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50 items found (0 items not approved), displaying 21 to 30.[First/Prev] 1, 2, 3, 4, 5 [Next/Last]

Instruments / Technical Area	Publication Details	Published
E02-JEM ARM 300CF	Atomic structural catalogue of defects and vertical stacking in 2H/3R mixed polytype multilayer WS 2 pyramids Gyeong Hee Ryu , Jun Chen , Yi Wen , Si Zhou , Ren-jie Chang , Jamie H. Warner Nanoscale 10 DOI: 10.1039/C9NR01783F Diamond Proposal Number(s): [16854] Show Abstract ▼ Abstract: We examine the atomic structure of chemical vapour deposition grown multilayer WS2 pyramids using aberration corrected annular dark field scanning transmission electron microscopy coupled with an in situ heating holder. The stacking orders and specific types of defects after partial degradation by S and W atomic loss at high temperature are resolved layer-by-layer. Our study of an individual WS2 pyramid with at least six layers, reveals a mixed 2H and 3R polytype stacking. Etching occurred both top and bottom of the WS2 pyramid, which aids in determining the exact vertical layer stacking configurations in the thicker regions. We provide an extensive catalogue of the contrast profiles associated with defects in WS2 as a function of layer number and stacking type, as imaged using ADF-STEM. These results provide extensive details about the identification of a wide range of defects in S2 layers, and the unique ADF-STEM contrast patterns that arise from complex multilayer stacking.	May 2019
I20-Scanning-X-ray spectroscopy (XAS/XES)	Extracting structural information of Au colloids at ultra-dilute concentrations: identification of growth during nanoparticle immobilization George F. Tierney , Donato Decarolis , Norli Abdullah , Scott M. Rogers , Shusaku Hayama , Martha Briceno De Gutierrez , Alberto Villa , C. Richard A. Catlow , Paul Collier , Nikolaos Dimitratos , Peter Wells Nanoscale Advances 4 DOI: 10.1039/C9NA00159J Diamond Proposal Number(s): [17283] Open Access Show Abstract ▼ Abstract: Sol-immobilization is increasingly used to achieve supported metal nanoparticles (NPs) with controllable size and shape; it affords a high degree of control of the metal particle size and yields a narrow particle size distribution. Using state-of-the-art beamlines, we demonstrate how X-ray absorption fine structure (XAFS) techniques are now able to provide accurate structural information on nano-sized colloidal Au solutions at μM concentrations. This study demonstrates: (i) the size of Au colloids can be accurately tuned by adjusting the temperature of reduction, (ii) Au concentration, from 50 μM to 1000 μM, has little influence on the average size of colloidal Au NPs in solution and (iii) the immobilization step is responsible for significant growth in Au particle size, which is further exacerbated at increased Au concentrations. The work presented demonstrates that an increased understanding of the primary steps in sol-immobilization allows improved optimization of materials for catalytic applications.	May 2019
I22-Small angle scattering & Diffraction	A template-free and low temperature method for the synthesis of mesoporous magnesium phosphate with uniform pore structure and high surface area Jorn Hovelmann , Tomasz M. Stawski , Rogier Besselink , Helen M. Freeman , Karen M. Dietmann , Sathish Mayanna , Brian R. Pauw , Liane G. Benning Nanoscale 11, 6939 - 6951 DOI: 10.1039/C8NR09205B Diamond Proposal Number(s): [16256] Open Access Show Abstract ▼ Abstract: Mesoporous phosphates are a group of nanostructured materials with promising applications, particularly in biomedicine and catalysis. However, their controlled synthesis via conventional template-based routes presents a number of challenges and limitations. Here, we show how to synthesize a mesoporous magnesium phosphate with a high surface area and a well-defined pore structure through thermal decomposition of a crystalline struvite (MgNH4PO4·6H2O) precursor. In a first step, struvite crystals with various morphologies and sizes, ranging from a few micrometers to several millimeters, had been synthesized from supersaturated aqueous solutions (saturation index (SI) between 0.5 and 4) at ambient pressure and temperature conditions. Afterwards, the crystals were thermally treated at 70–250 °C leading to the release of structurally bound water (H2O) and ammonia (NH3). By combining thermogravimetric analyses (TGA), scanning and transmission electron microscopy (SEM, TEM), N2 sorption analyses and small- and wide-angle X-ray scattering (SAXS/WAXS) we show that this decomposition process results in a pseudomorphic transformation of the original struvite into an amorphous Mg-phosphate. Of particular importance is the fact that the final material is characterized by a very uniform mesoporous structure with 2–5 nm wide pore channels, a large specific surface area of up to 300 m2 g−1 and a total pore volume of up to 0.28 cm3 g−1. Our struvite decomposition method is well controllable and reproducible and can be easily extended to the synthesis of other mesoporous phosphates. In addition, the so produced mesoporous material is a prime candidate for use in biomedical applications considering that magnesium phosphate is a widely used, non-toxic substance that has already shown excellent biocompatibility and biodegradability.	Apr 2019
I09-Surface and Interface Structural Analysis	Two-dimensional growth of dendritic islands of NTCDA on Cu(001) studied in real time Janina Felter , Markus Franke , Jana Wolters , Caroline Henneke , Christian Kumpf Nanoscale 11, 1798 DOI: 10.1039/C8NR08943D Diamond Proposal Number(s): [13837] Show Abstract ▼ Abstract: The success of future organic electronic devices distinctively depends on the electronic and geometric properties of thin organic films. Although obviously these properties are strongly influenced by the growth mechanisms, real time growth studies are relatively rare since not many experimental techniques exist that allow in situ studies in ultra high vacuum. In this context, we investigated the prototypical system 1,4,5,8-naphtalene-tetracarboxylic-dianhydride (NTCDA) on Cu(001). We used low-energy electron microscopy (LEEM) for the real-time growth study, and a variety of other techniques for investigating the geometric and electronic structure. While for similar model systems well known and well characterized growth modi occur (e.g., compact, well ordered islands or disordered, gas-like layers), for NTCDA/Cu(001) we observe the growth of dendrite-like, fractal structures. The dendritic structures arise from a strongly preferred one-dimensional growth mode forming a long-range ordered network of thin molecular chains spanning over the entire surface already at small coverages. Later in the growth process, the voids in the network structure are incrementally filled. These results are very unexpected for such a simple adsorbate system consisting of well investigated components, the properties of which were believed to be already well understood. We explain this unexpected behavior by a dendritic growth model that is supported by energetic arguments based on pair-potential calculations. These calculations give reason for the experimentally observed growth of one-dimensional structures, and therefore represent the key to a semi-quantitative understanding of this dendritic growth mode.	Jan 2019
E02-JEM ARM 300CF	In situ high temperature atomic level dynamics of large inversion domain formations in monolayer MoS 2 Jun Chen , Si Zhou , Yi Wen , Gyeong Hee Ryu , Christopher Allen , Yang Lu , Angus I. Kirkland , Jamie H. Warner Nanoscale 27 DOI: 10.1039/C8NR08821G Show Abstract ▼ Abstract: Here we study the high-temperature formation and dynamics of large inversion domains (IDs) that form in monolayer MoS2 using atomic-resolution annular dark-field scanning transmission electron microscopy (ADF-STEM) with an in situ heating stage. We use temperatures above 700 °C to thermally activate rapid S vacancy migration and this leads to a formation mechanism of IDs that differs from the one at room temperature, where S vacancy migration is limited. We show that at high temperatures the formation of IDs occurs from intersected networks of long S vacancy line defects, whose strain fields are non-orthogonal and trigger large scale atomic reconstructions. Once formed, the IDs are influenced by the dynamic behaviour of nearby line defects and voids. With Mo and S atoms undergoing movement, the two types of ID grain boundaries can shift to allow further expansion of the ID area along the adjoining line defects. We reveal that IDs serve as metastable configurations between line defect rearrangements and eventual void formation under electron beam irradiation during heating. The formation of voids near to the IDs causes them to revert back to pristine lattice, which has the effect of restricting the ID domain size to a certain range (e.g. 3–5 nm in our observation) instead of continuously enlarging. This study provides insights into how the MoS2 IDs form and evolve at high temperature and can benefit the tailoring of electronic properties of two dimensional materials by structural manipulation.	Jan 2019
I09-Surface and Interface Structural Analysis	Quantitative determination of a model organic/insulator/metal interface structure Martin Schwarz , David A. Duncan , Manuela Garnica , Jacob Ducke , Peter S. Deimel , Pardeep K. Thakur , Tien-lin Lee , Francesco Allegretti , Willi Auwärter Nanoscale 28 DOI: 10.1039/C8NR06387G Diamond Proposal Number(s): [14624] Open Access Show Abstract ▼ Abstract: By combining X-ray photoelectron spectroscopy, X-ray standing waves and scanning tunneling microscopy, we investigate the geometric and electronic structure of a prototypical organic/insulator/metal interface, namely cobalt porphine on monolayer hexagonal boron nitride (h-BN) on Cu(111). Specifically, we determine the adsorption height of the organic molecule and show that the original planar molecular conformation is preserved in contrast to the adsorption on Cu(111). In addition, we highlight the electronic decoupling provided by the h-BN spacer layer and find that the h-BN–metal separation is not significantly modified by the molecular adsorption. Finally, we find indication of a temperature dependence of the adsorption height, which might be a signature of strongly-anisotropic thermal vibrations of the weakly bonded molecules.	Nov 2018
E02-JEM ARM 300CF	Atomically sharp interlayer stacking shifts at anti-phase grain boundaries in overlapping MoS 2 secondary layers Si Zhou , Shanshan Wang , Zhe Shi , Hidetaka Sawada , Angus I. Kirkland , Ju Li , Jamie H. Warner Nanoscale 13 DOI: 10.1039/C8NR04486D Show Abstract ▼ Abstract: When secondary domains nucleate and grow on the surface of monolayer MoS2, they can extend across grain boundaries in the underlying monolayer MoS2 and form overlapping sections. We present an atomic level study of overlapping antiphase grain boundaries (GBs) in MoS2 monolayer-bilayers using aberration-corrected annular dark field scanning transmission electron microscopy. In particular we focus on the antiphase GB within a monolayer and track its propagation through an overlapping bilayer domain. We show that this leads to an atomically sharp interface between 2H and 3R interlayer stacking in the bilayer region. We have studied the micro-nanoscale “meandering” of the antiphase GB in MoS2, which shows a directional dependence on the density of 4 and 8 member ring defects, as well as sharp turning angles 90°–100° that are mediated by a special 8-member ring defect. Density functional theory has been used to explore the overlapping interlayer stacking around the antiphase GBs, confirming our experimental findings. These results show that overlapping secondary bilayer MoS2 domains cause atomic structure modification to underlying anti-phase GB sites to accommodate the van der Waals interactions.	Aug 2018
I09-Surface and Interface Structural Analysis	Re-evaluating how charge transfer modifies the conformation of adsorbed molecules P. J. Blowey , S. Velari , L. A. Rochford , Da. A. Duncan , D. A. Warr , T.-l. Lee , A. De Vita , G. Costantini , D. P. Woodruff Nanoscale 4 DOI: 10.1039/C8NR02237B Diamond Proposal Number(s): [8436] Open Access Show Abstract ▼ Abstract: The archetypal electron acceptor molecule, TCNQ, is generally believed to become bent into an inverted bowl shape upon adsorption on the coinage metal surfaces on which it becomes negatively charged. New quantitative experimental structural measurements show that this is not the case for TCNQ on Ag(111). DFT calculations show that the inclusion of dispersion force corrections reduces not only the molecule-substrate layer spacing but also the degree of predicted molecular bonding. However, complete agreement between experimentally-determined and theoretically-predicted structural parameters is only achieved with the inclusion of Ag adatoms into the molecular layer, which is also the energetically favoured configuration. The results highlight the need for both experimental and theoretical quantitative structural methods to reliably understand similar metal–organic interfaces and highlight the need to re-evaluate some previously-investigated systems.	Jul 2018
B21-High Throughput SAXS	An acid-compatible co-polymer for the solubilization of membranes and proteins into lipid bilayer-containing nanoparticles Stephen C. L. Hall , Cecilia Tognoloni , Jack Charlton , Eilis C. Bragginton , Alice J. Rothnie , Pooja Sridhar , Mark Wheatley , Timothy J. Knowles , Thomas Arnold , Karen J. Edler , Tim R. Dafforn Nanoscale DOI: 10.1039/C8NR01322E Diamond Proposal Number(s): [9727] Open Access Show Abstract ▼ Abstract: The fundamental importance of membrane proteins in drug discovery has meant that membrane mimetic systems for studying membrane proteins is of increasing interest. One such system has been the amphipathic, negatively charged poly(styrene-co-maleic acid) (SMA) polymer to form “SMA Lipid Particles” (SMALPs) which have been widely adopted to solubilize membrane proteins directly from the cell membrane. However, SMALPs are only soluble under basic conditions and precipitate in the presence of divalent cations required for many downstream applications. Here, we show that the positively charged poly(styrene-co-maleimide) (SMI) forms similar nanoparticles with comparable efficiency to SMA, whilst remaining functional at acidic pH and compatible with high concentrations of divalent cations. We have performed a detailed characterization of the performance of SMI that enables a direct comparison with similar data published for SMA. We also demonstrate that SMI is capable of extracting proteins directly from the cell membrane and can solubilize functional human G-protein coupled receptors (GPCRs) expressed in cultured HEK 293T cells. “SMILPs” thus provide an alternative membrane solubilization method that successfully overcomes some of the limitations of the SMALP method.	May 2018
I07-Surface & interface diffraction	Efficient long - range electron transfer processes in polyfluorene – perylene diimide blends Anna Isakova , Safakath Karuthedath , Thomas Arnold , Jonathan R. Howse , Paul D. Topham , Daniel T. W. Toolan , Frédéric Laquai , Larry Lüer Nanoscale DOI: 10.1039/C8NR01064A Diamond Proposal Number(s): [16697] Show Abstract ▼ Abstract: In bulk heterojunction donor-acceptor (D-A) blends, high photovoltaic yields require charge carrier separation to outcompete geminate recombination. Recently, evidence for long-range electron transfer mechanisms has been presented, avoiding strongly-bound interfacial charge transfer (CT) states. However, due to the lack of specific optical probes at the D-A interface, a detailed quantification of the long-range processes has not been feasible, until now. Here, we present a transient absorption study of long-range processes in a unique phase consisting of perylene diimide (PDI) crystals intercalated with polyfluorene (PFO), as widely used non-fullerene electron acceptor and donor, respectively. The intercalated PDI:PFO phase possesses specific well-separated spectral features for the excited states at the D-A interface. By use of femtosecond spectroscopy we reveal the excitation dynamics in this blend. PDI excitons undergo a clear symmetry-breaking charge separation in the PDI bulk, which occurs within several hundred femtoseconds, thus outcompeting excimer formation, known to limit charge separation yields when PDI is used as an acceptor. In contrast, PFO excitons are dissociated with very high yields in a one-step long-range process, enabled by large delocalization of the PFO exciton wavefunction. Moreover, both scenarios circumvent the formation of strongly-bound interfacial CT states and enable a targeted interfacial design for bulk heterojunction blends with near unity charge separation yields.	May 2018

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