Energy Transfer in Single‐Molecule Photonic Wires

García‐Parajó, María F.; Hernando, Jordi; Mosteiro, Gabriel Sanchez; Hoogenboom, Jacob P.; Dijk, E.M.H.P. van; Hulst, Niek F. van

doi:10.1002/cphc.200400630

Cited by 65 publications

(52 citation statements)

References 49 publications

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“…One major motivation was the elaboration of artificial analogues of the light-harvesting complexes of photosynthetic organisms. [1][2][3][4][5][6][7] However, multichromophoric molecules have also been developed for other applications such as, for example, molecular wires, 8,9 single photon sources, 10 logic gates, 11 light stabilizers, 12 fluorescent DNA probes, 13,14 or nonlinear optical materials. 15 The covalent bonding allows the degree of interaction between the chromophoric units to be controlled to some extent.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast Photoinduced Charge Separation in Naphthalene Diimide Based Multichromophoric Systems in Liquid Solutions and in a Lipid Membrane

et al. 2008

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The photophysical properties of multichromophoric systems consisting of eight red or blue naphthalene diimides (NDIs) covalently attached to a p-octiphenyl scaffold, as well as a blue bichromophoric system with a biphenyl scaffold, have been investigated in detail using femtosecond time-resolved spectroscopy. The blue octachromophoric systems have been recently shown to self-assemble as supramolecular tetramers in lipid bilayer membranes and to enable generation of a transmembrane proton gradient upon photoexcitation (Bhosale, S.; Sisson, A. L.; Talukdar, P.; Fürstenberg, A.; Banerji, N.; Vauthey, E.; Bollot, G.; Mareda, J.; Röger, C.; Würthner, F.; Sakai, N.; Matile, S. Science 2006, 313, 84). A strong reduction of the fluorescence quantum yield was observed when going from the single NDI units to the multichromophoric systems in methanol, the effect being even stronger in a vesicular lipid membrane. Fluorescence up-conversion measurements reveal ultrafast self-quenching in the multichromophoric systems, whereas the formation of the NDI radical anion, evidenced by transient absorption measurements, points to the occurrence of photoinduced charge separation. The location of the positive charge could not be established unambiguously from the transient absorption measurements, but energetic considerations indicate that charge separation should occur between two NDI units in the blue systems, whereas both an NDI unit and the p-octiphenyl scaffold could act as electron donor in the red system. The lifetime of the charge-separated state was found to increase from 22 to 45 ps by going from the bi-to the octachromophoric blue systems in methanol, while a 400 ps decay component was observed in the lipid membrane. This lifetime lengthening is explained in terms of charge migration that is most efficient when the octachromophoric systems are assembled as supramolecular tetramers in the lipid membrane. Furthermore, the average charge-separated state lifetime of the red system in methanol is even larger and amounts to 750 ps. This effect cannot be simply explained in terms of Marcus inverted regime as the driving force for charge recombination in the red system is only slightly larger than in the blue one. A better spatial separation of the charges in the red system stemming from the localization of the hole on the p-octiphenyl scaffold could additionally contribute to the slowing down of charge recombination.

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Section: Introductionmentioning

confidence: 99%

Ultrafast Photoinduced Charge Separation in Naphthalene Diimide Based Multichromophoric Systems in Liquid Solutions and in a Lipid Membrane

et al. 2008

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“…Alternating laser excitation has been applied to achieve fluorescence-aided molecule sorting and enable simultaneous analysis of biomolecular structure and interactions at the level of single molecules by spFRET (81). FRET efficiency could be measured for a DNA-based photonic wire (82,83). The ATP-waiting conformation of rotating F 1 -ATPase has been revealed by spFRET (84).…”

Section: Single-pair Fluorescence Resonance Energy Transfermentioning

confidence: 99%

Application and New Developments in Fluorescence Spectroscopic Techniques in Studying Individual Molecules

Patra

2008

Applied Spectroscopy Reviews

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Techniques based on fluorescence have played a variety of roles in chemistry, physics, spectroscopy, medicine, nanotechnology, and biotechnology due to their high selectivity, sensitivity, simplicity, and fastness in spectroscopic and imaging measurements. While detecting fluorescence from individual molecules by fluorescence-based techniques, poor signal, limited lifespan of fluorophores, trade-off between time resolution, and the level of detail of information were few major concerns. Ultrasensitive detectors permit the combination of the high time resolution of single photon counting devices with the large field of view and spectral resolution allowed by twodimensional detectors. Photobleaching and on-off blinking of fluorophores can be improved dramatically by chemical modifications or changing the reagents. New ways of controlling local fields such as optic, electric, magnetic, chemical, or biochemical environments take advantage of the noninvasiveness and high temporal and spatial resolution of single-molecule fluorescence (SMF) to get a direct feedback of events at the nanometer scale in various domains of research. Some of the applications and new developments in fluorescence spectroscopic techniques in detecting, investigating, and/or manipulating individual molecules have been discussed.

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“…This concept may be extended with the use of several jumper dyes to form "photonic wires" capable of transporting energy over large molecular distances [86]. Garcia-Parajo et al studied such a system composed of five distinct fluorophores placed along a double-stranded DNA molecule from the bluest at one end to the reddest at the other end [87]. Single-molecule fluorescence spectroscopy showed that these systems exhibited complex fluctuations in FRET rates due to dye blinking and spectral and/or orientational fluctuations.…”

Section: 41mentioning

confidence: 99%

Single‐Molecule Applications

Pons

2013

FRET – Förster Resonance Energy Transfer

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Recent years have witnessed major progress in fluorescence microscopy instrumentation, raising its detection sensitivity to the single-molecule level. Observation of single molecules has since brought a wealth of information and allowed a better understanding of many physical, chemical, and biological processes [1][2][3][4][5][6]. Singlemolecule fluorescence has become in particular a powerful tool to study biomolecular functions [7][8][9][10][11][12]. Indeed, these functions most often involve conformational changes and/or multimolecular association/dissociation. This implies that, in the absence of an external synchronization, biomolecules in solution fluctuate between different states independently of each other. Whereas ensemble experiments provide only average measurements over all these different states, singlemolecule measurements can reveal both heterogeneity in the population (in the equilibrium distribution of states) and dynamics (i.e., sequence of transitions, frequencies, rates, etc.).Single-molecule F€ orster (or Fluorescence) resonance energy transfer is certainly one of the most fertile single-molecule fluorescence techniques [13][14][15][16][17][18][19]. The vast majority of smFRET studies involve labeling of the target biomolecules with a donor and an acceptor fluorophore at specific sites. The FRET distance dependence translates changes in donor-acceptor separation distance into measurable photophysical parameters, such as donor/acceptor emission ratios, lifetimes, and anisotropy. This in turn provides a tool to follow conformational changes in a single biomolecule or association/dissociation dynamics in a single complex of interacting partners.Observation of single-molecule fluorescence signals raises several difficulties, including weak fluorescence signals and the need to isolate the signal from one molecule from the large background of other molecules, without perturbing the functional integrity of the biomolecule. These challenges can be overcome using mainly two categories of microscopy modalities. The first modality relies on immobilization of molecules on a substrate. A time trace of fluorescence signals FRET -Förster Resonance Energy Transfer: From Theory to Applications, First Edition. Edited by Igor Medintz and Niko Hildebrandt.

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Energy Transfer in Single‐Molecule Photonic Wires

Cited by 65 publications

References 49 publications

Ultrafast Photoinduced Charge Separation in Naphthalene Diimide Based Multichromophoric Systems in Liquid Solutions and in a Lipid Membrane

Ultrafast Photoinduced Charge Separation in Naphthalene Diimide Based Multichromophoric Systems in Liquid Solutions and in a Lipid Membrane

Application and New Developments in Fluorescence Spectroscopic Techniques in Studying Individual Molecules

Single‐Molecule Applications

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