Artificial light-harvesting arrays for solar energy conversion

Harriman, Anthony

doi:10.1039/c5cc03577e

Cited by 71 publications

(42 citation statements)

References 107 publications

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“…6 Inspired by these natural architectures, novel artificial light-harvesting systems attempting to replicate the efficiency of the natural systems are being explored for potential use as light collectors and energy funnels in solar energy conversion systems. 7,8 FRET also plays an important role in nanosensors applications, 9,10 and can be used to tune colour composition in white-light-emitting structures. 11 In many of these applications the limited range of R DA may pose restrictions on the design and efficiency of the systems.…”

Section: Introductionmentioning

confidence: 99%

Selective turn-on and modulation of resonant energy transfer in single plasmonic hybrid nanostructures

et al. 2017

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Förster resonant energy transfer (FRET) is a nonradiative process by which the energy of light absorbed by a donor molecule is transferred to an acceptor molecule over a distance of several nanometers. FRET plays a crucial role in photosynthesis and nature-inspired artificial light-harvesting systems that are being explored for use in energy conversion applications. Localized plasmons of metal nanoparticles can potentially lead to a significant increase of FRET efficiency and effective donor-acceptor distance. Here, we prepare hybrid nanostructures composed of a gold nanorod and donor and acceptor molecules covalently attached to its surface, and study them on the level of a single nanoparticle by simultaneous dark-field scattering, fluorescence imaging and spectroscopy. The single-particle approach enables selective excitation of the longitudinal plasmon of the gold nanorod by polarization of the excitation light. The emission intensity of the acceptor molecules can be controllably and reversibly modulated over a wide range by the polarization angle, thus enabling a selective turn-on of the FRET process and control over the emission color of the hybrid nanostructure. Numerical simulations show that the interactions of the donor and acceptor molecules with the plasmon lead to an increase of the energy transfer efficiency by a factor of ∼65. These findings represent the concept of a novel colour switching approach and could pave the way for innovative applications in optoelectronics and nanophotonics.

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Section: Introductionmentioning

confidence: 99%

Selective turn-on and modulation of resonant energy transfer in single plasmonic hybrid nanostructures

et al. 2017

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“…Here, donor and acceptor are so weakly coupled that they retain the spectroscopic characteristics of the isolated components but other issues such as orientation of transition moments and spectral overlap of donor fluorescence with acceptor absorption are important parameters governing the rate of the process. [1][2][3][4][5][6][7][8] On the other extreme, two or more chromophores may be coupled so strongly that the eigenstates of the newly formed super-chromophore deviate dramatically from those of its constituents.…”

Section: Introductionmentioning

confidence: 99%

Dynamic exciton localisation in a pyrene–BODIPY–pyrene dye conjugate

Auerhammer

Schulz

Schmiedel

et al. 2019

Phys. Chem. Chem. Phys.

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The photophysics of a molecular triad consisting of a BODIPY dye and two pyrene chromophores attached in 2-position are investigated by steady state and fs-time resolved transient absorption spectroscopy as well as by field induced surface hopping (FISH) simulations. While the steady state measurements indicate moderate chromophore interactions within the triad, the time resolved measurements show upon pyrene excitation a delocalised excited state which localises onto the BODIPY chromophore with a time constant of 0.12 ps. This could either be interpreted as an internal conversion process within the excitonically coupled chromophores or as an energy transfer from the pyrenes to the BODIPY dye. The analysis of FISH-trajectories reveals an oscillatory behaviour where the excitation hops between the pyrene units and the BODIPY dye several times until finally they become localised on the BODIPY chromophore within 100 fs. This is accompanied by an ultrafast nonradiative relaxation within the excitonic manifold mediated by the nonadiabatic coupling. Averaging over an ensemble of trajectories allowed us to simulate the electronic state population dynamics and determine the time constants for the nonradiative transitions that mediate the ultrafast energy transfer and exciton localisation on BODIPY.

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“…Artificial photosynthetic systems designed as bio‐inspired analogues have tended to avoid the light‐harvesting antennae in favour of focussing on the light driven electron‐transfer chemistry . The rather limited progress that has been made in the field, despite major advances in the synthesis of intricate molecular assemblies which closely resemble the photosynthetic reaction centre complex, might be used to argue that light‐harvesting is crucial to the successful storage of sunlight as chemical potential …”

Section: Introductionmentioning

confidence: 99%

“…[9,10] The rather limited progress that has been made in the field, [11] despite major advances in the synthesis of intricate molecular assemblies which closely resemble the photosynthetic reaction centrec omplex, might be used to argue that light-harvesting is crucialt ot he successfulstorage of sunlight as chemical potential. [12] Light-harvesting antennae operate by arranging selected fluorophores in close proximity such that efficient electronic energyt ransfer (EET) can occur between neighbouring chromophores. Many artificial molecular arraysh ave been describedt hat duplicates uch EET processes.…”

Section: Introductionmentioning

confidence: 99%

Exciton Migration and Surface Trapping for a Photonic Crystal Displaying Charge‐Recombination Fluorescence

Al-Aqar

Atahan

Benniston

et al. 2016

Chemistry A European J

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A compact donor-acceptor molecular dyad has been synthesized by attaching an N,N-dimethylamino fragment to a naphthalic anhydride residue. The dyad shows fluorescence from an intramolecular charge-transfer state (i.e., charge-recombination fluorescence) in solution, with the photo-physical properties being strongly dependent on the solvent polarity. Similar emission is seen for single crystals of the target compound, the molecules being aligned head-to-head, although time-resolved emission profiles display dual-exponential kinetics. A second polymorph with the head-to-tail alignment also gives rise to two lifetimes that differ somewhat from those of the first structure, which are assigned to bulk and surface-bound molecules. Growing the crystal in the presence of Rhodamine B localizes the dye around the surface. Excitation of the crystal is followed by sub-ps exciton migration along the aligned stacks, with occasional crossing to adjacent stacks and trapping at the surface. Rhodamine B present at very low levels acts as the acceptor for excitons entering the surface layer. Crystals embedded in a polyester resin form an artificial light-harvesting antenna able to sensitize an amorphous silicon solar cell.

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Artificial light-harvesting arrays for solar energy conversion

Cited by 71 publications

References 107 publications

Selective turn-on and modulation of resonant energy transfer in single plasmonic hybrid nanostructures

Selective turn-on and modulation of resonant energy transfer in single plasmonic hybrid nanostructures

Dynamic exciton localisation in a pyrene–BODIPY–pyrene dye conjugate

Exciton Migration and Surface Trapping for a Photonic Crystal Displaying Charge‐Recombination Fluorescence

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