Anisotropic energy and electron migration in multichromophore-laden polymers on metal surfaces

Whitesell, James K.; Chang, Hye Kyung; Fox, Marye Anne; Galoppini, Elena; Watkins, D. M.; Fox, Harold H.; Hong, Bo Min

doi:10.1351/pac199668071469

Cited by 20 publications

(17 citation statements)

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“…Such fields will influence rates of electron flow and, in extreme cases, will bias their competitiveness vis-a-vis fluorescence. Galoppini and Fox find significant control of PET rate by the net electric field of an α-helical polypeptide. , Opposite regioisomers differ in their PET rates by up to a factor of 27. The PET thermodynamics also differ.…”

Section: Switches With More Complex Behaviormentioning

confidence: 99%

Signaling Recognition Events with Fluorescent Sensors and Switches

et al. 1997

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Section: Switches With More Complex Behaviormentioning

confidence: 99%

Signaling Recognition Events with Fluorescent Sensors and Switches

et al. 1997

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“…Aminotrimercaptoamide 1 has been shown to be a versatile linker, having been used both as a seed site for the growth of oriented helical peptides and as an attachment site for anchoring preformed polymers of defined composition [5]. In addition, the amino functional group in 1 participates in in situ coupling with active esters, e.g., for the attachment of the emissive dye fluorescamine [6].…”

Section: Introduction ± Previouslymentioning

confidence: 99%

α-Helical Polypeptide Films Grown From Sulfide or Thiol Linkers on Gold Surfaces

Kittredge

Minton

Fox

et al. 2002

HCA

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Dedicated to Professor Andre¬ M. Braun on the occasion of his 60th birthday We prepared two new linkers, S-functionalized adamantane derivatives 2 and 3, which bind as monolayers on polycrystalline gold. From these surface anchors, both l-and d-isomers of alanine can be grown as thin films of a-helical polypeptides directed from the gold surface by using the appropriate N-carboxyalanine anhydride. FT-IR Studies show that these layers are roughly 1000-ä thick and that, under the same growth conditions, the l-polypeptide layers grow at a rate ca. 30% greater than that of the non-natural d-amino acid. X-Ray photoelectron spectroscopy studies show that, upon equilibration, all three S-atoms of the sulfide moieties of 2 are bound to the gold surface, and that, on average, three of the four thiols of 3 are chemoadsorbed. The essential role of H 2 O on the surface of these films as a necessary component in these gas-phase polymerization reactions is demonstrated.

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“…One is based on constructing complex supramolecular assemblies in which the various components are linked together by chemical bonds (11)(12)(13)(14)(15)(16)(17)(18)(19)(20)(21)(22). The second utilizes various supports such as polymers (23)(24)(25)(26)(27)(28)(29)(30)(31)(32), zeolites (33)(34)(35)(36)(37)(38), sol-gel glasses (39 -41), lipid membranes (42,43), or selfassembled films (44 -47) as scaffolds for incorporating and organizing the necessary components.…”

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confidence: 99%

Mimicking the antenna-electron transfer properties of photosynthesis

Sýkora

Maxwell

DeSimone

et al. 2000

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

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A molecular assembly based on derivatized polystyrene is described, which mimics both the light-harvesting and energy-conversion steps of photosynthesis. The system is unique in that the two key parts of a photosynthetic system are incorporated in a functional assembly constructed from polypyridine complexes of Ru II . This system is truly artificial, as none of the components used in construction of the assembly are present in a natural photosynthetic system. Quantitative evaluation of the energy and electron transfer dynamics after transient irradiation by visible light offers important insights into the mechanisms of energy transport and electron transfer that lead to photosynthetic light-to-chemical energy conversion. In natural photosynthesis, light is converted into chemical energy by a sequence of coupled energy and electron transfer events. Initially, sunlight is absorbed by light-harvesting pigments, chlorophylls and carotenoids, which act as antenna fragments. The energy collected by absorption creates molecular excited states and is subsequently transferred between chromophores through an energy cascade ultimately reaching the reaction center. At the reaction center, the light energy is converted into chemical energy by a series of electron transfer steps (1-5). Understanding of these concepts has motivated chemists to design assemblies that have related properties and may provide the basis for artificial solar energy conversion devices (6 -10). The construction of a functional and efficient artificial solar energy conversion device would have a significant impact on our ability to use solar energy.To date, most research on the artificial solar energy conversion has focused on mimicking various aspects of natural photosynthesis. Through these studies, a reasonable understanding of various components necessary for construction of an artificial photosynthetic system has been developed. The main challenge at the moment is to assemble these components in a spatially organized manner, which will allow their efficient collaboration in harvesting the light energy and converting it efficiently into chemical energy. There are currently two strategies. One is based on constructing complex supramolecular assemblies in which the various components are linked together by chemical bonds (11)(12)(13)(14)(15)(16)(17)(18)(19)(20)(21)(22). The second utilizes various supports such as polymers (23-32), zeolites (33-38), sol-gel glasses (39 -41), lipid membranes (42, 43), or selfassembled films (44 -47) as scaffolds for incorporating and organizing the necessary components.Derivatized polymers provide an attractive approach to this problem because they offer f lexibility and simplicity in the design of multifunctional assemblies. We (23-28) and others (29 -32) have used derivatized polymers to gain insight into various aspects of the photosynthetic process. Recently, we showed, for example, that polymeric assemblies derivatized with polypyridyl complexes of Ru II and Os II display antenna and energy transport properties ...

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Anisotropic energy and electron migration in multichromophore-laden polymers on metal surfaces

Abstract: Abstract

Cited by 20 publications

References 0 publications

Signaling Recognition Events with Fluorescent Sensors and Switches

Signaling Recognition Events with Fluorescent Sensors and Switches

α-Helical Polypeptide Films Grown From Sulfide or Thiol Linkers on Gold Surfaces

Mimicking the antenna-electron transfer properties of photosynthesis

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