Coherent Control Protocol for Separating Energy-Transfer Pathways in Photosynthetic Complexes by Chiral Multidimensional Signals

Voronine, Dmitri V.; Abramavičius, Darius; Mukamel, Shaul

doi:10.1021/jp111555h

Cited by 12 publications

(13 citation statements)

References 36 publications

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“…In particular, coherence between eigenstates can be generated when there is coherence between the light modes which excite those eigenstates. This can be achieved either through coherence between frequency modes [6,7,[44][45][46][47] or, when eigenstates couple to different polarisation modes, using polarised light [21,39]. For example, the energy-basis coherences detected in spectroscopic experiments on light-harvesting systems [2][3][4][5]43] are due to the spectral coherence of the laser pulses [6][7][8][9][10].…”

Section: Toward Experimental Demonstrations Of Enhancementsmentioning

confidence: 99%

“…Energy-basis coherence needed for type II enhancements can be prepared optically because light couples directly to eigenstates and not to individual sites [6,7,[44][45][46][47]. In particular, coherence between eigenstates can be generated when there is coherence between the light modes which excite those eigenstates.…”

Section: Toward Experimental Demonstrations Of Enhancementsmentioning

confidence: 99%

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Classification of Coherent Enhancements of Light-Harvesting Processes

Tomasi

Kassal

2020

J. Phys. Chem. Lett.

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In recent years, several kinds of coherence have been shown to affect the performance of lightharvesting systems, in some cases significantly improving their efficiency. Here, we classify the possible mechanisms of coherent efficiency enhancements, based on the types of coherence that can characterise a light-harvesting system and the types of processes these coherences can affect. We show that enhancements are possible only when coherences and dissipative effects are best described in different bases of states. Our classification allows us to predict a previously unreported coherent enhancement mechanism, where coherence between delocalised eigenstates can be used to localise excitons away from dissipation, thus reducing recombination and increasing efficiency.

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Section: Toward Experimental Demonstrations Of Enhancementsmentioning

confidence: 99%

Section: Toward Experimental Demonstrations Of Enhancementsmentioning

confidence: 99%

Classification of Coherent Enhancements of Light-Harvesting Processes

Tomasi

Kassal

2020

J. Phys. Chem. Lett.

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“…12 Genetic algorithms have also been developed to construct optimal pulse polarizations and analyze selected features of simulated two-dimensional spectra of porphyrin dimers, 13 and the Fenna-Matthews-Olson (FMO) photosynthetic complex. 14 …”

Section: Introductionmentioning

confidence: 99%

Dissecting Two-Dimensional Ultraviolet Spectra of Amyloid Fibrils into Beta-Strand and Turn Contributions

Rodríguez

Mukamel

2012

J. Phys. Chem. B

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We present an analysis of the contributions of various secondary structure elements of the amyloid β-protein to the two-dimensional far ultraviolet (2DFUV) signal of an amyloid fibril model. The contributions of the turns and the β-strands are affected by the geometry of the backbone peptide amide π → π* transition dipoles, the backbone inter-amide coupling in the excited state, and the exciton delocalization. These contributions are clearly distinguishable in the xyxy-xyyx pulse polarization configuration. The differences are attributed to the smaller splitting of the exciton energies and the larger fluctuations of the geometry of the peptide amide π → π * transition dipoles at the turns, while make the 2DFUV signal sensitive to the secondary structure. This signal may be used to determine the proportion of turns and β -strands.

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“…Many experiments in physics [1][2][3][4], chemistry [5][6][7], communication technology [8][9][10], and quantum information technology [11,12] make use of shaped ultrafast laser pulses, e.g. for addressing dynamic processes in molecules [13][14][15][16][17][18], to optimize contrast in stimulated emission [19] or Raman spectroscopy [20,21] and to enhance stability and output power in pulse amplification [22], parametric conversion [23], and supercontinuum generation [24,25].…”

Section: Introductionmentioning

confidence: 99%

Beating spatio-temporal coupling: implications for pulse shaping and coherent control experiments

et al. 2011

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Diffraction of finite sized laser beams imposes a limit on the control that can be exerted over ultrafast pulses. This limit manifests as spatio-temporal coupling induced in standard implementations of pulse shaping schemes. We demonstrate the influence this has on coherent control experiments that depend on finite excitation, sample, and detection volumes. Based on solutions used in pulse stretching experiments, we introduce a double-pass scheme that reduces the errors produced through spatio-temporal coupling by at least one order of magnitude. Finally, employing single molecules as nanoscale probes, we prove that such a double pass scheme is capable of artifact-free pulse shaping at dimensions two orders of magnitude smaller than the diffraction limit.

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Coherent Control Protocol for Separating Energy-Transfer Pathways in Photosynthetic Complexes by Chiral Multidimensional Signals

Cited by 12 publications

References 36 publications

Classification of Coherent Enhancements of Light-Harvesting Processes

Classification of Coherent Enhancements of Light-Harvesting Processes

Dissecting Two-Dimensional Ultraviolet Spectra of Amyloid Fibrils into Beta-Strand and Turn Contributions

Beating spatio-temporal coupling: implications for pulse shaping and coherent control experiments

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