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Article ; Online: Tools for Low-Dimensional Chemistry.

Leggett, Graham J

Langmuir : the ACS journal of surfaces and colloids

2018 Volume 35, Issue 24, Page(s) 7589–7602

Abstract: Many biological mechanisms can be considered to be low-dimensional systems: their function is determined by molecular objects of reduced dimensionality. Bacterial photosynthesis is a very good example: the photosynthetic pathway is contained within nano- ... ...

Abstract	Many biological mechanisms can be considered to be low-dimensional systems: their function is determined by molecular objects of reduced dimensionality. Bacterial photosynthesis is a very good example: the photosynthetic pathway is contained within nano-objects (vesicles) whose function is determined by the numbers and nanoscale organization of membrane proteins and by the ratios of the different types of protein that they contain. Systems biology has provided computational models for studying these processes, but there is a need for experimental platforms with which to test their predictions. This Invited Feature Article reviews recent work on the development of tools for the reconstruction of membrane processes on solid surfaces. Photochemical methods provide a powerful, versatile means for the organization of molecules and membranes across length scales from the molecular to the macroscopic. Polymer brushes are highly effective supports for model membranes and versatile functional and structural components in low-dimensional systems. The incorporation of plasmonic elements facilitates enhanced measurement of spectroscopic properties and provides an additional design strategy via the exploitation of quantum optical phenomena. A low-dimensional system that incorporates functional transmembrane proteins and a mechanism for the in situ measurement of proton transport is described.
Language	English
Publishing date	2018-11-23
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	2005937-1
ISSN	1520-5827 ; 0743-7463
ISSN (online)	1520-5827
ISSN	0743-7463
DOI	10.1021/acs.langmuir.8b02672
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Tools for Low-Dimensional Chemistry

Leggett, Graham J

Langmuir. 2018 Oct. 26, v. 35, no. 24

2018

Abstract	Many biological mechanisms can be considered to be low-dimensional systems: their function is determined by molecular objects of reduced dimensionality. Bacterial photosynthesis is a very good example: the photosynthetic pathway is contained within nano-objects (vesicles) whose function is determined by the numbers and nanoscale organization of membrane proteins and by the ratios of the different types of protein that they contain. Systems biology has provided computational models for studying these processes, but there is a need for experimental platforms with which to test their predictions. This Invited Feature Article reviews recent work on the development of tools for the reconstruction of membrane processes on solid surfaces. Photochemical methods provide a powerful, versatile means for the organization of molecules and membranes across length scales from the molecular to the macroscopic. Polymer brushes are highly effective supports for model membranes and versatile functional and structural components in low-dimensional systems. The incorporation of plasmonic elements facilitates enhanced measurement of spectroscopic properties and provides an additional design strategy via the exploitation of quantum optical phenomena. A low-dimensional system that incorporates functional transmembrane proteins and a mechanism for the in situ measurement of proton transport is described.
Keywords	models ; photochemistry ; photosynthesis ; polymers ; prediction ; spectral analysis ; transmembrane proteins
Language	English
Dates of publication	2018-1026
Size	p. 7589-7602.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	2005937-1
ISSN	1520-5827 ; 0743-7463
ISSN (online)	1520-5827
ISSN	0743-7463
DOI	10.1021/acs.langmuir.8b02672
Database	NAL-Catalogue (AGRICOLA)

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Article: Tribochemical nanolithography: selective mechanochemical removal of photocleavable nitrophenyl protecting groups with 23 nm resolution at speeds of up to 1 mm s

Ducker, Robert E / Brügge, Oscar Siles / Meijer, Anthony J H M / Leggett, Graham J

Chemical science

2023 Volume 14, Issue 7, Page(s) 1752–1761

Abstract: We describe the mechanochemical regulation of a reaction that would otherwise be considered to be photochemical, ...

Abstract	We describe the mechanochemical regulation of a reaction that would otherwise be considered to be photochemical,
Language	English
Publishing date	2023-01-16
Publishing country	England
Document type	Journal Article
ZDB-ID	2559110-1
ISSN	2041-6539 ; 2041-6520
ISSN (online)	2041-6539
ISSN	2041-6520
DOI	10.1039/d2sc06305k
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Controlling Adsorption of Diblock Copolymer Nanoparticles onto an Aldehyde-Functionalized Hydrophilic Polymer Brush via pH Modulation.

Astier, Samuel / Johnson, Edwin C / Norvilaite, Oleta / Varlas, Spyridon / Brotherton, Emma E / Sanderson, George / Leggett, Graham J / Armes, Steven P

Langmuir : the ACS journal of surfaces and colloids

2024

Abstract: Sterically stabilized diblock copolymer nanoparticles with a well-defined spherical morphology and tunable diameter were prepared by RAFT aqueous emulsion polymerization of benzyl methacrylate at 70 °C. The steric stabilizer precursor used for these ... ...

Abstract	Sterically stabilized diblock copolymer nanoparticles with a well-defined spherical morphology and tunable diameter were prepared by RAFT aqueous emulsion polymerization of benzyl methacrylate at 70 °C. The steric stabilizer precursor used for these syntheses contained pendent
Language	English
Publishing date	2024-02-06
Publishing country	United States
Document type	Journal Article
ZDB-ID	2005937-1
ISSN	1520-5827 ; 0743-7463
ISSN (online)	1520-5827
ISSN	0743-7463
DOI	10.1021/acs.langmuir.3c03392
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Active control of strong plasmon-exciton coupling in biomimetic pigment-polymer antenna complexes grown by surface-initiated polymerisation from gold nanostructures.

Lishchuk, Anna / Csányi, Evelin / Darroch, Brice / Wilson, Chloe / Nabok, Alexei / Leggett, Graham J

Chemical science

2022 Volume 13, Issue 8, Page(s) 2405–2417

Abstract: Plexcitonic antenna complexes, inspired by photosynthetic light-harvesting complexes, are formed by attachment of chlorophylls (Chl) to poly(cysteine methacrylate) (PCysMA) scaffolds grown by atom-transfer radical polymerisation from gold nanostructure ... ...

Abstract	Plexcitonic antenna complexes, inspired by photosynthetic light-harvesting complexes, are formed by attachment of chlorophylls (Chl) to poly(cysteine methacrylate) (PCysMA) scaffolds grown by atom-transfer radical polymerisation from gold nanostructure arrays. In these pigment-polymer antenna complexes, localised surface plasmon resonances on gold nanostructures are strongly coupled to Chl excitons, yielding hybrid light-matter states (plexcitons) that are manifested in splitting of the plasmon band. Modelling of the extinction spectra of these systems using a simple coupled oscillator model indicates that their coupling energies are up to twice as large as those measured for LHCs from plants and bacteria. Coupling energies are correlated with the exciton density in the grafted polymer layer, consistent with the collective nature of strong plasmon-exciton coupling. Steric hindrance in fully-dense PCysMA brushes limits binding of bulky chlorophylls, but the chlorophyll concentration can be increased to ∼2 M, exceeding that in biological light-harvesting complexes, by controlling the grafting density and polymerisation time. Moreover, synthetic plexcitonic antenna complexes display pH- and temperature-responsiveness, facilitating active control of plasmon-exciton coupling. Because of the wide range of compatible polymer chemistries and the mild reaction conditions, plexcitonic antenna complexes may offer a versatile route to programmable molecular photonic materials.
Language	English
Publishing date	2022-02-03
Publishing country	England
Document type	Journal Article
ZDB-ID	2559110-1
ISSN	2041-6539 ; 2041-6520
ISSN (online)	2041-6539
ISSN	2041-6520
DOI	10.1039/d1sc05842h
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Adsorption of Aldehyde-Functional Diblock Copolymer Spheres onto Surface-Grafted Polymer Brushes via Dynamic Covalent Chemistry Enables Friction Modification.

Johnson, Edwin C / Varlas, Spyridon / Norvilaite, Oleta / Neal, Thomas J / Brotherton, Emma E / Sanderson, George / Leggett, Graham J / Armes, Steven P

Chemistry of materials : a publication of the American Chemical Society

2023 Volume 35, Issue 15, Page(s) 6109–6122

Abstract: Dynamic covalent chemistry has been exploited to prepare numerous examples of adaptable polymeric materials that exhibit unique properties. Herein, the chemical adsorption of aldehyde-functional diblock copolymer spherical nanoparticles onto amine- ... ...

Abstract	Dynamic covalent chemistry has been exploited to prepare numerous examples of adaptable polymeric materials that exhibit unique properties. Herein, the chemical adsorption of aldehyde-functional diblock copolymer spherical nanoparticles onto amine-functionalized surface-grafted polymer brushes via dynamic Schiff base chemistry is demonstrated. Initially, a series of
Language	English
Publishing date	2023-07-19
Publishing country	United States
Document type	Journal Article
ZDB-ID	1500399-1
ISSN	1520-5002 ; 0897-4756
ISSN (online)	1520-5002
ISSN	0897-4756
DOI	10.1021/acs.chemmater.3c01227
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Hydrophilic Aldehyde-Functional Polymer Brushes: Synthesis, Characterization, and Potential Bioapplications.

Brotherton, Emma E / Johnson, Edwin C / Smallridge, Mark J / Hammond, Deborah B / Leggett, Graham J / Armes, Steven P

Macromolecules

2023 Volume 56, Issue 5, Page(s) 2070–2080

Abstract: Surface-initiated activators regenerated by electron transfer atom transfer radical polymerization (ARGET ATRP) is used to polymerize ... ...

Abstract	Surface-initiated activators regenerated by electron transfer atom transfer radical polymerization (ARGET ATRP) is used to polymerize a
Language	English
Publishing date	2023-02-22
Publishing country	United States
Document type	Journal Article
ZDB-ID	3436-8
ISSN	0024-9297
ISSN	0024-9297
DOI	10.1021/acs.macromol.2c02471
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Light-directed nanosynthesis: near-field optical approaches to integration of the top-down and bottom-up fabrication paradigms.

Leggett, Graham J

Nanoscale

2012 Volume 4, Issue 6, Page(s) 1840–1855

Abstract: The integration of top-down (lithographic) and bottom-up (synthetic chemical) methodologies remains a major goal in nanoscience. At larger length scales, light-directed chemical synthesis, first reported two decades ago, provides a model for this ... ...

Abstract	The integration of top-down (lithographic) and bottom-up (synthetic chemical) methodologies remains a major goal in nanoscience. At larger length scales, light-directed chemical synthesis, first reported two decades ago, provides a model for this integration, by combining the spatial selectivity of photolithography with the synthetic utility of photochemistry. This review describes attempts to realise a similar integration at the nanoscale, by employing near-field optical probes to initiate selective chemical transformations in regions a few tens of nm in size. A combination of near-field exposure and an ultra-thin resist yields exceptional performance: in self-assembled monolayers, an ultimate resolution of 9 nm (ca. λ/30) has been achieved. A wide range of methodologies, based on monolayers of thiols, silanes and phosphonic acids, and thin films of nanoparticles and polymers, have been developed for use on metal and oxide surfaces, enabling the fabrication of metal nanowires, nanostructured polymers and nanopatterned oligonucleotides and proteins. Recently parallel lithography approaches have demonstrated the capacity to pattern macroscopic areas, and the ability to function under fluid, suggesting exciting possibilities for surface chemistry at the nanoscale.
MeSH term(s)	Crystallization/trends ; Light ; Macromolecular Substances/chemistry ; Materials Testing ; Molecular Conformation/radiation effects ; Nanostructures/chemistry ; Nanostructures/radiation effects ; Nanostructures/ultrastructure ; Nanotechnology/trends ; Particle Size ; Photochemistry/trends ; Surface Properties/radiation effects
Chemical Substances	Macromolecular Substances
Language	English
Publishing date	2012-03-21
Publishing country	England
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Review
ZDB-ID	2515664-0
ISSN	2040-3372 ; 2040-3364
ISSN (online)	2040-3372
ISSN	2040-3364
DOI	10.1039/c2nr11458e
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Direct writing of metal nanostructures: lithographic tools for nanoplasmonics research.

Leggett, Graham J

ACS nano

2011 Volume 5, Issue 3, Page(s) 1575–1579

Abstract: Continued progress in the fast-growing field of nanoplasmonics will require the development of new methods for the fabrication of metal nanostructures. Optical lithography provides a continually expanding tool box. Two-photon processes, as demonstrated ... ...

Abstract	Continued progress in the fast-growing field of nanoplasmonics will require the development of new methods for the fabrication of metal nanostructures. Optical lithography provides a continually expanding tool box. Two-photon processes, as demonstrated by Shukla et al. (doi: 10.1021/nn103015g), enable the fabrication of gold nanostructures encapsulated in dielectric material in a simple, direct process and offer the prospect of three-dimensional fabrication. At higher resolution, scanning probe techniques enable nanoparticle particle placement by localized oxidation, and near-field sintering of nanoparticulate films enables direct writing of nanowires. Direct laser "printing" of single gold nanoparticles offers a remarkable capability for the controlled fabrication of model structures for fundamental studies, particle-by-particle. Optical methods continue to provide a powerful support for research into metamaterials.
MeSH term(s)	Crystallization/methods ; Gold/chemistry ; Gold/radiation effects ; Lasers ; Macromolecular Substances/chemistry ; Macromolecular Substances/radiation effects ; Materials Testing ; Molecular Conformation/radiation effects ; Nanostructures/chemistry ; Nanostructures/radiation effects ; Nanostructures/ultrastructure ; Oxidation-Reduction ; Particle Size ; Photography/methods ; Surface Plasmon Resonance/methods ; Surface Properties/radiation effects
Chemical Substances	Macromolecular Substances ; Gold (7440-57-5)
Language	English
Publishing date	2011-03-22
Publishing country	United States
Document type	Comment ; Journal Article
ISSN	1936-086X
ISSN (online)	1936-086X
DOI	10.1021/nn2006442
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Slow polymer diffusion on brush-patterned surfaces in aqueous solution.

Clarkson, Christopher G / Johnson, Alexander / Leggett, Graham J / Geoghegan, Mark

Nanoscale

2019 Volume 11, Issue 13, Page(s) 6052–6061

Abstract: A model system for the investigation of diffusional transport in compartmentalized nanosystems is described. Arrays of "corrals" enclosed within poly[oligo(ethylene glycol)methyl ether methacrylate] (POEGMA) "walls" were fabricated using double-exposure ... ...

Abstract	A model system for the investigation of diffusional transport in compartmentalized nanosystems is described. Arrays of "corrals" enclosed within poly[oligo(ethylene glycol)methyl ether methacrylate] (POEGMA) "walls" were fabricated using double-exposure interferometric lithography to deprotect aminosilane films protected by a nitrophenyl group. In exposed regions, removal of the nitrophenyl group enabled attachment of an initiator for the atom-transfer radical polymerization of end-grafted POEGMA (brushes). Diffusion coefficients for poly(ethylene glycol) in these corrals were obtained by fluorescence correlation spectroscopy. Two modes of surface diffusion were observed: one which is similar to diffusion on the unpatterned surface and a very slow mode of surface diffusion that becomes increasingly important as confinement increases. Diffusion within the POEGMA brushes does not significantly contribute to the results.
Language	English
Publishing date	2019-03-14
Publishing country	England
Document type	Journal Article
ZDB-ID	2515664-0
ISSN	2040-3372 ; 2040-3364
ISSN (online)	2040-3372
ISSN	2040-3364
DOI	10.1039/c9nr00341j
Database	MEDical Literature Analysis and Retrieval System OnLINE

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