Biomedical subjects

J C H Spence

Publications and source records attributed to J C H Spence.

10 recordsLinked to original sources

PubMed2003

Structure and bonding in alpha-copper phthalocyanine by electron diffraction.

Energy-filtered quantitative electron diffraction at liquid nitrogen temperature has been used to examine the atomic structure and bonding of metastable alpha-Cu phthalocyanine crystals. Three theoretical methods (kinematic, kinematic with excitation errors and Bloch wave) were employed for the intensity calculations. The Bloch-wave method was found to account for dynamical effects by greatly reducing the residual factor between experimental and simulated results. A new method for calculating electron scattering factors for partially charged ions is proposed and the sensitivity of electron diffraction to charge transfer is discussed. The atomic charge states were analyzed for alpha-Cu phthalocyanine using a charge cloud model in which the Gaussian bond charge is positioned along the bonds. Spot patterns were collected in the Kohler mode at two beam energies to reduce error. Using the best-fitting model, a deformation charge-density map is produced and compared to the neutral-atom model. From this, the main features of atomic charge transfer in the alpha-Cu phthalocyanine structure can be seen in the (010) plane.

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PubMed2003

Charge density and chemical bonding in rutile, TiO2.

The low-order structure factors of rutile (TiO(2)) have been measured with an accuracy of up to 0.09% by quantitative convergent-beam electron diffraction (QCBED). This error is an order of magnitude smaller than that in conventional Bragg X-ray diffraction and equivalent to the accuracy of the X-ray Pendellösung method. It is sufficient to distinguish atomic, covalent and ionic bonding. By refinement of the combined data of low-order reflections measured by electron diffraction with high-order reflections from X-ray diffraction, accurate charge-density maps are obtained and used to understand the role of the 3d electrons in Ti-O bonding. The results are combined with electron energy-loss spectra (EELS) in a study of the electronic structure.

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PubMed2003

Solving non-periodic structures using direct methods: phasing diffuse scattering.

The problem of reconstructing the charge density of a non-periodic sample from its diffuse X-ray scattering is considered. For a sample known to be isolated, an artificial superlattice may be assumed and the numerical direct methods of crystallography applied to the continuous distribution of diffuse scattering in order to solve the phase problem. This method is applied to simulated soft-X-ray transmission speckle patterns from a two-dimensional array of gold balls of 50 nm diameter. The results are relevant to efforts to phase the scattering from many individual macromolecules that cannot be crystallized, and to the scattering from individual inorganic nanoparticles.

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PubMed2003

Experimental lensless soft-X-ray imaging using iterative algorithms: phasing diffuse scattering.

Images of randomly placed two-dimensional arrays of gold balls have been reconstructed from their soft-X-ray transmission diffraction patterns. An iterative hybrid input-output (HiO) algorithm was used to solve the phase problem for the continuous distribution of diffuse X-ray scattering. Knowledge of the approximate size of the clusters was required. The images compare well with scanning electron microscope (SEM) images of the same sample. The use of micrometre-sized silicon nitride window supports is suggested, and absorption filters have been used to allow collection of low spatial frequencies often obscured by a beam stop. This method of phasing diffuse scattering may have application to scattering from individual inorganic nanostructures or single macromolecules.

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PubMed2002

Kinematic and dynamical CBED for solving thin organic films at low temperature; experimental tests with anthracene.

Low-dose, low-temperature kinematic and dynamical convergent-beam electron diffraction (CBED) patterns from thin organic crystalline films have been used for the measurement of structure-factor amplitudes and phases. Kinematic conditions are identified by the observation of uniform intensity within the CBED discs and used to determine structure-factor magnitudes. CBED patterns from thicker regions affected by multiple scattering give structure-factor signs, which are varied for best fit. The use of a small probe (and the Kohler SAD mode) minimizes bending artifacts. A new method of thickness determination is evaluated. The approach is tested using experimental data from the centrosymmetric anthracene structure, the results compared with direct methods, and a potential map derived from experimental data. The faint peaks due to H-atom positions may be distinguished. Key issues influencing the validity of the method such as the appropriate dimension of the structure-factor matrix, sample thickness and crystal orientation are discussed.

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PubMed2002

Phase recovery and lensless imaging by iterative methods in optical, X-ray and electron diffraction.

Thomas Young's quantitative analysis of interference effects provided the confidence needed to revive the wave theory of light, and firmly established the concept of phase in optics. Phase plays a similarly fundamental role in matter-wave interferometry, for which the field-emission electron microscope provides ideal instrumentation. The wave-particle duality is vividly demonstrated by experimental 'Young's fringes' using coherent electron beams under conditions in which the flight time is less than the time between particle emission. A brief historical review is given of electron interferometry and holography, including the Aharonov-Bohm effect and the electron Sagnac interferometer. The simultaneous development of phase-contrast imaging at subnanometre spatial resolution has greatly deepened our understanding of atomic processes in biology, materials science and condensed-matter physics, while electron holography has become a routine tool for the mapping of electrostatic and magnetic fields in materials on a nanometre scale. The encoding of phase information in scattered farfield intensities is discussed, and non-interferometric, non-crystallographic methods for phase retrieval are reviewed in relationship to electron holography. Examples of phase measurement and diffraction-limited imaging using the hybrid input-output iterative algorithm are given, including simulations for soft X-ray imaging, and new experimental results for coherent electron and visible-light scattering. Image reconstruction is demonstrated from experimental electron and visible-light Fraunhofer diffraction patterns. The prospects this provides for lensless imaging using particles for which no lenses exist (such as neutrons, condensates, coherent atom beams and X-rays) are discussed. These new interactions can be expected to provide new information, perhaps, for example, in biology, with the advantage of less damage to samples.

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PubMed2002

Electron holography of field-emitting carbon nanotubes.

Electron holography performed in situ inside a high resolution transmission electron microscope has been used to determine the magnitude and spatial distribution of the electric field surrounding individual field-emitting carbon nanotubes. The electric field (and hence the associated field emission current) is concentrated precisely at the tips of the nanotubes and not at other nanotube defects such as sidewall imperfections. The electric field magnitude and distribution are stable in time, even in cases where the nanotube field emission current exhibits extensive temporal fluctuations.

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PubMed2002

Synchrotron soft X-ray and field-emission electron sources: a comparison.

The soft X-ray spectral region and the useful range of electron energy-loss spectroscopy are very similar, both including the energy range 100-1000 eV. Moreover, well-developed monochromators and parallel detection devices with comparable resolution exist for both. Despite the differing interactions of electrons and photons, many complementary experiments in imaging, spectroscopy and diffraction have been performed using both techniques. We therefore compare the brightness, degeneracy, monochromaticity, beam size, source size, spatial and temporal coherence of field-emission electron beams and soft X-ray synchrotron radiation from typical undulators. Recent brightness values for nanotip field emitters and undulators, both measured and calculated, are provided with examples from the Advanced Light Source synchrotron-radiation facility at Berkeley USA. The quantum mechanical upper limit on source brightness, as well as relationships among beam brightness, coherence parameters, and degeneracy, are discussed. Factors which limit these parameters and methods of measurement are reviewed, and the implications for diffraction, imaging and spectroscopic experiments as well as radiation damage are briefly commented on.

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PubMed2002

Ordering energies and occupancies in doped TiAl, and dedicated ALCHEMI instrumentation.

Alloy design has been a lifelong interest of Gareth Thomas, and modern design algorithms include atomistic parameters which are obtainable from new electron microscope techniques such as ALCHEMI. In this paper, we discuss the relevance of ALCHEMI site occupancy measurements to intermetallic alloys, and summarize prior work. The results are found to lie in regions of a site-occupancy diagram (SOC) relating ordering energies to occupancy, as predicted by the Bragg-Williams theory of short-range order. These predictions also explain previous inconsistencies in the ALCHEMI measurements. A diffraction camera and X-ray detector system of novel design is proposed for dedicated ALCHEMI analysis for substitutional and interstitial dopant site-occupancy measurement, and details of the design given. Using this novel hardware design, the data-collection times for two-dimensional ALCHEMI patterns should be reduced by an order of magnitude or more, and the full data collection process automated. The resulting occupancy information can provide essential input parameters for atomistic alloy design algorithms, and can provide entirely new information on interstitial occupancies in minerals, ceramics, semiconductors, and alloys.

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PubMed2001

Orbital ordering in LaMnO3: estimates of structure factors and comparison of measurement methods.

This paper shows that the phenomenon of orbital ordering should be detectable by energy-filtered quantitative convergent-beam electron diffraction (QCBED). The structure factors of LaMnO(3) crystals are calculated using a non-spherical atomic scattering model of the Mn(3+) ion. Several low-order electron structure factors showed pronounced change with orbital ordering, in which the e(g)(1) electron orders in the 3d(3z(2) - r(2)) orbital leaving the 3d(x(2) - y(2)) unoccupied. In contrast, the X-ray structure factors showed very small change. Orbital order is important in transition-metal oxides, including colossal magnetoresistive manganite oxides. The calculations show that by using QCBED it is possible to measure the subtle changes in electron structure factors due to orbital ordering of the e(g)(1) electron of the Mn(3+) ion in an LaMnO(3) crystal. A comparison of methods for structure-factor measurement is given, including Bragg X-ray and gamma-ray diffraction, X-ray Pendellösung and critical-voltage methods. New measurements by QCBED of structure factors in rutile are compared with the Bragg X-ray values. These show that QCEBD can provide an accurate extinction-free measurement of low-order structure factors, which is extremely difficult or perhaps impossible when using other methods applied to real crystals.

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