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| Open AccessTrapping gases in metal-organic frameworks with a selective surface molecular barrier layer
Metal-organic frameworks are extensively studied for gas storage applications, but one potential limitation is their relatively weak adsorption of gases. Here, the authors report that the exposure of metal-organic frameworks to ethylenediamine forms a monolayer thick cap which improves gas molecule retention.
- Kui Tan
- , Sebastian Zuluaga
- & Yves J. Chabal
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Article
| Open AccessConditional repair by locally switching the thermal healing capability of dynamic covalent polymers with light
Healable materials are typically repaired by heat, which can affect the properties of the substance. Here the authors report a dynamic covalent polymer network in which light can switch the healing abilities on or off, allowing healing at defined locations without affecting the polymer as a whole.
- Anne Fuhrmann
- , Robert Göstl
- & Stefan Hecht
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Article
| Open AccessEngineering the magnetic coupling and anisotropy at the molecule–magnetic surface interface in molecular spintronic devices
Controlling the magnetic response of a molecular device is important for spintronic applications. Here the authors report the self-assembly, magnetic coupling, and anisotropy of two transition metal complexes bound to a ferrimagnetic surface, and probe the role of the nature of the transition metal ion.
- Victoria E. Campbell
- , Monica Tonelli
- & Talal Mallah
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Article
| Open AccessAn ultra-tunable platform for molecular engineering of high-performance crystalline porous materials
Synthetic design of crystalline porous materials is important for applications such as catalysis and adsorption. Here, the authors demonstrate a platform for the development of crystalline porous materials with a variety of organic ligands and metallic clusters, and control of their gas sorption properties.
- Quan-Guo Zhai
- , Xianhui Bu
- & Pingyun Feng
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Article
| Open AccessKaleidoscopic imaging patterns of complex structures fabricated by laser-induced deformation
Complex surface micro- and nanostructures can be useful in many device applications, but are challenging in terms of controllability, low cost and high throughput. Here the authors have fabricated quasi 3D structures by the thermal deformation of simple two-dimensional laser-induced patterns.
- Haoran Zhang
- , Fengyou Yang
- & Qian Liu
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Article
| Open AccessA grand unified model for liganded gold clusters
There is no one theoretical model that can explain the stability of all known liganded gold clusters. Here, the authors present a grand unified model, inspired by the quark model of particle physics, which describes gold clusters as combinations of stable triangular Au3(2e) and tetragonal Au4(2e) ‘composite particles’ built from gold atom ‘elementary particles’.
- Wen Wu Xu
- , Beien Zhu
- & Yi Gao
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Article
| Open AccessAll-gas-phase synthesis of UiO-66 through modulated atomic layer deposition
Thin films of metal-organic frameworks (MOFs) are promising for catalysis, gas storage, and microelectronics. Here, the authors introduce a vapour-phase synthesis of UiO-66 thin films, beginning with modulated atomic layer deposition of porous, amorphous films, followed by acetic acid vapour-enabled crystallization to the MOF structure.
- Kristian Blindheim Lausund
- & Ola Nilsen
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Article
| Open Access3D visualization of additive occlusion and tunable full-spectrum fluorescence in calcite
Introducing organic guests to a crystal is a convenient way to tailor its properties. Here, the authors occlude fluorescent dyes within calcite to reveal that additives can occupy distinct zones of a crystal, and strategically embed green, blue, and red dyes to create white fluorescent calcite.
- David C. Green
- , Johannes Ihli
- & Fiona C. Meldrum
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Article
| Open AccessStructure-conserving spontaneous transformations between nanoparticles
Ambient chemical transformations between nanoparticles are poorly explored in materials science. Here, the authors find that two atomically precise, isomorphic clusters of gold and silver can convert between each other in solution through a series of alloy clusters, preserving structure, topology, and metal-ligand stoichiometry.
- K. R. Krishnadas
- , Ananya Baksi
- & Thalappil Pradeep
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Article
| Open AccessCharge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks
Porous materials for aqueous contaminant removal are common, but there are few examples of size and charge-dependent separation. Here, the authors report the charge-specific size-dependent separation of water-soluble molecules through a polymeric network where fluorines are the predominant surface groups.
- Jeehye Byun
- , Hasmukh A. Patel
- & Cafer T. Yavuz
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Article
| Open AccessOrigin and structure of polar domains in doped molecular crystals
Doping can introduce structural distortions in a molecular crystal in the form of polar domains. Here, the authors combine pyroelectric measurements and computation to reveal the molecular structure of such domains in centrosymmetric α-glycine crystals doped with L-amino acids.
- E. Meirzadeh
- , I. Azuri
- & I. Lubomirsky
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Article
| Open AccessRapid and reversible photoinduced switching of a rotaxane crystal
Crystalline phase transition can be used to detect changes in the solid state properties of materials. Here, the authors describe the mechanical response of a crystal composed of ferrocene-containing rotaxane to laser irradiation.
- Kai-Jen Chen
- , Ya-Ching Tsai
- & Masaki Horie
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Article
| Open AccessTowards first-principles molecular design of liquid crystal-based chemoresponsive systems
Nematic liquid crystals have potential as sensors for various molecules. Here, the authors present a computational chemistry model for describing the detection of a warfare agent by liquid crystals, opening the door for the atomic-scale design of sensitive and selective chemoresponsive systems.
- Luke T. Roling
- , Jessica Scaranto
- & Manos Mavrikakis
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Article
| Open AccessImparting amphiphobicity on single-crystalline porous materials
The inherent instabilities of metal-organic frameworks (MOFs) in the presence of water or organic compounds have limited their real-world applicability. Here, Ma and co-workers present a coating strategy to fabricate MOFs with amphiphobic surfaces, simultaneously protecting them from moisture and organic vapours.
- Qi Sun
- , Hongming He
- & Shengqian Ma
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Article
| Open AccessDonor polymer design enables efficient non-fullerene organic solar cells
In organic photovoltaics, electron acceptors are developed to replace fullerenes, and new donors need to be designed to match these acceptors. Here, the authors show that a polymer with strong temperature dependent aggregation and intentionally reduced crystallinity matches non-fullerene acceptors.
- Zhengke Li
- , Kui Jiang
- & He Yan
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Article
| Open AccessOrdered fragmentation of oxide thin films at submicron scale
Fracture and related processes are typically considered detrimental, but have also attracted interest in more constructive roles. Here authors demonstrate ordered fragmentation at submicron scales of a metal oxide/hydroxide thin film by introducing preferential sites for fracture on the underlying substrate.
- L. Guo
- , Y. Ren
- & S. Y. Chiam
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Article
| Open AccessFlexible ferroelectric organic crystals
Mechanical flexibility gives organic ferroelectric materials a potential advantage over their inorganic counterparts, yet it is challenging to produce them. Owczareket al. report flexible crystals based on trisubstituted haloimidazoles that show both ferroelectric and piezoelectric properties.
- Magdalena Owczarek
- , Karl A. Hujsak
- & J. Fraser Stoddart
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Article
| Open AccessMetal-free photochemical silylations and transfer hydrogenations of benzenoid hydrocarbons and graphene
Baird’s rules say that the first triplet state of benzene displays antiaromatic character. Here, the authors exploit this to show that aromatic molecules can undergo rapid transfer hydrogenation or silylations without the need for metal catalysts when photochemcially excited into this state.
- Raffaello Papadakis
- , Hu Li
- & Henrik Ottosson
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Article
| Open AccessMulticolour synthesis in lanthanide-doped nanocrystals through cation exchange in water
De novosynthesis is the primary way to tune the emission colour of lanthanide-doped upconversion nanocrystals. Here, the authors introduce post-synthetic cation exchange as a strategy to access multiple colours of luminescent nanocrystals, preserving the size and morphology of the original template.
- Sanyang Han
- , Xian Qin
- & Xiaogang Liu
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Article
| Open AccessOscillating edge states in one-dimensional MoS2 nanowires
Unusual properties arise in transition metal dichalcogenides as dimensionality decreases. Here, the authors introduce a templated growth approach to precisely control the width of MoS2nanowires on a substrate, allowing them to reveal a relationship between size and electronic properties.
- Hai Xu
- , Shuanglong Liu
- & Kian Ping Loh
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Article
| Open AccessStructural and quantum chemical analysis of exciton coupling in homo- and heteroaggregate stacks of merocyanines
Exciton coupling between organic dyes is important for opto-electronic and photovoltaic devices and it is well-known that strong coupling occurs between equal chromophores. Here, Würthner and others show quadruple dye stacks that have strong exciton coupling between different chromophores within a heteroaggregate.
- David Bialas
- , André Zitzler-Kunkel
- & Frank Würthner
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Article
| Open AccessEngineering island-chain silicon nanowires via a droplet mediated Plateau-Rayleigh transformation
The ability to program periodic morphology into nanowires affords control over photonic and electronic transport properties. Here, the authors stimulate Plateau-Rayleigh transformations in silicon nanowires through an oscillating catalyst droplet, resulting in nanowires with island-chain morphology.
- Zhaoguo Xue
- , Mingkun Xu
- & Pere Roca i Cabarrocas
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Article
| Open AccessA novel perovskite oxide chemically designed to show multiferroic phase boundary with room-temperature magnetoelectricity
Structural change at multiferroic phase boundary is anticipated to have an associated large magnetoelectric response, which yet awaits to be evidenced. Here, Fernández-Posada et al. report electric field-induced phase change for a BiFeO3–BiMnO3–PbTiO3solid solution with distinctive magnetic signature.
- Carmen M. Fernández-Posada
- , Alicia Castro
- & Harvey Amorín
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Article
| Open AccessProgramming temporal shapeshifting
Actuation of shape-shifting materials has typically required an external trigger. Here, the authors design a shape-memory hydrogel, regulated by a dual network of covalent and temporary hydrogen bonds, whose actuations are encoded by an intrinsic temporal mechanism.
- Xiaobo Hu
- , Jing Zhou
- & Sergei S. Sheiko
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Article
| Open AccessMolecular transport through large-diameter DNA nanopores
Artificial DNA membrane channels are promising molecular devices for biotechnology but suffer from low affinity for lipid bilayers. Here, the authors report a large DNA nanopore that spontaneously inserts into a flat lipid membrane, driven by engineered hydrophobic or streptavidin-biotin interactions.
- Swati Krishnan
- , Daniela Ziegler
- & Friedrich C. Simmel
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Article
| Open AccessThree-dimensional protonic conductivity in porous organic cage solids
Proton conduction is a fundamental process for fuel cell development, but three-dimensional proton conduction in crystalline porous solids is rare. Here, the authors report organic molecular cages in which the structure imposes three-dimensional proton conductivity competing with metal-organic frameworks.
- Ming Liu
- , Linjiang Chen
- & Andrew I. Cooper
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Article
| Open AccessSimple direct formation of self-assembled N-heterocyclic carbene monolayers on gold and their application in biosensing
Self-assembled monolayers (SAMs) have shown tremendous number of applications but can suffer from low stability. Here, the authors report air and bench stable carbene precursors allowing facile SAM formation, and furthermore demonstrate an application in biosensing
- Cathleen M. Crudden
- , J. Hugh Horton
- & Akiko Yagi
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Article
| Open AccessShaping polymersomes into predictable morphologies via out-of-equilibrium self-assembly
Polymersomes are used in many applications, ranging from drug delivery to microfluidics, but controlling their shape is difficult. Here, Christianen and co-workers have precisely controlled polymersome shape via an out-of-equilibrium process and fully understood the mechanism of this procedure.
- R. S. M. Rikken
- , H. Engelkamp
- & P. C. M. Christianen
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Article
| Open AccessHeterogeneous reduction of carbon dioxide by hydride-terminated silicon nanocrystals
Elemental silicon is widely studied for photovoltaic applications. Here, the authors report that hydride-terminated silicon nanocrystals can also function as single component heterogeneous reducing agent for converting gaseous carbon dioxide selectively to carbon monoxide.
- Wei Sun
- , Chenxi Qian
- & Geoffrey A. Ozin
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Article
| Open AccessMicrofibres and macroscopic films from the coordination-driven hierarchical self-assembly of cylindrical micelles
Anisotropic nanoparticles made from block copolymers are important building blocks for synthetic hierarchical materials. Here, the authors report a reversible coordination-driven self-assembly strategy for the preparation of micron-scale fibres and macroscopic films based on monodisperse cylindrical micelles.
- David J. Lunn
- , Oliver E. C. Gould
- & Ian Manners
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Article
| Open AccessCore-shell nanoscale coordination polymers combine chemotherapy and photodynamic therapy to potentiate checkpoint blockade cancer immunotherapy
Blockade of PD-L1 is usually not very effective in colon cancer patients. Here, the authors show the efficacy of PD-L1 blockade in combination with coordination polymer nanoparticles carrying oxaliplatin and a photosensitizer to induce anti-tumor immunity in metastatic models of colon cancer.
- Chunbai He
- , Xiaopin Duan
- & Wenbin Lin
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Article
| Open AccessA robust molecular probe for Ångstrom-scale analytics in liquids
Single-molecule-terminated scanning probes typically operate under ultra-high vacuum conditions at low temperatures. Here, the authors show that tips functionalized with C60 can image single-layer graphene and MoS2with high definition in a liquid environment at room temperature
- Peter Nirmalraj
- , Damien Thompson
- & Heike Riel
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| Open AccessSelective directed self-assembly of coexisting morphologies using block copolymer blends
There is a limited range of structures available in nanolithography using directed self-assembled block copolymers. Here, Black and co-workers expand directed self-assembly chemical patterning by using a blend of lamellar and cylinder forming block copolymers on surface chemical line gratings.
- A. Stein
- , G. Wright
- & C. T. Black
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Article
| Open AccessChemical control over the energy-level alignment in a two-terminal junction
Energy alignment in molecular tunnelling junctions is desirable for altering their electrical properties, however controllability is still an issue. Here the authors report a 2 orders-of-magnitude increase in the tunnelling current via chemical control of the energy-level alignment at a two-terminal junction.
- Li Yuan
- , Carlos Franco
- & Christian A. Nijhuis
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Article
| Open AccessThe crucial effect of early-stage gelation on the mechanical properties of cement hydrates
The origins of the unique properties of cement are poorly understood. Using simulations the authors show that the early formation of a soft nano-particle gel, followed by slow densification, plays a crucial role in giving cement its unique mechanical properties.
- Katerina Ioannidou
- , Matej Kanduč
- & Emanuela Del Gado
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Article
| Open AccessA chaotic self-oscillating sunlight-driven polymer actuator
It is highly desirable, yet challenging to build actuators in a dry environment that can undergo autonomous oscillation. Here, Kumar et al.achieve this goal in a soft actuator based on the use of a nematic liquid crystal film doped by ortho-fluoroazobenzene that is responsive to sunlight.
- Kamlesh Kumar
- , Christopher Knie
- & Albertus P. H. J. Schenning
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Article
| Open AccessSuper stretchable hydrogel achieved by non-aggregated spherulites with diameters <5 nm
Hydrogels containing nanoparticles have enhanced mechanical properties that can be limited if the size of the crosslinking nanoparticles is too large. Here, Zhang and others have produced non-aggregated spherulite nanoparticles with diameters of less than 5 nm and investigated their effect on hydrogels.
- Guoxing Sun
- , Zongjin Li
- & Lina Zhang
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Article
| Open AccessStructural lubricity under ambient conditions
Structural lubricity—referring to ultralow levels of friction between atomically flat, incommensurate surfaces—has previously been observed under ultrahigh vacuum. Here, the authors report structural lubricity at gold-graphite interfaces under ambient conditions and on mesoscopic scales.
- Ebru Cihan
- , Semran İpek
- & Mehmet Z. Baykara
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Article
| Open AccessA facile route to old and new cyclophanes via self-assembly and capture
Cyclophanes—consisting of aromatic rings formed into a macrocycle—can display interesting properties but are challenging targets for synthesis. Here, the authors report a route to form cyclophanes by dynamic covalent chemistry, forming disulfides that can be subsequently converted to stable thioethers.
- Mary S. Collins
- , Matthew E. Carnes
- & Darren W. Johnson
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Article
| Open AccessTowards controlled polymer brushes via a self-assembly-assisted-grafting-to approach
Polymer brushes, whereby single layers of polymers are tethered to surfaces, can be made by various methods but greater control over their fabrication is desirable. Here, by pre-assembling polymer chains into 2D crystalline sheets, the authors achieve high precision and unprecedented grafting densities.
- Tian Zhou
- , Hao Qi
- & Christopher Y. Li
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Article
| Open AccessOptically responsive supramolecular polymer glasses
The ability to heal whilst maintaining original functionality is important for establishing materials with superior longevity. Here, the authors demonstrate a supramolecular polymeric coating which exhibits excellent optical and mechanical properties, even following damage repair.
- Diederik W. R. Balkenende
- , Christophe A. Monnier
- & Christoph Weder
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Article
| Open AccessPolarized three-photon-pumped laser in a single MOF microcrystal
Higher-order multi-photon pumped polarized lasers promise application in future optoelectronic and biomedical applications. Here, the authors demonstrate a polarized three-photon pumped (3PP) microcavity laser in a single host-guest composite MOF crystal via a controllable in situ self-assembly strategy.
- Huajun He
- , En Ma
- & Guodong Qian
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Article
| Open AccessPhotoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics
Aerosol droplets have significant effects on atmospheric photochemistry, however measuring absorption from single droplets is a challenge. Here, the authors report a method to measure absorption of nanodroplets with attolitre sensitivity, showing rate enhancements for light focusing in photolysis reactions.
- Johannes W. Cremer
- , Klemens M. Thaler
- & Ruth Signorell
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Article
| Open AccessNon-equilibrium behaviour in coacervate-based protocells under electric-field-induced excitation
Synthetic cells are designed to mimic basic life processes, but it is challenging to prepare cells that can persist and operate at non-equilibrium conditions. Here, Yin et al.show complex dynamical behaviors of protocells made by exposing polylysine and single-stranded DNA droplets to an electric field.
- Yudan Yin
- , Lin Niu
- & Dehai Liang
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Article
| Open AccessHighly robust crystalsome via directed polymer crystallization at curved liquid/liquid interface
Self-assemblies of polymers to form polymersomes in solution can be used as carriers for drug delivery, but it is challenging to control polymer crystallization to improve their mechanical stability. Here, Wang et al.show the formation of nanosized crystalsomes composed of polymer lamellar single crystals.
- Wenda Wang
- , Hao Qi
- & Christopher Y. Li
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Article
| Open AccessHomochiral D4-symmetric metal–organic cages from stereogenic Ru(II) metalloligands for effective enantioseparation of atropisomeric molecules
Homochiral molecular capsules offer potential applications in chiral separation and stereospecific catalysis. Here, by pre-resolution of Δ/Λ-metalloligand precursors, the authors are able to assemble enantiopure supramolecular cages capable of stereoselective host-guest behaviour.
- Kai Wu
- , Kang Li
- & Cheng-Yong Su
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Article
| Open AccessIn vivo covalent cross-linking of photon-converted rare-earth nanostructures for tumour localization and theranostics
Directing nanomedicines to desired locations - such as tumour sites - is difficult to achieve selectively. Here, the authors develop a method to covalently crosslink peptide-modified upconversion nanocrystals into tumour sites for photodynamic therapy and show in vivotumour inhibition in mice.
- Xiangzhao Ai
- , Chris Jun Hui Ho
- & Bengang Xing
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Article
| Open AccessPolyoxometalate-based homochiral metal-organic frameworks for tandem asymmetric transformation of cyclic carbonates from olefins
Using a single catalyst to promote multiple distinct reactions without alteration in reaction conditions is an attractive synthetic goal. Here, to this end, the authors have developed a polyoxometalate-based metal-organic framework for the synthesis of cyclic carbonates from olefins.
- Qiuxia Han
- , Bo Qi
- & Chunying Duan
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Article
| Open AccessThe microscopic structure of charge density waves in underdoped YBa2Cu3O6.54 revealed by X-ray diffraction
Near to the superconducting state, cuprates display spatially-periodic charge density variations. Here, the authors use x-ray diffraction to determine the microscopic structure, showing how charge density waves in underdoped YBa2Cu3O6.54break the symmetry of the superconducting layers.
- E. M. Forgan
- , E. Blackburn
- & S. M. Hayden