Publications
Publications:
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Simulation of Bragg coherent diffraction imaging J. Phys. Commun. Volume 6, 055003 (2022) The arrangement of atoms within a crystal and information on deviations from the ideal lattice is encoded in the diffraction pattern obtained from an appropriately conducted Bragg coherent diffraction imaging (BCDI) experiment. A foreknowledge of how specific displacements of atoms within the unit cell alter the BCDI diffraction pattern and the subsequent real-space image is often useful for interpretation and can provide valuable insight for materials design. Here we report on an atomistic approach to efficiently simulate BCDI diffraction patterns by factorising and eliminating certain redundancies in the conventional approach. Our method is able to reduce the computation time by several orders of magnitude without compromising the recovered phase information and therefore enables feasible atomistic simulations on nanoscale crystals with arbitrary lattice distortions. |
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UK-XFEL Science Case STFC Following the Strategic FEL Review in 2016, this draft science case, led by Professor Jon Marangos (Imperial College) sets out the scientific rationale for a potential sovereign machine in the UK. |
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Concurrent phase retrieval for imaging strain in nanocrystals Phys. Rev. B Volume 102, 014104 (2020) Coherent diffraction imaging is a form of microscopy that permits high resolution imaging of atomic displacements from equilibrium where the use of conventional optics is not feasible. Approaches to date for the recovery of atomic displacements from equilibrium and subsequently strain information occur after phase reconstruction of the complex real-space images from at least three independent Bragg diffraction amplitude measurements. While this is a more accessible and effective approach to recover strain information, there is potential for erroneous results if the recovered phase information is not carefully treated. Here we present a strategy for imaging strain with coherent x rays that eliminates the technical challenges that exist in conventional approaches by constructing the strain field concurrently during the phase retrieval process of recovering phase information. |
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Coherent diffraction imaging of a progressively deformed nanocrystal Phys. Rev. Materials, Volume 3, 043803 (2019) Imaging ordered materials with coherent x rays holds great potential to improve our understanding of phenomena in complex materials systems where emergent behavior can arise due to coupling of spin, lattice, and orbital degrees of freedom. Coherent diffractive imaging (CDI) is a lensless imaging technique for probing the structure of materials in three dimensions. Central to the success of the CDI method is the inversion of propagated wave field information to recover a quantitative image of the illuminated crystalline structure. Present challenges faced with existing approaches to image recovery are often due to nonuniqueness of wave propagated forms of the electron density information that can cause prohibitive stagnation of the reconstruction algorithm. Here we report on a major advancement in image recovery that is able to recover the three-dimensional image of a 492 nm gold single crystal undergoing progressive deformation to a highly strained condition without the use of a priori information. Our findings also demonstrate the significance of robust image recovery techniques for revealing high resolution topological structure. |
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Ab initio molecular dynamics study of the structural and electronic transition in VO2 Phys. Rev. B, Volume 96, 054111 (2017) The temperature-induced structural and electronic transformation in VO2 between the monoclinic M1 and tetragonal rutile phases was studied by means of ab initio molecular dynamics, based on density functional theory with Hubbard correction (DFT+U). We compare the structure of both phases, transition temperature and atomic fluctuations both above and below the transition, as well as the phonon density of states and scattering intensity of centroid position, with experimental data. The good quantitative agreement indicates that the chosen DFT+U scheme is able to provide a fairly good description of the energetics of the system. Analysis of the dynamical processes associated with the structural transformation was carried out on the atomic scale by following the time evolution of dimerization amplitudes of vanadium atom chains and the twisting angle of vanadium dimers. The electronic transition was studied by tracing the changes in projected densities of states and their correlation with the evolution of the structural transformation. Our results reveal a strong interconnection between the structural and electronic transformations and show that they take place on the same time scale. |
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Deformation of a bismuth ferrite nanocrystal imaged by coherent X-ray diffraction Journal of Physics: Conference Series, Volume 849, conference 1 (2017) Perovskite materials that contain transition metal-oxides often exhibit multifunctional properties with considerable utility in a device setting. BiFeO3 is a multiferroic perovskite material that exhibits room temperature anti-ferromagnetic and ferroelectric ordering. Optical excitation of BiFeO3 crystals results in an elastic structural deformation of the lattice with a fast response on the pico-second time scale. Here we report on dynamic optical excitation coupled with Bragg coherent X-ray diffraction measurements to investigate the structural properties of BiFeO3 nanoscale crystals. A continuous distortion of the diffraction speckle pattern was observed with increasing illumination. This was attributed to strain resulting from photo-induced lattice deformation. |
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Coherent x-ray diffraction imaging of photo-induced structural changes in BiFeO3 nanocrystals New Journal of Physics, Volume 18, 093003 (2016) Multiferroic materials that exhibit coupling between ferroelectric and magnetic properties are of considerable utility for technological applications and are also interesting from a fundamental standpoint. When reduced to the nanoscale, multiferroic materials often display additional functionality that is dominated by interfacial and confinement effects. Bismuth ferrite (BiFeO3) is one such material with room temperature anti-ferromagnetic and ferroelectric ordering. Optical excitation of BiFeO3 crystals results in an elastic structural deformation of the lattice with a fast response on the pico-second time scale. Here we report on dynamic measurements to investigate the structural properties of BiFeO3 nanoscale crystals using laser excitation and three-dimensional Bragg coherent x-ray diffraction imaging. Tensile strain beyond 8 × 10-2 was observed predominantly at the surface of the nanoscale crystal as evidenced in the reconstructed phase information and was correlated to photo-induced lattice deformation. |
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Crystalline Solids Course Notes for PHYS3004 (2016) Solids state physics is concerned with the study of matter in a condensed form as found in the world around us. It is often considered synonymous with the study of crystalline solids but extends to include liquids and amorphous materials that have partial ordering. Its primary aim is to provide an explanation of the macroscopic properties of materials through an understanding of underlying atomic structure. These course notes define the content to be delivered for the Level 3 core module on Crystalline Solids. |
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Framework for Automatic Information Extraction from Research Papers on Nanocrystal Devices Beilstein J. Nanotechnology 6, 1872–1882 (2015) To support nanocrystal device development, we have been working on a computational framework to utilize information in research papers on nanocrystal devices. We developed an annotated corpus called “ NaDev” (Nanocrystal Device Development) for this purpose. We also proposed an automatic information extraction system called “NaDevEx” (Nanocrystal Device Automatic Information Extraction Framework). NaDevEx aims at extracting information from research papers on nanocrystal devices using the NaDev corpus and machine-learning techniques. However, the characteristics of NaDevEx were not examined in detail. In this paper, we conduct system evaluation experiments for NaDevEx using the NaDev corpus. We discuss three main issues: system performance, compared with human annotators; the effect of paper type (synthesis or characterization) on system performance; and the effects of domain knowledge features (e.g., a chemical named entity recognition system and list of names of physical quantities) on system performance. We found that overall system performance was 89% in precision and 69% in recall. If we consider identification of terms that intersect with correct terms for the same information category as the correct identification, i.e., loose agreement (in many cases, we can find that appropriate head nouns such as temperature or pressure loosely match between two terms), the overall performance is 95% in precision and 74% in recall. The system performance is almost comparable with results of human annotators for information categories with rich domain knowledge information (source material). However, for other information categories, given the relatively large number of terms that exist only in one paper, recall of individual information categories is not high (39–73%); however, precision is better (75–97%). The average performance for synthesis papers is better than that for characterization papers because of the lack of training examples for characterization papers. Based on these results, we discuss future research plans for improving the performance of the system. |
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Time-Resolved Coherent Diffraction of Ultrafast Structural Dynamics in a Single Nanowire Nano Letters 14 (5) 2413–2418 (2014) The continuing effort to utilize the unique properties present in a number of strongly correlated transition metal oxides for novel device applications has led to intense study of their transitional phase state behavior. Here we report on time-resolved coherent X-ray diffraction measurements on a single vanadium dioxide nanocrystal undergoing a solid–solid phase transition, using the SACLA X-ray Free Electron Laser (XFEL) facility. We observe an ultrafast transition from monoclinic to tetragonal crystal structure in a single vanadium dioxide nanocrystal. Our findings demonstrate that the structural change occurs in a number of distinct stages attributed to differing expansion modes of vanadium atom pairs. |
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Time-resolved Bragg coherent X-ray diffraction revealing ultrafast lattice dynamics in nano-thickness crystal layer using X-ray free electron laser Journal of the Ceramic Society of Japan 121 (1411) 283-286 (2013) Ultrafast time-resolved Bragg coherent X-ray diffraction (CXD) has been performed to investigate lattice dynamics in a thin crystal layer with a nanoscale thickness by using a SASE (Self-Amplified Spontaneous Emission)-XFEL (X-ray Free Electron Laser) facility, SACLA. Single-shot Bragg coherent diffraction patterns of a 100 nm-thick silicon crystal were measured in the asymmetric configuration with a grazing exit using an area detector. The measured coherent diffraction patterns showed fringes extending in the surface normal direction. By using an optical femtosecond laser-pump and the XFEL-probe, a transient broadening of coherent diffraction pattern profile was observed at a delay time of around a few tens of picosecond, indicating transient crystal lattice fluctuation induced by the optical laser. A perspective application of the time-resolved Bragg CXD method to investigate small sized grains composing ceramic materials is discussed. |
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Bonsu: the interactive phase retrieval suite Journal of Applied Crystallography 45 840-843 (2012) Coherent X-ray diffraction imaging has received considerable attention as a nondestructive method for probing material structure at the nanoscale. However, tools for reconstructing and analysing data in both two and three dimensions have lagged somewhat behind. Bonsu, the interactive phase retrieval suite, is the first software package that allows real-time visualization of the reconstruction of phase information in both two and three dimensions. It comes complete with an inventory of algorithms and routines for data manipulation and reconstruction. Bonsu is open source, is designed around the Python language (with C++ bindings) and is largely platform independent. Bonsu is made available under version three of the GNU General Public License. |
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Compressed sensing for phase retrieval Physical Review E 85 (5) (2012) To date there are several iterative techniques that enjoy moderate success when reconstructing phase information, where only intensity measurements are made. There remains, however, a number of cases in which conventional approaches are unsuccessful. In the last decade, the theory of compressed sensing has emerged and provides a route to solving convex optimisation problems exactly via l(1)-norm minimization. Here the application of compressed sensing to phase retrieval in a nonconvex setting is reported. An algorithm is presented that applies reweighted l(1)-norm minimization to yield accurate reconstruction where conventional methods fail. |
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Coherent X-ray Diffraction Imaging for Strain Analysis on Single ZnO Nanorod AIP Conference Proceedings 1399 (2011) Strain induced in nanostructure semiconductor materials can result in different electronic properties. Coherent x-ray diffraction (CXD) has emerged as a non-destructive tool for imaging of strain and defects. In this work CXD is applied on a single ZnO nanorod, diffraction patterns from Bragg reflection are used to reconstruct the strain distribution in the samples at a resolution of 40 nm. |
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Coherent x-ray diffraction imaging of ZnO nanostructures under confined illumination New Journal of Physics 13 033006 (2011) Coherent x-ray diffraction imaging has been used to study a single ZnO nanorod in a confined illuminating condition. The focused beam size is smaller than the length of the nanorod, and the diffraction intensity is strongly dependent on the illumination position. The density maps show that the nanorod width in the radial direction is around 210 nm and has a length of 1.5 mu m, in agreement with the scanning electron microscope measurement. Reconstructed phase maps show a maximum phase change of 0.8 radians. The reconstructed direct space structures reveal the exit wavefront profile, which includes that of the focused x-ray beam. The beam profile presents in reconstructions some 'hill and valley' surface features with a typical size of a few tens of nanometres and are attributed to the noise due to the slow variation of the focused beam intensity along the boundary. A single ZnO tetrapod has been investigated with the same method to recover the beam profile in the horizontal direction. |
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Phase retrieval of diffraction from highly strained crystals Physical Review B 82 (16) (2010) An important application of phase retrieval methods is to invert coherent x-ray diffraction measurements to obtain real-space images of nanoscale crystals. The phase information is currently recovered from reciprocal-space amplitude measurements by the application of iterative projective algorithms that solve the nonlinear and nonconvex optimization problem. Various algorithms have been developed each of which apply constraints in real and reciprocal space on the reconstructed object. In general, these methods rely on experimental data that is oversampled above the Nyquist frequency. To date, support-based methods have worked well, but are less successful for highly strained structures, defined as those which contain (real-space) phase information outside the range of +/-pi/2. As a direct result the acquired experimental data is, in general, inadvertently subsampled below the Nyquist frequency. In recent years, a new theory of "compressive sensing" has emerged, which dictates that an appropriately subsampled (or compressed ) signal can be recovered exactly through iterative reconstruction and various routes to minimizing the l(1) norm or total variation in that signal. This has proven effective in solving several classes of convex optimization problems. Here we report on a "density-modification" phase reconstruction algorithm that applies the principles of compressive sensing to solve the nonconvex phase retrieval problem for highly strained crystalline materials. The application of a nonlinear operator in real-space minimizes the l(1) norm of the amplitude by a promotion-penalization (or "propenal") operation that confines the density bandwidth. This was found to significantly aid in the reconstruction of highly strained nanocrystals. We show how this method is able to successfully reconstruct phase information that otherwise could not be recovered. |
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Three-dimensional imaging of strain in a single ZnO nanorod Nature Materials 9 (2) 120-124 (2010) Nanoscale structures can be highly strained because of confinement effects and the strong influence of their external boundaries. This results in dramatically different electronic, magnetic and optical material properties of considerable utility. Third-generation synchrotron-based coherent X-ray diffraction has emerged as a non-destructive tool for three-dimensional (3D) imaging of strain and defects in crystals that are smaller than the coherence volume, typically a few cubic micrometres, of the available beams that have sufficient flux to reveal the material's structure(1). Until now, measurements have been possible only at a single Bragg point of a given crystal because of the limited ability to maintain alignment(2); it has therefore been possible to determine only one component of displacement and not the full strain tensor. Here we report key advances in our fabrication and experimental techniques, which have enabled diffraction patterns to be obtained from six Bragg reflections of the same ZnO nanocrystal for the first time. All three Cartesian components of the ion displacement field, and in turn the full nine-component strain tensor, have thereby been imaged in three dimensions. |
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Longitudinal coherence function in X-ray imaging of crystals Optics Express 17 (18) 15853-15859 (2009) The longitudinal coherence function at the Advanced Photon Source beamline 34-ID-C has been measured by a novel method and the coherence length (xi(L)) determined to be, xi(L) = 0.66 +/- 0.02 mu m. Three dimensional Coherent X-ray Diffraction (CXD) patterns were measured for multiple Bragg reflections from two Zinc Oxide (ZnO) nanorods with differing aspect ratios. The visibility of fringes corresponding to the 002 crystal direction for each reflection were found to be different and used to map the coherence function of the incident radiation. Partial coherence was found to be associated with amplitude 'hot' spots in three dimensional reconstructions of the crystal structure. |
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ZnO tetrapod p-n junction diodes Applied Physics Letters 94 15 (2009) ZnO nanocrystals hold the potential for use in a wide range of applications particularly in optoelectronics. We report on the fabrication of a highly sensitive p-n junction diode structure based on a single ZnO tetrapod shaped nanocrystal. This device shows a noted response to ultraviolet light with high internal gain. The high reponsivities we have observed exceed 10(4) A/W and are likely due to impact-ionization effects at the p-n junction interface. |
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Photoresponse of ZnO tetrapod nanocrystal Schottky diodes IEEE Transactions on Nanotechnology 7 (1) 20-23 (2008) The fabrication of an ultraviolet photodiode employing a single ZnO tetrapod nanocrystal is reported. We have attached two tungsten leads and one platinum lead to three of the arms of the tetrapod. By measuring the transport properties between each pair of leads we show that the tungsten contacts are ohmic and the platinum contacts are rectifying. Photoresponse measurements were carried out with above and below band gap illumination. We observe a much larger ultraviolet photoresponse for the rectifying Pt-ZnO-W junction than the linear W-ZnO-W junction. We conclude that the enhanced photoresponse of our rectifying junction results from a photoinduced reduction of the Schottky barrier height at the Pt-ZnO interface. |
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Zinc Oxide Nanostructures and High Electron Mobility Nanocomposite Thin Film Transistors IEEE Transactions on Electron Devices 55 (11) 3001-3011 (2008) This paper reports on the synthesis of zinc oxide (ZnO) nanostructures and examines the performance of nanocomposite thin-film transistors (TFTs) fabricated using ZnO dispersed in both n- and p-type polymer host matrices. The ZnO nanostructures considered here comprise nanowires and tetrapods and were synthesized using vapor phase deposition techniques involving the carbothermal reduction of solid-phase zinc-containing compounds. Measurement results of nanocomposite TFTs based on dispersion of ZnO nanorods in an n-type organic semiconductor ([6, 6]-phenyl-C-61-butyric acid methyl ester) show electron field-effect mobilities in the range 0.3-0.6 cm(2)V(-1)s(-1), representing an approximate enhancement by as much as a factor of 40 from the pristine state. The on/off current ratio of the nanocomposite TFTs approach 10(6) at saturation with off-currents on the order of 10 pA. The results presented here, although preliminary, show a highly promising enhancement for realization of high-performance solution-processable n-type organic TFTs. |
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ZnO tetrapod nanocrystals Materials Today 10 (5) 50-54 (2007) ZnO has received considerable attention because of its unique optical, piezoelectric, and magnetic properties. It also readily self-assembles into a family of nanocrystalline structures. We review the current status of research into ZnO tetrapod nanocrystals. These crystals consist of a ZnO core in the zinc blende structure from which four ZnO arms in the wurtzite structure radiate. The arms are cylinders of hexagonal cross section, with each arm of equal length and diameter. Possible applications in optoelectronics, photovoltaics, spintronics, and piezoelectricity are discussed. |
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ZnO tetrapod Schottky photodiodes Applied Physics Letters 89 (7) (2006) The fabrication of an ultraviolet photodiode employing a single ZnO tetrapod nanocrystal is reported. This diode structure is prepared by depositing W and Pt electrodes to form Ohmic and Schottky contacts, respectively. Dark current-voltage measurements show rectifying behavior. The properties of the metal-semiconductor interface are studied with above and below band gap illumination. It is found that with increasing UV excitation the device converts from a rectifying to an Ohmic behavior. This effect is attributed to a flattening of the energy bands due to the migration of photogenerated carriers within the space charge region at the metal-semiconductor interface. |
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Synthesis and characterisation of zinc oxide tetrapod nanocrystals Journal of Physics Conference Series 26 251-255 (2006) Zinc oxide is an important group II-VI semiconductor material with optical properties that permit stable- emission at room temperature. We report on the synthesis of highly uniform nanocrystalline ZnO tetrapod (ZnO-T) nanostructures through a modified chemical vapour transport process. These self assembled nanocrystals are characterised by four cylindrical arms with a hexagonal facet all of which are joined at a tetrahedral core. Studies are carried out on ZnO tetrapods using scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), photoluminescence spectroscopy (PLS) and Raman measurements. We find a simple technique to quench visible emission found in ZnO tetrapods as grown. We also observe Raman active modes suggesting that nitrogen is incorporated within our samples. |