Lateral Self-Sorting on Surfaces: A Practical Approach to Double-Channel Photosystems

Abstract

We report that self-sorting during self-organizing surface-initiated copolymerization (co-SOSIP) provides facile access to oriented multicomponent architectures. Alternate lateral and uniform axial self-sorting into formal supramolecular n/p-heterojunction photosystems is found to generate up to 40 times more photocurrent. More or less topological matching gives rise to alternate axial self-sorting into inactive charge-transfer complexes or uniform lateral sorting into the less active macrodomains, respectively. Experimental support for self-repair during co-SOSIP is reported. Initiators on the surface are shown to serve as templates for the self-sorting into multichannel architectures of freely variable composition.

Naphthalenebisimides as photofunctional surfactants for SWCNTs – towards water-soluble electron donor–acceptor hybrids

“…11 Despite their smaller size, interesting features of NBIs such as being an n-type semiconductor and exhibiting high π-acidity and chemical versatility renders them promising candidates for novel photoactive SWCNT based hybrids, yielding oxidized SWCNTs as well as reduced NBIs upon illumination or even in the dark. 12 Some of these properties have been proven upon implementing NBIs as electron acceptors in photoactive electron donor–acceptor hybrids, 13 anion transport 14 as well as electron conducting channels 15 and layers or even in π-catalysis. 16 …”

Multistep organic synthesis of modular photosystems

“…Initiator 2 is composed of a central naphthalenediimide (NDI) [4–19] to act as a template for the central stack and two peripheral NDIs to act as templates for stack exchange. They are embedded into hydrogen-bonded networks, to assure self-organization, and four geminal diphosphonates [20–21] for tetravalent anchoring on the ITO surface.…”

Interfacing Functional Systems

“…Limited only by our imagination, functional components or systems conceivable for interfacing reach from additional simple but meaningful functional groups to solid surfaces, [5,[13][14][15][16][17] proteins, [6] polymersomes, [9] liposomes, [3] cells, [4] and so on. Success with MSE will ultimately be judged from the significance, practical or conceptual, of the emergent properties obtained.…”

“…[4,5,[13][14][15][16][17] For systems interfacing, this dual nature promises access to self-sorting, self-healing, adaptability, templation, amplification, replication, transcription, and so on. [18] These expected advantages of dynamiccovalent chemistry for systems engineering have been validated with multicomponent photosystems on solid surfaces (Figs 4 and 5).…”

“…[18] These expected advantages of dynamiccovalent chemistry for systems engineering have been validated with multicomponent photosystems on solid surfaces (Figs 4 and 5). [5,[13][14][15][16][17] A chromophore is taken as a primary component with absorption and emission as intrinsic properties. The alignment of these primary components in oriented π stacks on conducting solid oxide surfaces affords primary system 5 (Fig.…”