Darius

doi:10.1063/1.4914098

Cited by 34 publications

(52 citation statements)

References 62 publications

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“…The effect of the laser spectrum on coherences has been recently discussed in the literature, but the filtering effect was not discussed [48]. The selection of specific pathways through two-color experiments has also been described [49][50][51], but the concept that some vibronic signatures may be missing in one-color experiments, as described here, was previously only briefly noted by Butkus et al [52]. Recently, there have been efforts to model excitonic systems with the inclusion of vibrational coupling, giving rise to more complex energy level structures [53], which were experimentally verified in an artificial light harvesting complex whose structure proved especially convenient for rigorous polarization experiments [54].…”

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confidence: 85%

Resolving Vibrational from Electronic Coherences in Two-Dimensional Electronic Spectroscopy: The Role of the Laser Spectrum

et al. 2017

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The observation of coherent quantum effects in photosynthetic light-harvesting complexes prompted the question whether quantum coherence could be exploited to improve the efficiency in new energy materials. The detailed characterization of coherent effects relies on sensitive methods such as two-dimensional electronic spectroscopy (2D-ES). However, the interpretation of the results produced by 2D-ES is challenging due to the many possible couplings present in complex molecular structures. In this work, we demonstrate how the laser spectral profile can induce electronic coherencelike signals in monomeric chromophores, potentially leading to data misinterpretation. We argue that the laser spectrum acts as a filter for certain coherence pathways and thus propose a general method to differentiate vibrational from electronic coherences.

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confidence: 85%

Resolving Vibrational from Electronic Coherences in Two-Dimensional Electronic Spectroscopy: The Role of the Laser Spectrum

et al. 2017

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“…The evidence for essential quantum effects during photosynthesis has already been shown (Engel, 2007;Whaley, 2011, Butkus, 2015. The reason that efficiency of this process is so high in living plants, is that the entire process of transmitting solar energy inside the leafs takes place under the conditions in which the energy remains in a quantum state.…”

Section: Photosynthesismentioning

confidence: 98%

Quantum Wave Information of Life Revealed: An Algorithm for Electromagnetic Frequencies that Create Stability of Biological Order, With Implications for Brain Function and Consciousness

Geesink¹,

Meijer

2016

Neuroquantology

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We propose a hypothesis of a mathematical algorithm for coherent quantum frequencies, that may create stability of biological order. The concept is based on an extensive literature survey, comprising 175 articles from 1950 to 2015, dealing with effects of electromagnetic radiation on in vitro and in vivo life systems, indicating that typical discrete coherent frequencies of electromagnetic waves are able to stabilize cells, whereas others cause a clear destabilization. We find support for the hypothesis of H. Fröhlich, that a driven set of oscillators condenses in a broad energy range, may activate a vibrational mode in life organisms at room temperature. Taking into account the life sustaining frequencies, as extracted from literature, an algorithm of coherent frequencies of standing waves for the stability of biological order was inferred. Interestingly, we found that the origin of the particular biological algorithm can be mathematically approached by a selected "tempered Pythagorean" reference acoustic scale. The algorithm expresses one-dimensional wave equations known for vibrating strings. The origin of the biological algorithm was condensed in a mathematical expression, in which all frequencies have ratios of 1:2 and closely approach ratios of 2:3. This inferred algorithm was subsequently verified with regard to various frequencies of electromagnetic waves, as applied in the above-mentioned independent biological studies. It was also matched with a range of 23 different measured quantum resonances emitted by a selected inorganic silicate mineral, that is able to catalyze the oligomerization of RNA. The selected silicate was experimentally shown to act as a quantum replicator, specifically emitting EM radiation at frequencies that are fully in line with this algorithm. Such silicate quantum replicators, therefore may have been instrumental in the initiation of first replicating, life, cells at the edge of pre-biotic evolution. Our model may imply that, at the quantum scale, an underlying electromagnetically defined order may have been present, that was a prerequisite for the coding of synthesis and functional arrangement of cellular elements in biological evolution. Far infrared dynamics, reminiscent of coherent nonrelativistic super fluids in 3+1-dimensions, may have played a role. Finally, we address the question whether the identified electromagnetic fields may also influence neural systems in general and human (self) consciousness in particular. We are finding support for recent electromagnetic and stochastic zero-point energy field theories in quantum consciousness studies. The striking similarity of electromagnetic wave frequencies, detected by us in the biological studies, and in selected clay minerals, as well as in color spectra, tone scales and sound induced geometric Chladni patterns, may indicate that we identified the involvement of a universal electromagnetic principle, that underlies the observed life sustaining effects and also may have been instrumental in the creation of biologica...

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“…FCPb is composed of only fcp5 proteins, which are quite homologous to fcp1-3 (8,9,15,25), and assemble into nonamers (10). Each monomeric subunit of FCPb binds up to eight Chl a, two Chl c, and eight Fx pigment molecules (11,12), while FCPa is generally isolated with an identical pigment composition but one Chl a less per monomer, likely due to pigment loss during isolation (11). This gives a total of 18 pigments per monomer of FCPb, the same number as for an LHCII monomer.…”

Section: Significancementioning

confidence: 99%

“…23), as well as Chl b609, which is likely replaced with Chl c in FCPa/b (11). Specifically, the transmembrane helices 1 and 3, which contain the residues that bind Chls 602, 603, 610, 612, and 613, are highly homologous in these complexes, and helix 2 and the C terminus of FCPa/b contain residues that are expected to bind Chls 614 and 609 in similar positions as in LHCII (11,12). As a result, at least two of LHCII's terminal-emitter Chls (a610, a611, and a612) as well as the two other low-energy Chl dimers (a602-a603 and a613-a614) are conserved in FCPa/b.…”

Section: Significancementioning

confidence: 99%

“…The major types of FCP that can be isolated from centric diatoms like Cyclotella meneghiniana are known as FCPa and FCPb (8). The monomeric subunits of FCPa and FCPb are physically smaller than an LHCII monomer (9,10), and there is strong indication that FCPa and FCPb bind the same number of pigments per monomer as LHCII (11,12), yet various experimental results have indicated that the interpigment coupling, especially between chlorophyll (Chl) a's, is considerably weaker in FCP than in LHCII. First, circular dichroism spectroscopy shows a lack of Chl a-Chl a excitonic bands in the Q y region of isolated FCPs (9,13) as well as for FCPs in isolated thylakoids and in intact cells (14).…”

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confidence: 99%

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How reduced excitonic coupling enhances light harvesting in the main photosynthetic antennae of diatoms

Krüger

Malý

Alexandre

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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Strong excitonic interactions are a key design strategy in photosynthetic light harvesting, expanding the spectral cross-section for light absorption and creating considerably faster and more robust excitation energy transfer. These molecular excitons are a direct result of exceptionally densely packed pigments in photosynthetic proteins. The main light-harvesting complexes of diatoms, known as fucoxanthin-chlorophyll proteins (FCPs), are an exception, displaying surprisingly weak excitonic coupling between their chlorophyll (Chl) 's, despite a high pigment density. Here, we show, using single-molecule spectroscopy, that the FCP complexes of switch frequently into stable, strongly emissive states shifted 4-10 nm toward the red. A few percent of isolated FCPa complexes and ∼20% of isolated FCPb complexes, on average, were observed to populate these previously unobserved states, percentages that agree with the steady-state fluorescence spectra of FCP ensembles. Thus, the complexes use their enhanced sensitivity to static disorder to increase their light-harvesting capability in a number of ways. A disordered exciton model based on the structure of the main plant light-harvesting complex explains the red-shifted emission by strong localization of the excitation energy on a single Chl pigment in the terminal emitter domain due to very specific pigment orientations. We suggest that the specific construction of FCP gives the complex a unique strategy to ensure that its light-harvesting function remains robust in the fluctuating protein environment despite limited excitonic interactions.

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Coherence and population dynamics of chlorophyll excitations in FCP complex: Two-dimensional spectroscopy study

Cited by 34 publications

References 62 publications

Resolving Vibrational from Electronic Coherences in Two-Dimensional Electronic Spectroscopy: The Role of the Laser Spectrum

Resolving Vibrational from Electronic Coherences in Two-Dimensional Electronic Spectroscopy: The Role of the Laser Spectrum

Quantum Wave Information of Life Revealed: An Algorithm for Electromagnetic Frequencies that Create Stability of Biological Order, With Implications for Brain Function and Consciousness

How reduced excitonic coupling enhances light harvesting in the main photosynthetic antennae of diatoms

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