Richard A. Campbell's research while affiliated with The University of Manchester and other places

Publications (119)

Article
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We have directly resolved in the present work the interfacial composition during and after the interactions of a saturated atmosphere of oil vapor with soluble surfactant solutions at a planar water/air interface for the first time. Experiments were conducted on interactions of hexane vapor with solutions of alkyltrimethylammonium bromides and sodi...
Article
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Reversible control of the 3D structure of polyelectrolyte/surfactant films at the air/water interface is showcased. A recently discovered mechanism is exploited to form highly efficient, stable and biocompatible films by spreading aggregates composed of poly-L-lysine and sodium dodecyl sulfate on the surface of water. Reversible control of: (1) the...
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Lipid nanoparticles (LNPs) are important delivery systems for RNA-based therapeutics, yet the mechanism of their interaction with endosomal membranes remains unclear. Here, the interactions of nucleic acid-loaded LNPs that contain an ionizable lipid with models of the early and late endosomal membranes are studied, for the first time, using differe...
Article
This paper addresses the effect of polyelectrolyte stiffness on the surface structure of polyelectrolyte (P)/surfactant (S) mixtures. Therefore, two different anionic Ps with different intrinsic persistence length lP are studied while varying the salt concentration (0-10-2 M). Either monosulfonated polyphenylene sulfone (sPSO2-220, lP ∼20 nm) or so...
Article
Hypothesis Self-assembly of amphipathic styrene maleic acid copolymers with phospholipids in aqueous solution results in the formation of ‘nanodiscs’ containing a planar segment of phospholipid bilayer encapsulated by a polymer belt. Recently, studies have reported that lipids rapidly exchange between both nanodiscs in solution and external sources...
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The ageing of organic-coated aqueous aerosols at night is investigated by reacting NO3 with binary surfactant mixtures floating on water. The surfactants are oleic acid (OA), methyl oleate (MO) and...
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The formation of ordered 2D nanostructures of double stranded DNA molecules at various interfaces attracts more and more focus in medical and engineering research, but the underlying intermolecular interactions still require elucidation. Recently, it has been revealed that mixtures of DNA with a series of hydrophobic cationic polyelectrolytes inclu...
Article
Hypothesis Neutral amphiphilic PEG-g-PVAc co-polymer (a “tardigrade” polymer consisting of a hydrophilic polyethylene glycol, PEG, backbone with hydrophobic polyvinyl acetate, PVAc, grafts) can form complexes at the air-water interface with cationic dodecyltrimethylammonium bromide (DTAB) via self-assembly. Compared to anionic SDS, cationic DTAB he...
Article
GS-9695 and GS-9822 are next generation Non-Catalytic Site Integrase Inhibitors (NCINIs) with significantly improved potency against HIV compared with previous drugs such as BI-224436. Development stopped due to vacuolation of the bladder urothelium seen in cynomolgus monkey but not in rat; this lesion was absent in equivalent preclinical studies w...
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Hypothesis Antimicrobial peptides (AMPs) kill microorganisms by causing structural damage to bacterial membranes. Different microorganisms often require a different type and concentration of an AMP to achieve full microbial killing. We hypothesise that the difference is caused by different membrane structure and composition. Experiments Given the...
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Hypothesis: Fluorocarbon gases introduced above monolayers of phospholipids at the air/water interface were recently found to promote the adsorption of diverse molecular compounds, with potential application in drug-loaded microbubble design. Quantitative determination of the fluorocarbon present in the monolayers is strongly needed for the develop...
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Reaction of gas-phase ozone with oleic acid monolayer at the air–water interface leaves no product film. Reaction kinetics change with surface coverage but not with addition of unreactive material or with change of viscosity of the water.
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It is shown that the air–liquid interface can be made to display the same rich curvature phenomena as common lyotropic liquid crystal systems. Through mixing an insoluble, naturally occurring, branched fatty acid, with an unbranched fatty acid of the same length, systematic variation in the packing constraints at the air–water interface could be ob...
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Developing more efficient manufacturing methods for nano therapeutic systems is becoming important, not only to better control their physico-chemical characteristics and therapeutic efficacy but also to ensure scale-up is cost-effective. The principle of cross-flow chemistry allows precise control over manufacturing parameters for the fabrication o...
Preprint
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Arylazopyrazoles (AAPs) as substitutes for azo derivatives have gained considerable attention due to their superior properties offering E/Z photo-isomerization with high yield. In order to compare and quantify their performance, azobenzene tetraethylammonium (Azo-TB) and arylazopyrazole tetraethylammonium (AAP-TB) bromides were synthesized and char...
Article
Arylazopyrazoles (AAPs) as substitutes for azo derivatives have gained considerable attention due to their superior properties offering E/Z photo-isomerization with high yield. In order to compare and quantify their performance, azobenzene tetraethylammonium (Azo-TB) and ar-ylazopyrazole tetraethylammonium (AAP-TB) bromides were synthesized and cha...
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We quantify directly here for the first time the extents of interactions of two different anthracycline drugs with pure and mixed lipid monolayers with respect to the surface pressure and elucidate differences in the resulting interaction mechanisms. The work concerns interactions of doxorubicin (DOx) and idarubicin (IDA) with monolayers of the zwi...
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A simple, insoluble monolayer of fatty acid is shown to induce 3D nanotexturing of the air–water interface. This advance has been achieved through the study of monolayers of a methyl-branched long chain fatty acid, analogous to those found on the surface of hair and wool, directly at the air–water interface. Specular neutron reflectometry combined...
Article
Cellular membranes are complex structures and simplified analogues in the form of model membranes or biomembranes are used as platforms to understand fundamental properties of the membrane itself as well as interactions with various biomolecules such as drugs, peptides and proteins. Model membranes at the air-liquid and solid-liquid interfaces can...
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A novel structural framework is presented to rationalize the foam film stability of polyelectrolyte/surfactant mixtures using neutron reflectivity data. Provision of electrostatic or steric stabilization in thin foam films is related to the spatial distributions of molecules interacting from opposing air/water interfaces. The advance is discussed i...
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Interfaces that can change their chemistry on demand have huge potential for applications and are prerequisite for responsive or adaptive materials. We report on the performance of a newly designed n-butyl-arylazopyrazole butyl sulfonate (butyl-AAP-C4S) surfactant that can change its structure at the air-water interface by E/Z photo-isomerization i...
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This work showcases the remarkable viscoelasticity of films consisting of α-cyclodextrin (α-CD) and anionic surfactants (S) at the water/air interface, the magnitude of which has not been observed in similar systems. The anionic surfactants employed are sodium salts of a homologous series of n-alkylsulfates (n = 8-14) and of dodecylsulfonate. Our h...
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Bare interfaces between water and hydrophobic media like air or oil are of fundamental scientific interest and of great relevance for numerous applications. A number of observations involving water/hydrophobic interfaces have, however, eluded a consensus mechanistic interpretation so far. Recent theoretical studies ascribe these phenomena to an int...
Article
Several characteristics of β-lactoglobulin (BLG) layers adsorbed at the air/water interface exhibit a strong pH dependence, but our knowledge on the underlying structure-property relations is still fragmental. Here, we therefore extend our recent studies by neutron reflectometry (NR) and provide a comprehensive overview through direct measurements...
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Understanding the structure of polymer/surfactant mixtures at the air-water interface is of fundamental importance and also of relevance to a variety of practical applications. Here, the complexation between a neutral 'tardigrade' comb co-polymer (consisting of a hydrophilic polyethylene glycol backbone with hydrophobic polyvinyl acetate grafts, PE...
Article
It is discovered that complexes of DNA and hydrophobically modified polyelectrolytes form a rigid network of threadlike or fibrous aggregates at the liquid – gas interface whose morphology can dramatically affect the mechanical properties. While mixed solutions of DNA and poly(N,N-diallyl-N,N-dimethylammonium chloride) (PDADMAC) exhibit no notable...
Preprint
A simple, insoluble monolayer of fatty acid is shown to induce 3D nanotexturing of the water–air interface. This advance has been achieved through the study of monolayers of a methyl-branched long chain fatty acid, analogous to those found on the surface of hair and wool, directly at the water–air interface. Specular neutron reflectometry combined...
Article
The surface properties of mixed aqueous dispersions of lysozyme and silica nanoparticles were studied using surface-sensitive techniques in order to gain insight into the mechanism of simultaneous adsorption of protein/nanoparticle complexes and free protein as well as the resulting layer morphologies. The properties were first monitored in situ du...
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In this work, we present the first example of the self-assembly of phospholipid monolayers at the interface between air and an ionic solvent. Deep eutectic solvents are a novel class of environmentally friendly non-aqueous room temperature liquids with tunable properties, that have wide ranging potential applications and are capable of promoting th...
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Propofol is an amphiphilic non-surfactant that strongly influences the function of cell membranes, yet data regarding interfacial properties of propofol remains scarce. Here we consider propofol adsorption at the air/water interface as elucidated by means of vibrational sum frequency spectroscopy (VSFS), neutron reflectometry (NR), and surface tens...
Preprint
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In this work, we present the first example of the self-assembly of phospholipid monolayers at the interface between air and a non-aqueous liquid. Deep eutectic solvents are a novel class of environmentally friendly non-aqueous room temperature liquids with tunable properties, that have wide ranging potential applications and are capable of promotin...
Article
Specular neutron reflectometry is a powerful technique to resolve interfacial compositions and structures in soft matter. Surprisingly however, even after several decades, a universal modeling approach for the treatment of data of surfactant and phospholipid monolayers at the air/water interface has not yet been established. To address this shortco...
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This review addresses significant recent advances in kinetic and dynamic studies at the air/water interface using specular neutron reflectometry. A step change in the capabilities to resolve these processes in systems related to soft matter, biophysics, environment and health has been delivered primarily by the FIGARO instrument at the Institut Lau...
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The demand for highly efficient macromolecular drugs, used in the treatment of many severe diseases, is continuously increasing. However, the hydrophilic character and large molecular size of these drugs significantly limit their ability to permeate across cellular membranes and thus impede the drugs in reaching their target sites in the body. Cell...
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The application of protein deuteration and high flux neutron reflectometry has allowed a comparison of the adsorption properties of lysozyme at the air–water interface from dilute solutions with and without strong denaturants, urea and guanidine hydrochloride (GuHCl). The surface excess and adsorption layer thickness were resolved and complemented...
Article
Surface tension and specular neutron reflectivity measurements have been used, for the first time to systematically study both the interfacial structure and composition of monolayers of the soluble surfactant, sodium dodecyl sulfate containing a low-dose, poorly water soluble drug, testosterone enanthate. Modelling of the specular neutron reflectiv...
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Reactions of the key atmospheric nighttime oxidant NO3 with organic monolayers at the air–water interface are used as proxies for the ageing of organic-coated aqueous aerosols. The surfactant molecules chosen for this study are oleic acid (OA), palmitoleic acid (POA), methyl oleate (MO) and stearic acid (SA) to investigate the effects of chain leng...
Article
Reactions of the key atmospheric night-time oxidant NO3 with organic monolayers at the air–water interface are used as proxies for the ageing of organic-coated aqueous aerosols. The surfactant molecules chosen for this study are oleic acid (OA), palmitoleic acid (POA), methyl oleate (MO) and stearic acid (SA) to investigate the effects of chain len...
Article
Vibrational sum frequency spectroscopy (VSFS) complemented by surface pressure isotherm and neutron reflectometry (NR) experiments were employed to investigate the interactions between propofol, a small amphiphilic molecule that currently is the most common general anaesthetic drug, and phospholipid monolayers. A series of biologically relevant sat...
Article
The adsorption of mixtures of poly(diallyldimethylammonium chloride) (PDADMAC) and sodium N-lauroyl-N-methyltaurate (SLMT) at the water / vapor interface has been studied using drop profile tensiometry and neutron reflectometry. This study sheds light on the mechanisms involved in the adsorption of polyelectrolyte – oppositely charged surfactants b...
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Deuteration of biomolecules has a great impact on both quality and scope of neutron scattering experiments. Cholesterol is a major component of mammalian cells, where it plays a critical role in membrane permeability, rigidity and dynamics, and contributes to specific membrane structures such as lipid rafts. Cholesterol is the main cargo in low and...
Article
Polyelectrolyte – surfactant mixtures and their interactions with fluid interfaces are an important research field due to their use in technological applications. Most of the existing knowledge on these systems is based on models in which the polyelectrolyte concentration is around 50 times lower than that used in commercial formulations. The prese...
Article
In this work we demonstrate the ability to tune the formation of extended structures in films of poly(sodium styrene sulfonate)/dodecyltrimethylammonium bromide at the air/water interface through control over the charge/structure of aggregates as well as the ionic strength of the subphase. Our methodology to prepare loaded polyelectrolyte/surfactan...
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Different bacterial types and their living environments can lead to different saturations in the chains of their membrane lipids. Such structural differences may influence the efficacy of antibiotics that target bacterial membranes. In this work, the effects of acyl chain saturation on the binding of an antimicrobial peptide G4 have been examined a...
Article
Interactions between soft interfaces govern the behavior of emulsions and foams and crucially influence the functions of biological entities like membranes. To understand the character of these interactions, detailed insight into the interfaces' structural response in terms of molecular arrangements and conformations is often essential. This requir...
Article
DPPC (dipalmitoylphosphatidylcholine) is a disaturated lipid capable of forming closely packed monolayers at the air–liquid interface of the lung and allows the surface tension within the alveoli to reduce to almost zero and thus prevent alveolar collapse. Carbon nanoparticles are formed in natural and man-made combustion events, including diesel e...
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The thermal responsive behavior of adsorbed layers of diblock copolymers of poly(N-isopropylacrylamide) (PNIPAAM) and poly((3-acrylamidopropyl)trimethylammonium chloride) (PAMPTMA(+)) with γ-cyclodextrin (γ-CD) at the solid/liquid interface has been investigated using three in situ techniques: null ellipsometry, quartz–crystal microbalance with dis...
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This review addresses the advances made with specular neutron reflectometry in studies of aqueous mixtures of polymers and surfactants at fluid interfaces during the last decade. The increase in neutron flux due to improvements in instrumentation has led to routine measurements at the air/water interface that are both faster and involve samples wit...
Article
We have used neutron reflectivity (NR) measurements in combination with dynamic light scattering (DLS), surface tension and ellipsometry, to study the adsoprtion behaviour at the air/water interface of N-isopropylacrylamide-based nanogels as a function of concentration. The data provide clear evidence that the nanogels are adsorbed at the interface...
Article
This work reports a unifying general physical description of the behavior of oppositely charged polyelectrolyte/surfactant mixtures at the air/water interface in terms of equilibrium vs. nonequilibrium extremes. The poly(diallyldimethylammonium chloride)/sodium dodecyl sulfate system with added NaCl at two different bulk polyelectrolyte concentrati...
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Surface and interfacial adsorption of antibody molecules could cause structural unfolding and desorbed molecules could trigger solution aggregation, resulting in the compromise of physical stability.Although antibody adsorption is important and its relevance to many mechanistic processes has been proposed, few techniques can offer direct structural...
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Deep eutectic solvents have shown the ability to promote the self-assembly of surfactants in solution. However, some differences have been found compared with self-assembly in pure water and other polar organic solvents. The behaviour of alkyltrimethylammonium bromides in choline chloride:glycerol deep eutectic solvent has been studied by means of...
Article
Many antibacterial peptides (AMPs) target bacterial membranes and they kill bacteria by causing structural disruptions. One of the fundamental issues however lies in the selective responses of AMPs to different cell membranes as a lack of selectivity can elicit toxic side effects to mammalian host cells. A key difference between the outer surfaces...
Article
Reversed lipid liquid crystalline nanoparticles (LCNPs) of the cubic micellar (I2) phase have high potential in drug delivery applications due to their ability to encapsulate both hydrophobic and hydrophilic drug molecules. Their interactions with various interfaces, and the consequences for the particle structure and integrity, are essential consi...
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The spontaneous aggregation of α-cyclodextrin (α-CD) molecules in the bulk aqueous solution and the interactions of the resulting aggregates at the liquid/air interface have been studied at 283 K and 298 K using a battery of techniques, namely transmission electron microscopy, dynamic light scattering, isothermal titration calorimetry, dynamic surf...
Article
Knowledge of the (supra)molecular structure of an interface that contains amphiphilic ligand molecules is necessary for a full understanding of ion transfer during solvent extraction. Even if molecular dynamics already yield some insight in the molecular configurations in solution, hardly any experimental data giving access to distributions of both...
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Knowledge of the (supra)molecular structure of an interface that contains amphiphilic ligand molecules is necessary for a full understanding of ion transfer during solvent extraction. Even if molecular dynamics already yield some insight in the molecular configurations in solution, hardly any experimental data giving access to distributions of both...
Article
We describe a new methodology to prepare loaded polyelectrolyte/surfactant films at the air/water interface by exploiting Marangoni spreading resulting from the dynamic dissociation of hydrophobic neutral aggregates dispensed from an aqueous dispersion. The system studied is mixtures of poly(sodium styrene sulfonate) with dodecyl trimethylammonium...
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The development of effective transdermal drug delivery systems based on nanosized polymers requires a better understanding of the behaviour of such nanomaterials at interfaces. N-Isopropylacrylamide-based nanogels synthesized with different percentages of N,N'-methylenebisacrylamide as cross-linker, ranging from 10 to 30%, were characterized at phy...
Article
The combined application of neutron reflectometry (NR) and ellipsometry to determine the oxidation kinetics of organic monolayers at the air–water interface is described for the first time. This advance was possible thanks to a new miniaturised reaction chamber that is compatible with the two techniques and has controlled gas delivery. The rate coe...
Article
Reflectometry is a powerful technique for determining many physical quantities of stratified media, including length scales, densities and magnetism. However, experimentally neutron reflectometry in particular suffers from the relatively feeble brilliance of the sources compared with those of X-rays, for example. In this paper, a simple modificatio...
Article
It has been known for almost one hundred years that a lower surface tension can be achieved at the air-water interface by spreading protein from a concentrated solution than by adsorption from an equivalent total bulk concentration. Nevertheless the factors that control this non-equilibrium process have not been fully understood. In the present wor...
Article
Lung surfactant protein B (SP-B) is an essential protein found in the surfactant fluid at the air-water interface of the lung. Exposure to the air pollutant ozone could potentially damage SP-B and lead to respiratory distress. We have studied two peptides, one consisting of the N-terminus of SP-B [SP-B(1-25)] and the other a construct of the N- and...
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We have resolved the molecular structure of a bulk oil/water interface that contains amphiphilic ligand molecules using a combination of X-ray and neutron reflectivity measurements for the first time. This new capability can greatly impact future work in the field of ion separation by phase transfer, i.e. liquid/liquid extraction.
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We describe the formation and structure of nucleolipid-dendrimer multilayer films controlled by non-covalent interactions to obtain biomaterials that exhibit molecular recognition of nucleic acids. Layers of cationic poly(amidoamine) (PAMAM) dendrimers of generation 4 and the anionic nucleolipids 1,2-dilauroyl-sn-glycero-3-phosphatidylnucleosides (...
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A study of the dilational surface viscoelastic properties of mixed solutions of lysozyme and denaturing agents of different chemical nature allows us to characterize the changes of protein tertiary structure in the surface layer upon adsorption at the liquid–gas interface. We show that guanidine hydrochloride (GuHCl) and urea influence the dynamic...
Article
We have studied the oppositely charged polyelectrolyte/surfactant mixture of poly (acrylamidomethyl propanesulfonate) sodium salt (PAMPS) and tetradecyl trimethyl ammonium bromide (C14TAB) using a combination of neutron reflectivity and ellipsometry measurements. The interfacial composition was determined using three different analysis methods invo...
Article
We have determined how the bulk behavior of mixtures of small cationic poly(amidoamine) dendrimers (generation 2, PAMAM-G2) and sodium dodecyl sulfate (SDS) affects the structure and composition of the adsorbed layers at the air-water interface. The aim is to reveal how the size of a well-defined hyperbranched polyelectrolyte affects the interfacia...
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We show for the first time that 1,2-dilauroyl-sn-glycero-3-phosphatidyladenosine nucleolipid surface complexes with cationic poly(amidoamine) dendrimers can be used to selectively bind DNA including oligonucleotides. This molecular recognition has high potential for applications involving biomedical and bioanalytic devices as well as drug delivery...