Metal-Enhanced Fluorescence of Chlorophylls in Single Light-Harvesting Complexes

Maćkowski, Sebastian; Piatkowski, Dawid; Wörmke, Stephan; Hartschuh, Achim; Braeuchle, Christoph R.; Brotosudarmo, Tatas Hardo Panintingjati; Scheer, Hugo; Agarwal, Ashish; Kotov, Nicholas A.; Govorov, Alexander O.

doi:10.1557/proc-1208-o14-01

Cited by 21 publications

(46 citation statements)

References 30 publications

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“…In all cases, the intensities measured for RCs on SIF are substantially higher than those on glass. Moreover, the distributions of fluorescence intensity values measured for RCs deposited on SIF substrates are significantly broader than those on glass, which points toward inhomogeneities attributable to local variations of plasmonic enhancement due to changes in SIF morphology or different distance between photosynthetic complexes and the metallic layer . Experimentally obtained average intensities of RC emission are listed in Table , together with EFs calculated by dividing the average values measured on SIF and glass.…”

Section: Resultsmentioning

confidence: 99%

“…In the case of PSI deposited on silver island films (SIFs), we recently found exceptionally large (~ 200) enhancement factors of the fluorescence intensity . Enhancements by two orders of magnitude are remarkable, in particular, when compared to the results obtained for other photosynthetic pigment–protein complexes, ranging from a factor of 2 to 20 . The effect appears to reflect the complexity of PSI, or, more specifically, the large number of bound pigments (chlorophylls and carotenoids).…”

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confidence: 90%

“…Recently, the plasmon resonance in metallic nanoparticles was applied to modify the optical properties of a broad range of materials, including fluorescent dyes , rare‐earth ions , semiconductor quantum dots , and photosynthetic pigment–protein complexes . For properly designed hybrid structures, strong enhancement of the emission intensity, attributed either to enhancement of absorption rate or Purcell effect, was observed.…”

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confidence: 99%

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Origin of bimodal fluorescence enhancement factors of Chlorobaculum tepidum reaction centers on silver island films

et al. 2016

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We focus on the spectral dependence of plasmon-induced enhancement of fluorescence of Chlorobaculum tepidum reaction centers. When deposited on silver island film, they exhibit up to a 60-fold increase in fluorescence. The dependence of enhancement factors on the excitation wavelength is not correlated with the absorption spectrum of the plasmonic structure. In particular, the presence of one (or multiple) trimers of the Fenna-Matthews-Olson (FMO) protein reveals itself in bimodal distribution of enhancement factors for the excitation at 589 nm, the wavelength corresponding to bacteriochlorophyll absorption of FMO and the core of the RC. We conclude that the structure of multichromophoric complexes can substantially affect the impact of plasmonic excitations, which is important in the context of assembling functional biohybrid systems.

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Section: Resultsmentioning

confidence: 99%

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confidence: 90%

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confidence: 99%

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Origin of bimodal fluorescence enhancement factors of Chlorobaculum tepidum reaction centers on silver island films

et al. 2016

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“…[ 117 ], the model was shown to be able to reproduce the experimentally determined amplification of the fluorescence signal for a LH protein (PCP) in the presence of silver nanoparticles. 119 More interestingly, the calculations allowed to gain insights into the role of metal to modulate the various involved optical processes (absorption, emission, EET between the pigments), and led to formulate design rules for building hybrid bio-nano-systems. Successively, the multilayer model was used to investigate how a plasmonic nanostructure affects excitonic states of the LH2 complex.…”

Section: Towards Composite Systemsmentioning

confidence: 99%

Multiscale modelling of photoinduced processes in composite systems

2019

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| In the last decades, the quantum mechanical modeling has moved from isolated molecules made of few atoms, to large supramolecular aggregates embedded in complex environments. This has been made possible by the important progress achieved by multiscale models based on the integration of QM methods with classical descriptions. One of the first example of this integration is represented by continuum solvation models that starting from the eighties of the last century have been largely and successfully applied to predict properties and processes of solvated molecules. Almost in the same years, another alternative classical description, based on Molecular Mechanics (MM) has been coupled to QM methods to give the hybrid QM/MM approach. Since their first formulations, these QM/classical models have seen an enormous development in terms of accuracy, robustness and generalizability. This progress has allowed their application to systems of increasing complexity and to processes never faced before within a QM framework. An important example of such an achievement is represented by the novel insights reached in the fundamental understanding and the possible exploitation of photoinduced processes in biomolecules, nanomaterials and, more in general, composite systems where different "objects" of molecular, nano and mesoscopic scale are coupled together. In this review, we highlight the potentials and the limitations of such modeling, thereby showing which developments are still needed to definitely make the QM-based multiscale strategy the gold-standard for explaining the outputs of novel advanced spectroscopic techniques and predicting the outcome of light-activated events in composite systems. The multiscale strategiesIn the years, two main strategies to combine QM descriptions of the target and classical models of the environment, have been proposed. Interestingly, their first formulations date back to the same years, namely the end of the seventies of the previous century. [8][9][10] The two strategies refer to continuum and discrete (or atomistic) descriptions of the environment, respectively. In the latter case, the atoms of the environment (or group of atoms in coarser grained versions of the model) are treated through a Molecular Mechanics (MM) force field (FF). [11][12][13][14][15] In the former case, instead, the atomic nature of the environment is lost and a continuum description in terms of macroscopic properties is introduced instead. 16-18 Despite this huge "modellistic" difference, the two formulations present important common elements when reconsidered from the point of view of the QM target. In any case, for simplicity's sake two separate presentations will be given. QM/continuum. If the environment loses its atomic nature, an effective description has to be introduced which is based on some macroscopic properties. This is exactly what is done in continuum models where the target sees the environment as an infinite dielectric medium characterized by a (generally) frequency and position dependent permittivit...

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“…The effects of metals on fluorescence have been subject to prior reports. Using intrinsic(24), visible(25, 26, 28, 29) and NIR(27) fluorophores we have shown that the incident light-induced fields around the metallic nanoparticles can result in locally enhanced excitation, and the excited state fluorophores can crease plasmons in the particles, resulting in increased emission from the system of fluorophores and particles. We have shown proximity of fluorophores to metallic surfaces can increase the total radiative decay rate(31).…”

Section: Introductionmentioning

confidence: 99%

Metal-enhanced fluorescence of single green fluorescent protein (GFP)

Zhang

Lakowicz

2008

Biochemical and Biophysical Research Communications

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The green fluorescent protein (GFP) has emerged as a powerful reporter molecule for monitoring gene expression, protein localization and protein-protein interaction. However, the detection of low concentrations of GFPs is limited by the weakness of the fluorescent signal and the low photostability. In this report, we observed the proximity of single GFPs to metallic silver nanoparticles increases its fluorescence intensity approximately 6-fold and decreases the decay time. Single protein molecules on the silvered surfaces emitted 10-fold more photons as compared to glass prior to photobleaching. The photostability of single GFP has increased to some extent. Accordingly, we observed longer duration time and suppressed blinking. The single-molecule lifetime histograms indicate the relatively heterogeneous distributions of protein mutants inside the structure.

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Metal-Enhanced Fluorescence of Chlorophylls in Single Light-Harvesting Complexes

Cited by 21 publications

References 30 publications

Origin of bimodal fluorescence enhancement factors of Chlorobaculum tepidum reaction centers on silver island films

Origin of bimodal fluorescence enhancement factors of Chlorobaculum tepidum reaction centers on silver island films

Multiscale modelling of photoinduced processes in composite systems

Metal-enhanced fluorescence of single green fluorescent protein (GFP)

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