96 results on '"C Kisielowski"'
Search Results
52. Maintaining the genuine structure of 2D materials and catalytic nanoparticles at atomic resolution.
- Author
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Calderon HA, Kisielowski C, Specht P, Barton B, Godinez-Salomon F, and Solorza-Feria O
- Abstract
The recent development of atomic resolution, low dose-rate electron microscopy allows investigating 2D materials as well as catalytic nano particles without compromising their structural integrity. For graphene and a variety of nanoparticle compositions, it is shown that a critical dose rate exists of <100 e(-)/Å(2) s at 80 keV of electron acceleration that allows maintaining the genuine object structures including their surfaces and edges even if particles are only 3 nm large or smaller. Moreover, it is demonstrated that electron beam-induced phonon excitation from outside the field of view contributes to a contrast degradation in recorded images. These degradation effects can be eliminated by delivering electrons onto the imaged area, only, by using a Nilsonian illumination scheme in combination with a suitable aperture at the electron gun/monochromator assembly., (Copyright © 2014 Elsevier Ltd. All rights reserved.)
- Published
- 2015
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53. 3D reconstruction of nanocrystalline particles from a single projection.
- Author
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Chen FR, Kisielowski C, and Van Dyck D
- Abstract
This paper describes an approach to retrieve the three-dimensional atomic structure of a nanocrystalline particle from the reconstructed electron exit wave function in a single projection direction. The method employs wave propagation to determine the local exit surface of each atomic column together with its mass. The exit wave in between colums is used as internal calibration so as to remove the background noise and improve the precision to the level of single atom sensitivity. The validity of the approach is tested with exit wave functions of a gold wedge reconstructed from simulated images containing different levels of noise., (Copyright © 2014 Elsevier Ltd. All rights reserved.)
- Published
- 2015
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54. Controlling electron beam-induced structure modifications and cation exchange in cadmium sulfide-copper sulfide heterostructured nanorods.
- Author
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Zheng H, Sadtler B, Habenicht C, Freitag B, Alivisatos AP, and Kisielowski C
- Subjects
- Electrons, Cadmium Compounds chemistry, Copper Sulfate chemistry, Electron Microscope Tomography methods, Nanotubes chemistry, Sulfides chemistry
- Abstract
The atomic structure and interfaces of CdS/Cu2S heterostructured nanorods are investigated with the aberration-corrected TEAM 0.5 electron microscope operated at 80 kV and 300 kV applying in-line holography and complementary techniques. Cu2S exhibits a low-chalcocite structure in pristine CdS/Cu2S nanorods. Under electron beam irradiation the Cu2S phase transforms into a high-chalcocite phase while the CdS phase maintains its wurtzite structure. Time-resolved experiments reveal that Cu(+)-Cd(2+) cation exchange at the CdS/Cu2S interfaces is stimulated by the electron beam and proceeds within an undisturbed and coherent sulfur sub-lattice. A variation of the electron beam current provides an efficient way to control and exploit such irreversible solid-state chemical processes that provide unique information about system dynamics at the atomic scale. Specifically, we show that the electron beam-induced copper-cadmium exchange is site specific and anisotropic. A resulting displacement of the CdS/Cu2S interfaces caused by beam-induced cation interdiffusion equals within a factor of 3-10 previously reported Cu diffusion length measurements in heterostructured CdS/Cu2S thin film solar cells with an activation energy of 0.96 eV., (© 2013 Elsevier B.V. All rights reserved.)
- Published
- 2013
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55. Recording low and high spatial frequencies in exit wave reconstructions.
- Author
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Haigh SJ, Jiang B, Alloyeau D, Kisielowski C, and Kirkland AI
- Subjects
- Image Processing, Computer-Assisted methods, Microscopy, Electron, Transmission methods
- Abstract
Aberration corrected Transmission Electron Microscope (TEM) images can currently resolve information at significantly better than 0.1 nm. Aberration corrected imaging conditions seek to optimize the transfer of high-resolution information but in doing so they prevent the transfer of low spatial frequency information. To recover low spatial frequency information, aberration corrected images must be acquired at a large defocus which compromises high spatial frequency information transfer. In this paper we present two a posteriori solutions to this problem in which the information bandwidth in an exit wave reconstruction is increased. In the first we reconstruct the electron exit wavefunction from two focal series datasets, with different, uniform focal steps, experimentally demonstrating that the width of the transfer interval can be extended from 0.2 nm⁻¹ (∼5 nm) to better than 10 nm⁻¹ (0.1 nm). In the second we outline the use of a focal series recorded with a non-uniform focal step to recover a wider range of spatial frequencies without the need for a large number of images. Using simulated data we show that using this non-uniform focal step the spatial frequency interval for a five image data set may be increased to between 0.25 nm⁻¹ (4 nm) and 8.3 nm⁻¹ (0.12 nm) compared to between 0.74 nm⁻¹ (1.4 nm) and 8.3 nm⁻¹ (0.12 nm) for the standard focal series geometry., (Copyright © 2013 The Authors. Published by Elsevier B.V. All rights reserved.)
- Published
- 2013
- Full Text
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56. Atomically perfect torn graphene edges and their reversible reconstruction.
- Author
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Kim K, Coh S, Kisielowski C, Crommie MF, Louie SG, Cohen ML, and Zettl A
- Abstract
The atomic structure of graphene edges is critical in determining the electrical, magnetic and chemical properties of truncated graphene structures, notably nanoribbons. Unfortunately, graphene edges are typically far from ideal and suffer from atomic-scale defects, structural distortion and unintended chemical functionalization, leading to unpredictable properties. Here we report that graphene edges fabricated by electron beam-initiated mechanical rupture or tearing in high vacuum are clean and largely atomically perfect, oriented in either the armchair or zigzag direction. We demonstrate, via aberration-corrected transmission electron microscopy, reversible and extended pentagon-heptagon (5-7) reconstruction at zigzag edges, and explore experimentally and theoretically the dynamics of the transitions between configuration states. Good theoretical-experimental agreement is found for the flipping rates between 5-7 and 6-6 zigzag edge states. Our study demonstrates that simple ripping is remarkably effective in producing atomically clean, ideal terminations, thus providing a valuable tool for realizing atomically tailored graphene and facilitating meaningful experimental study.
- Published
- 2013
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57. Subangstrom edge relaxations probed by electron microscopy in hexagonal boron nitride.
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Alem N, Ramasse QM, Seabourne CR, Yazyev OV, Erickson K, Sarahan MC, Kisielowski C, Scott AJ, Louie SG, and Zettl A
- Abstract
Theoretical research on the two-dimensional crystal structure of hexagonal boron nitride (h-BN) has suggested that the physical properties of h-BN can be tailored for a wealth of applications by controlling the atomic structure of the membrane edges. Unexplored for h-BN, however, is the possibility that small additional edge-atom distortions could have electronic structure implications critically important to nanoengineering efforts. Here we demonstrate, using a combination of analytical scanning transmission electron microscopy and density functional theory, that covalent interlayer bonds form spontaneously at the edges of a h-BN bilayer, resulting in subangstrom distortions of the edge atomic structure. Orbital maps calculated in 3D around the closed edge reveal that the out-of-plane bonds retain a strong π(*) character. We show that this closed edge reconstruction, strikingly different from the equivalent case for graphene, helps the material recover its bulklike insulating behavior and thus largely negates the predicted metallic character of open edges.
- Published
- 2012
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58. Atomic resolution phase contrast imaging and in-line holography using variable voltage and dose rate.
- Author
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Barton B, Jiang B, Song C, Specht P, Calderon H, and Kisielowski C
- Abstract
The TEAM 0.5 electron microscope is employed to demonstrate atomic resolution phase contrast imaging and focal series reconstruction with acceleration voltages between 20 and 300 kV and a variable dose rate. A monochromator with an energy spread of ≤0.1 eV is used for dose variation by a factor of 1,000 and to provide a beam-limiting aperture. The sub-Ångstrøm performance of the instrument remains uncompromised. Using samples obtained from silicon wafers by chemical etching, the [200] atom dumbbell distance of 1.36 Å can be resolved in single images and reconstructed exit wave functions at 300, 80, and 50 kV. At 20 kV, atomic resolution <2 Å is readily available but limited by residual lens aberrations at large scattering angles. Exit wave functions reconstructed from images recorded under low dose rate conditions show sharper atom peaks as compared to high dose rate. The observed dose rate dependence of the signal is explained by a reduction of beam-induced atom displacements. If a combined sample and instrument instability is considered, the experimental image contrast can be matched quantitatively to simulations. The described development allows for atomic resolution transmission electron microscopy of interfaces between soft and hard materials over a wide range of voltages and electron doses.
- Published
- 2012
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59. Using a monochromator to improve the resolution in TEM to below 0.5 Å. Part II: application to focal series reconstruction.
- Author
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Tiemeijer PC, Bischoff M, Freitag B, and Kisielowski C
- Subjects
- Algorithms, Chromosome Aberrations, Equipment Design instrumentation, Equipment Design methods, Fourier Analysis, Lighting, Microscopy, Electron methods, Reproducibility of Results, Electrons, Image Processing, Computer-Assisted methods
- Abstract
We apply monochromated illumination to improve the information transfer in focal series reconstruction to 0.5 Å at 300 kV. Contrary to single images, which can be taken arbitrarily close to Gaussian focus in a C(S)-corrected microscope, images in a focal series are taken at a certain defocus. This defocus poses limits on the spatial coherence of the illumination, and through this, limits on the brightness of the monochromated illumination. We derive an estimate for the minimum spatial coherence and the minimal brightness needed for a certain resolution at a certain defocus and apply this estimate to our focal series experiments. We find that the 0.5 Å information transfer would have been difficult and probably impossible to obtain without the exceptionally high brightness of the monochromated illumination., (Copyright © 2012 Elsevier B.V. All rights reserved.)
- Published
- 2012
- Full Text
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60. Using a monochromator to improve the resolution in TEM to below 0.5Å. Part I: Creating highly coherent monochromated illumination.
- Author
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Tiemeijer PC, Bischoff M, Freitag B, and Kisielowski C
- Abstract
Chromatic aberration limits the resolution in spherical-aberration corrected Transmission Electron Microscopy to approximately 0.7Å at 300 kV. The energy spread in the beam is the main contribution to the chromatic aberration. This spread can be reduced with a monochromator. Another limitation to the resolution in TEM can be the finite brightness of the source and the consequent partial spatial coherence of the illumination. This limitation becomes important when spherical aberration and/or defocus are present such as in uncorrected TEM or in focal-series reconstruction in TEM. We used a monochromator optimized for minimum brightness loss and a prototype 'high-brightness' gun, and obtained brightness after monochromation comparable to that of the standard Schottky FEG before monochromation. The images were acquired on the prototype TEAM 0.5 microscope, which was developed on a Titan platform by increasing its electrical and mechanical stability., (Copyright © 2012 Elsevier B.V. All rights reserved.)
- Published
- 2012
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61. Surfactant-free preparation of supported cubic platinum nanoparticles.
- Author
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Peng Z, Kisielowski C, and Bell AT
- Subjects
- Spectroscopy, Fourier Transform Infrared, Surface-Active Agents, Metal Nanoparticles chemistry, Nanotechnology methods, Platinum chemistry
- Abstract
A novel method has been developed for preparing supported cubic platinum nanoparticles. Carbon monoxide and hydrogen are used to reduce platinum precursors present at a solid-gas interface and to control the shape of the growing Pt nanoparticles. By avoiding the use of any organic agents in the synthesis, cubic Pt particles free of hydrocarbons are formed, thereby avoiding possible contamination of the catalyst surface. The approach used is simple and readily scalable., (This journal is © The Royal Society of Chemistry 2012)
- Published
- 2012
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62. Understanding the metal-carbon interface in FePt catalyzed carbon nanotubes.
- Author
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Pohl D, Schäffel F, Rümmeli MH, Mohn E, Täschner C, Schultz L, Kisielowski C, and Rellinghaus B
- Abstract
Any tip functionalization of carbon nanotubes, for which the relative orientation between their (metallic) catalyst particle and the nanotube axis is essential, requires a detailed knowledge of the nature of the internal interface between the particle and the outgrown tube. In the present work, this interface is characterized with atomic precision using state-of-the-art low-voltage aberration-corrected transmission electron microscopy in combination with molecular dynamics simulations for the case of hard-magnetically terminated carbon nanotubes. Our results indicate that the physical principle based upon which the interfacial metal facet is chosen is a reduction of the desorption energy for carbon.
- Published
- 2011
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63. Atomic-scale edge structures on industrial-style MoS2 nanocatalysts.
- Author
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Hansen LP, Ramasse QM, Kisielowski C, Brorson M, Johnson E, Topsøe H, and Helveg S
- Subjects
- Catalysis, Crystallization, Particle Size, Surface Properties, Disulfides chemistry, Molybdenum chemistry, Nanostructures chemistry, Nanotechnology methods
- Published
- 2011
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64. Direct imaging and chemical analysis of unstained DNA origami performed with a transmission electron microscope.
- Author
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Alloyeau D, Ding B, Ramasse Q, Kisielowski C, Lee Z, and Jeon KJ
- Subjects
- Microscopy, Atomic Force, Microscopy, Electron, Transmission, Nanotechnology, DNA chemistry
- Abstract
Here, we report a simple and rapid characterisation technique combining physical and chemical analysis for DNA origami with conventional TEM., (This journal is © The Royal Society of Chemistry 2011)
- Published
- 2011
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65. Observation of transient structural-transformation dynamics in a Cu2S nanorod.
- Author
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Zheng H, Rivest JB, Miller TA, Sadtler B, Lindenberg A, Toney MF, Wang LW, Kisielowski C, and Alivisatos AP
- Abstract
The study of first-order structural transformations has been of great interest to scientists in many disciplines. Expectations from phase-transition theory are that the system fluctuates between two equilibrium structures near the transition point and that the region of transition broadens in small crystals. We report the direct observation of structural fluctuations within a single nanocrystal using transmission electron microscopy. We observed trajectories of structural transformations in individual nanocrystals with atomic resolution, which reveal details of the fluctuation dynamics, including nucleation, phase propagation, and pinning of structural domains by defects. Such observations provide crucial insight for the understanding of microscopic pathways of phase transitions.
- Published
- 2011
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66. Conversion of self-assembled monolayers into nanocrystalline graphene: structure and electric transport.
- Author
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Turchanin A, Weber D, Büenfeld M, Kisielowski C, Fistul MV, Efetov KB, Weimann T, Stosch R, Mayer J, and Gölzhäuser A
- Subjects
- Electron Transport, Macromolecular Substances chemistry, Materials Testing, Molecular Conformation, Particle Size, Surface Properties, Graphite chemistry, Nanostructures chemistry, Nanostructures ultrastructure
- Abstract
Graphene-based materials have been suggested for applications ranging from nanoelectronics to nanobiotechnology. However, the realization of graphene-based technologies will require large quantities of free-standing two-dimensional (2D) carbon materials with tunable physical and chemical properties. Bottom-up approaches via molecular self-assembly have great potential to fulfill this demand. Here, we report on the fabrication and characterization of graphene made by electron-radiation induced cross-linking of aromatic self-assembled monolayers (SAMs) and their subsequent annealing. In this process, the SAM is converted into a nanocrystalline graphene sheet with well-defined thickness and arbitrary dimensions. Electric transport data demonstrate that this transformation is accompanied by an insulator to metal transition that can be utilized to control electrical properties such as conductivity, electron mobility, and ambipolar electric field effect of the fabricated graphene sheets. The suggested route opens broad prospects toward the engineering of free-standing 2D carbon materials with tunable properties on various solid substrates and on holey substrates as suspended membranes.
- Published
- 2011
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67. Air-stable magnesium nanocomposites provide rapid and high-capacity hydrogen storage without using heavy-metal catalysts.
- Author
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Jeon KJ, Moon HR, Ruminski AM, Jiang B, Kisielowski C, Bardhan R, and Urban JJ
- Abstract
Hydrogen is a promising alternative energy carrier that can potentially facilitate the transition from fossil fuels to sources of clean energy because of its prominent advantages such as high energy density (142 MJ kg(-1); ref. 1), great variety of potential sources (for example water, biomass, organic matter), light weight, and low environmental impact (water is the sole combustion product). However, there remains a challenge to produce a material capable of simultaneously optimizing two conflicting criteria--absorbing hydrogen strongly enough to form a stable thermodynamic state, but weakly enough to release it on-demand with a small temperature rise. Many materials under development, including metal-organic frameworks, nanoporous polymers, and other carbon-based materials, physisorb only a small amount of hydrogen (typically 1-2 wt%) at room temperature. Metal hydrides were traditionally thought to be unsuitable materials because of their high bond formation enthalpies (for example MgH(2) has a ΔHf~75 kJ mol(-1)), thus requiring unacceptably high release temperatures resulting in low energy efficiency. However, recent theoretical calculations and metal-catalysed thin-film studies have shown that microstructuring of these materials can enhance the kinetics by decreasing diffusion path lengths for hydrogen and decreasing the required thickness of the poorly permeable hydride layer that forms during absorption. Here, we report the synthesis of an air-stable composite material that consists of metallic Mg nanocrystals (NCs) in a gas-barrier polymer matrix that enables both the storage of a high density of hydrogen (up to 6 wt% of Mg, 4 wt% for the composite) and rapid kinetics (loading in <30 min at 200 °C). Moreover, nanostructuring of the Mg provides rapid storage kinetics without using expensive heavy-metal catalysts.
- Published
- 2011
- Full Text
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68. Probing the out-of-plane distortion of single point defects in atomically thin hexagonal boron nitride at the picometer scale.
- Author
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Alem N, Yazyev OV, Kisielowski C, Denes P, Dahmen U, Hartel P, Haider M, Bischoff M, Jiang B, Louie SG, and Zettl A
- Abstract
Crystalline systems often lower their energy by atom displacements from regular high-symmetry lattice sites. We demonstrate that such symmetry lowering distortions can be visualized by ultrahigh resolution transmission electron microscopy even at single point defects. Experimental investigation of structural distortions at the monovacancy defects in suspended bilayers of hexagonal boron nitride (h-BN) accompanied by first-principles calculations reveals a characteristic charge-induced pm symmetry configuration of boron vacancies. This symmetry breaking is caused by interlayer bond reconstruction across the bilayer h-BN at the negatively charged boron vacancy defects and results in local membrane bending at the defect site. This study confirms that boron vacancies are dominantly present in the h-BN membrane.
- Published
- 2011
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69. Grain boundary mapping in polycrystalline graphene.
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Kim K, Lee Z, Regan W, Kisielowski C, Crommie MF, and Zettl A
- Subjects
- Macromolecular Substances chemistry, Molecular Conformation, Nanotechnology methods, Particle Size, Surface Properties, Crystallization methods, Graphite chemistry, Materials Testing methods, Nanostructures chemistry, Nanostructures ultrastructure
- Abstract
We report direct mapping of the grains and grain boundaries (GBs) of large-area monolayer polycrystalline graphene sheets, at large (several micrometer) and single-atom length scales. Global grain and GB mapping is performed using electron diffraction in scanning transmission electron microscopy (STEM) or using dark-field imaging in conventional TEM. Additionally, we employ aberration-corrected TEM to extract direct images of the local atomic arrangements of graphene GBs, which reveal the alternating pentagon-heptagon structure along high-angle GBs. Our findings provide a readily adaptable tool for graphene GB studies.
- Published
- 2011
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70. Free-floating ultrathin two-dimensional crystals from sequence-specific peptoid polymers.
- Author
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Nam KT, Shelby SA, Choi PH, Marciel AB, Chen R, Tan L, Chu TK, Mesch RA, Lee BC, Connolly MD, Kisielowski C, and Zuckermann RN
- Subjects
- Amino Acid Sequence, Buffers, Crystallization, Fourier Analysis, Ligands, Models, Chemical, Nanostructures chemistry, Nanostructures ultrastructure, Polymers chemical synthesis, Protein Binding, Sequence Homology, Amino Acid, Static Electricity, Water chemistry, Biomimetics, Glycine analogs & derivatives, Peptoids chemistry, Polymers chemistry, Protein Structure, Secondary
- Abstract
The design and synthesis of protein-like polymers is a fundamental challenge in materials science. A biomimetic approach is to explore the impact of monomer sequence on non-natural polymer structure and function. We present the aqueous self-assembly of two peptoid polymers into extremely thin two-dimensional (2D) crystalline sheets directed by periodic amphiphilicity, electrostatic recognition and aromatic interactions. Peptoids are sequence-specific, oligo-N-substituted glycine polymers designed to mimic the structure and functionality of proteins. Mixing a 1:1 ratio of two oppositely charged peptoid 36mers of a specific sequence in aqueous solution results in the formation of giant, free-floating sheets with only 2.7 nm thickness. Direct visualization of aligned individual peptoid chains in the sheet structure was achieved using aberration-corrected transmission electron microscopy. Specific binding of a protein to ligand-functionalized sheets was also demonstrated. The synthetic flexibility and biocompatibility of peptoids provide a flexible and robust platform for integrating functionality into defined 2D nanostructures.
- Published
- 2010
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71. Imaging MoS2 nanocatalysts with single-atom sensitivity.
- Author
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Kisielowski C, Ramasse QM, Hansen LP, Brorson M, Carlsson A, Molenbroek AM, Topsøe H, and Helveg S
- Published
- 2010
- Full Text
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72. Structural stability of icosahedral FePt nanoparticles.
- Author
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Wang R, Zhang H, Farle M, and Kisielowski C
- Abstract
The structural stability of FePt nanoparticles of about 5-6 nm diameter was investigated by dynamic high resolution transmission electron microscopy. The FePt icosahedra were very stable under an electron beam flux of approximately 20 A/cm(2) at 300 kV. Surface sputtering was suppressed due to the large sputtering threshold energy of a Pt-rich shell. Under a flux of approximately 50 A/cm(2), the trapping potential well of the FePt particle on the supporting carbon film was lowered by the magnetic interaction between the electron beam and the particle, which leads to rotational and translational motions of the particle. A large dose of electrons (approximately 200 A/cm(2)) initiated melting and recrystallization of the FePt particle. The structure of the FePt nanoparticle, a Pt enriched shell around an Fe/Pt magnetic core, is believed to be responsible for its dynamic behaviour under different beam conditions.
- Published
- 2009
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73. Observation of single colloidal platinum nanocrystal growth trajectories.
- Author
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Zheng H, Smith RK, Jun YW, Kisielowski C, Dahmen U, and Alivisatos AP
- Abstract
Understanding of colloidal nanocrystal growth mechanisms is essential for the syntheses of nanocrystals with desired physical properties. The classical model for the growth of monodisperse nanocrystals assumes a discrete nucleation stage followed by growth via monomer attachment, but has overlooked particle-particle interactions. Recent studies have suggested that interactions between particles play an important role. Using in situ transmission electron microscopy, we show that platinum nanocrystals can grow either by monomer attachment from solution or by particle coalescence. Through the combination of these two processes, an initially broad size distribution can spontaneously narrow into a nearly monodisperse distribution. We suggest that colloidal nanocrystals take different pathways of growth based on their size- and morphology-dependent internal energies.
- Published
- 2009
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74. Graphene at the edge: stability and dynamics.
- Author
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Girit CO, Meyer JC, Erni R, Rossell MD, Kisielowski C, Yang L, Park CH, Crommie MF, Cohen ML, Louie SG, and Zettl A
- Abstract
Although the physics of materials at surfaces and edges has been extensively studied, the movement of individual atoms at an isolated edge has not been directly observed in real time. With a transmission electron aberration-corrected microscope capable of simultaneous atomic spatial resolution and 1-second temporal resolution, we produced movies of the dynamics of carbon atoms at the edge of a hole in a suspended, single atomic layer of graphene. The rearrangement of bonds and beam-induced ejection of carbon atoms are recorded as the hole grows. We investigated the mechanism of edge reconstruction and demonstrated the stability of the "zigzag" edge configuration. This study of an ideal low-dimensional interface, a hole in graphene, exhibits the complex behavior of atoms at a boundary.
- Published
- 2009
- Full Text
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75. Atomic-resolution imaging with a sub-50-pm electron probe.
- Author
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Erni R, Rossell MD, Kisielowski C, and Dahmen U
- Abstract
Using a highly coherent focused electron probe in a fifth-order aberration-corrected transmission electron microscope, we report on resolving a crystal spacing less than 50 pm. Based on the geometrical source size and residual coherent and incoherent axial lens aberrations, an electron probe is calculated, which is theoretically capable of resolving an ideal 47 pm spacing with 29% contrast. Our experimental data show the 47 pm spacing of a Ge 114 crystal imaged with 11%-18% contrast at a 60%-95% confidence level, providing the first direct evidence for sub-50-pm resolution in annular dark-field scanning transmission electron microscopy imaging.
- Published
- 2009
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76. Effect of ion distribution on conductivity of block copolymer electrolytes.
- Author
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Gomez ED, Panday A, Feng EH, Chen V, Stone GM, Minor AM, Kisielowski C, Downing KH, Borodin O, Smith GD, and Balsara NP
- Subjects
- Algorithms, Cations, Electric Conductivity, Lithium chemistry, Microscopy, Electron, Transmission, Models, Chemical, Molecular Weight, Electrolytes, Ions, Nanotechnology methods, Polyethylene Glycols chemistry, Polymers chemistry
- Abstract
Energy-filtered transmission electron microscopy (EFTEM) was used to determine the distribution of lithium ions in solid polymer electrolytes for lithium batteries. The electrolytes of interest are mixtures of bis(trifluoromethane)sulfonimide lithium salt and symmetric poly(styrene-block-ethylene oxide) copolymers (SEO). In contrast to current solid and liquid electrolytes, the conductivity of SEO/salt mixtures increases with increasing molecular weight of the copolymers. EFTEM results show that the salt is increasingly localized in the middle of the poly(ethylene oxide) (PEO) lamellae as the molecular weight of the copolymers is increased. Calculations of the inhomogeneous local stress field in block copolymer microdomains, modeled using self-consistent field theory, provide a quantitative explanation for this observation. These stresses, which increase with increasing molecular weight, interfere with the ability of PEO chains to coordinate with lithium cations near the walls of the PEO channels where ion mobility is expected to be low.
- Published
- 2009
- Full Text
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77. Direct imaging of lattice atoms and topological defects in graphene membranes.
- Author
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Meyer JC, Kisielowski C, Erni R, Rossell MD, Crommie MF, and Zettl A
- Abstract
We present a transmission electron microscopy investigation of graphene membranes, crystalline foils with a thickness of only 1 atom. By using aberration-correction in combination with a monochromator, 1-A resolution is achieved at an acceleration voltage of only 80 kV. The low voltage is crucial for the stability of these membranes. As a result, every individual carbon atom in the field of view is detected and resolved. We observe a highly crystalline lattice along with occasional point defects. The formation and annealing of Stone-Wales defects is observed in situ. Multiple five- and seven-membered rings appear exclusively in combinations that avoid dislocations and disclinations, in contrast to previous observations on highly curved (tube- or fullerene-like) graphene surfaces.
- Published
- 2008
- Full Text
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78. Detection of single atoms and buried defects in three dimensions by aberration-corrected electron microscope with 0.5-A information limit.
- Author
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Kisielowski C, Freitag B, Bischoff M, van Lin H, Lazar S, Knippels G, Tiemeijer P, van der Stam M, von Harrach S, Stekelenburg M, Haider M, Uhlemann S, Müller H, Hartel P, Kabius B, Miller D, Petrov I, Olson EA, Donchev T, Kenik EA, Lupini AR, Bentley J, Pennycook SJ, Anderson IM, Minor AM, Schmid AK, Duden T, Radmilovic V, Ramasse QM, Watanabe M, Erni R, Stach EA, Denes P, and Dahmen U
- Abstract
The ability of electron microscopes to analyze all the atoms in individual nanostructures is limited by lens aberrations. However, recent advances in aberration-correcting electron optics have led to greatly enhanced instrument performance and new techniques of electron microscopy. The development of an ultrastable electron microscope with aberration-correcting optics and a monochromated high-brightness source has significantly improved instrument resolution and contrast. In the present work, we report information transfer beyond 50 pm and show images of single gold atoms with a signal-to-noise ratio as large as 10. The instrument's new capabilities were exploited to detect a buried Sigma3 {112} grain boundary and observe the dynamic arrangements of single atoms and atom pairs with sub-angstrom resolution. These results mark an important step toward meeting the challenge of determining the three-dimensional atomic-scale structure of nanomaterials.
- Published
- 2008
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79. A quantitative procedure to probe for compositional inhomogeneities in InxGa1-xN alloys.
- Author
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Bartel TP and Kisielowski C
- Abstract
The distribution of indium in a GaN/InxGa1-xN/AlyGa1-yN quantum well with x+/-Deltax=0.24+/-0.07 is quantitatively investigated by extraction of displacement fields from lattice images. Simulations accurately describe the measured strain relaxation across a wedge-shaped sample for a sample thickness up to 150nm. The proportionality between indium concentration and resulting lattice constant cx is approximated by cx=0.5185+0.111xnm. In general, it is challenging to discriminate the effects of random alloying against clustering. In InxGa1-xN this is particularly true at low indium concentrations x<0.2. For an accurate quantitative analysis, sample preparation and imaging were developed such that radiation damage can be recognized if present. Further, an analysis of detection limits and knowledge of the sample thickness are crucial for obtaining reproducible results. Data averaging is necessary to reach sufficient precision. Consequently, the size of the indium-rich clusters is poorly known if x is small. Beyond the interest in physical properties of InxGa1-xN alloys, the analysis of strain and its relaxation exemplifies how quantitative analysis is possible at an atomic level and is in excellent agreement with theoretical predictions.
- Published
- 2008
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80. 3-D reconstruction of the atomic positions in a simulated gold nanocrystal based on discrete tomography: prospects of atomic resolution electron tomography.
- Author
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Jinschek JR, Batenburg KJ, Calderon HA, Kilaas R, Radmilovic V, and Kisielowski C
- Abstract
A novel reconstruction procedure is proposed to achieve atomic resolution in electron tomography. The method exploits the fact that crystals are discrete assemblies of atoms (atomicity). This constraint enables us to obtain a three-dimensional (3-D) reconstruction of test structures from less than 10 projections even in the presence of noise and defects. Phase contrast transmission electron microscopy (TEM) images of a gold nanocrystal were simulated in six different zone axes. The discrete number of atoms in every column is determined by application of the channelling theory to reconstructed electron exit waves. The procedure is experimentally validated by experiments with gold samples. Our results show that discrete tomography recovers the shape of the particle as well as the position of its 309 atoms from only three projections. Experiments on a nanocrystal that contains several missing atoms, both on the surface and in the core of the nanocrystal, while considering a high noise level in each simulated image were performed to prove the stability of the approach to reconstruct defects. The algorithm is well capable of handling structural defects in a highly noisy environment, even if this causes atom count "errors" in the projection data.
- Published
- 2008
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81. Layer resolved structural relaxation at the surface of magnetic FePt icosahedral nanoparticles.
- Author
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Wang RM, Dmitrieva O, Farle M, Dumpich G, Ye HQ, Poppa H, Kilaas R, and Kisielowski C
- Abstract
The periodic shell structure and surface reconstruction of metallic FePt nanoparticles with icosahedral structure has been quantitatively studied by high-resolution transmission electron microscopy with focal series reconstruction with sub-angstrom resolution. The icosahedral FePt nanoparticles fabricated by the gas phase condensation technique in vacuum have been found to be surprisingly oxidation resistant and stable under electron beam irradiation. We find the lattice spacing of (111) planes in the surface region to be size dependent and to expand by as much as 9% with respect to the bulk value of Fe52Pt48. Controlled removal of the (111) surface layers in situ results in a similar outward relaxation of the new surface layer. This unusually large layerwise outward relaxation is discussed in terms of preferential Pt segregation to the surface forming a Pt enriched shell around a Fe-rich Fe/Pt core.
- Published
- 2008
- Full Text
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82. Electron channelling based crystallography.
- Author
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Van Aert S, Geuens P, Van Dyck D, Kisielowski C, and Jinschek JR
- Abstract
Electron channelling occurs when the incident electron beam is parallel to the atom columns of an object, such as a crystal or a particular crystal defect. Then, the electrons are trapped in the electrostatic potential of an atom column in which they scatter dynamically. This picture provides physical insight and explains why a one-to-one correspondence is maintained between the exit wave and the projected structure, even in case of strong dynamical scattering. Moreover, the theory is very useful to invert the dynamical scattering, that is, to derive the projected structure from the exit wave. Finally, it can be used to determine the composition of an atom column with single atom sensitivity or to explain dynamical electron diffraction effects. In this paper, an overview of the channelling theory will be given together with some recent applications.
- Published
- 2007
- Full Text
- View/download PDF
83. A transmission electron microscopy study of mineralization in age-induced transparent dentin.
- Author
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Porter AE, Nalla RK, Minor A, Jinschek JR, Kisielowski C, Radmilovic V, Kinney JH, Tomsia AP, and Ritchie RO
- Subjects
- Adult, Age Factors, Aged, Aging, Hardness, Humans, Ions, Microscopy, Atomic Force, Microscopy, Electron, Transmission instrumentation, Nanotechnology, Tooth chemistry, X-Ray Diffraction, Biocompatible Materials chemistry, Dental Materials chemistry, Dentin chemistry, Microscopy, Electron, Transmission methods, Tooth pathology, Tooth Demineralization
- Abstract
It is known that fractures are more likely to occur in altered teeth, particularly following restoration or endodontic repair; consequently, it is important to understand the structure of altered forms of dentin, the most abundant tissue in the human tooth, in order to better define the increased propensity for such fractures. Transparent (or sclerotic) dentin, wherein the dentinal tubules become occluded with mineral as a natural progressive consequence of aging, is one such altered form. In the present study, high-resolution transmission electron microscopy is used to investigate the effect of aging on the mineral phase of dentin. Such studies revealed that the intertubular mineral crystallites were smaller in transparent dentin, and that the intratubular mineral (larger crystals deposited within the tubules) was chemically similar to the surrounding intertubular mineral. Exit-wave reconstructed lattice-plane images suggested that the intratubular mineral had nanometer-size grains. These observations support a "dissolution and reprecipitation" mechanism for the formation of transparent dentin.
- Published
- 2005
- Full Text
- View/download PDF
84. Nonlinear imaging using annular dark field TEM.
- Author
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Bals S, Kilaas R, and Kisielowski C
- Abstract
Annular dark field TEM images exhibit a dominant mass-thickness contrast that can be quantified to extract single atom scattering cross sections. On top of this incoherent background, additional lattice fringes appear with a nonlinear information limit of 1.2A at 150 kV. The formation of these fringes is described by coherent nonlinear imaging theory and good agreement is found between experimental and simulated images. Calculations furthermore predict that the use of aberration corrected microscopes will improve the image quality dramatically.
- Published
- 2005
- Full Text
- View/download PDF
85. Distortion and segregation in a dislocation core region at atomic resolution.
- Author
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Xu X, Beckman SP, Specht P, Weber ER, Chrzan DC, Erni RP, Arslan I, Browning N, Bleloch A, and Kisielowski C
- Abstract
The structure of an isolated, Ga terminated, 30 degree partial dislocation in GaAs:Be is determined by high resolution transmission electron microscopes and focal series reconstruction. The positions of atomic columns in the core region are measured to an accuracy of better than 10 pm. A quantitative comparison of the structure predicted by an ab initio electronic structure total energy calculation to the experiment indicates that theory and experiment agree to within 20 pm. Further analysis shows the deviations between theory and experiment appear to be systematic. Electron energy loss spectroscopy establishes that defects segregate to the core region, thus accounting for the systematic deviations.
- Published
- 2005
- Full Text
- View/download PDF
86. Bicrystalline hematite nanowires.
- Author
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Wang R, Chen Y, Fu Y, Zhang H, and Kisielowski C
- Abstract
Bicrystalline nanowires of hematite (alpha-Fe(2)O(3)) have been successfully synthesized by the oxidation of pure iron. The product was characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy (TEM), high-resolution TEM in combination with focal series reconstruction, energy-dispersive X-ray spectroscopy, and electron energy-loss spectroscopy. The bicrystalline nanowires have diameters of 20-80 nm and lengths up to 20 microm. All of the investigated materials are found to be alpha-Fe(2)O(3) with a rhombohedral crystal structure. Investigations indicate that most of the bicrystalline nanowires are nanotwins with ellipsoidal heads. The orientation relationship between the nanotwins can be described as (110)(M)//(110)(T), [110](M)//[0](T). An energy-filtered TEM investigation indicates that the ellipsoidal head is iron-rich. The growth mechanism of such unique nanostructures is considered to be a solid-phase growth via surface and internal diffusions of molecules from base to tip.
- Published
- 2005
- Full Text
- View/download PDF
87. Interface structure and atomic bonding characteristics in silicon nitride ceramics.
- Author
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Ziegler A, Idrobo JC, Cinibulk MK, Kisielowski C, Browning ND, and Ritchie RO
- Abstract
Direct atomic resolution images have been obtained that illustrate how a range of rare-earth atoms bond to the interface between the intergranular phase and the matrix grains in an advanced silicon nitride ceramic. It has been found that each rare-earth atom bonds to the interface at a different location, depending on atom size, electronic configuration, and the presence of oxygen at the interface. This is the key factor to understanding the origin of the mechanical properties in these ceramics and will enable precise tailoring in the future to critically improve the materials' performance in wide-ranging applications.
- Published
- 2004
- Full Text
- View/download PDF
88. Thin dielectric film thickness determination by advanced transmission electron microscopy.
- Author
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Diebold AC, Foran B, Kisielowski C, Muller DA, Pennycook SJ, Principe E, and Stemmer S
- Subjects
- Image Processing, Computer-Assisted, Microscopy, Electron, Scanning Transmission methods, Sensitivity and Specificity, Silicon Dioxide chemistry, Microscopy, Electron methods
- Abstract
High-resolution transmission electron microscopy (HR-TEM) has been used as the ultimate method of thickness measurement for thin films. The appearance of phase contrast interference patterns in HR-TEM images has long been confused as the appearance of a crystal lattice by nonspecialists. Relatively easy to interpret crystal lattice images are now directly observed with the introduction of annular dark-field detectors for scanning TEM (STEM). With the recent development of reliable lattice image processing software that creates crystal structure images from phase contrast data, HR-TEM can also provide crystal lattice images. The resolution of both methods has been steadily improved reaching now into the sub-Angstrom region. Improvements in electron lens and image analysis software are increasing the spatial resolution of both methods. Optimum resolution for STEM requires that the probe beam be highly localized. In STEM, beam localization is enhanced by selection of the correct aperture. When STEM measurement is done using a highly localized probe beam, HR-TEM and STEM measurement of the thickness of silicon oxynitride films agree within experimental error. In this article, the optimum conditions for HR-TEM and STEM measurement are discussed along with a method for repeatable film thickness determination. The impact of sample thickness is also discussed. The key result in this article is the proposal of a reproducible method for film thickness determination.
- Published
- 2003
- Full Text
- View/download PDF
89. Imaging columns of the light elements carbon, nitrogen and oxygen with sub Angstrom resolution.
- Author
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Kisielowski C, Hetherington CJ, Wang YC, Kilaas R, O'Keefe MA, and Thust A
- Abstract
It is reported that lattice imaging with a 300 kV field emission microscope in combination with numerical reconstruction procedures can be used to reach an interpretable resolution of about 80 pm for the first time. A retrieval of the electron exit wave from focal series allows for the resolution of single atomic columns of the light elements carbon, nitrogen, and oxygen at a projected nearest neighbor spacing down to 85 pm. Lens aberrations are corrected on-line during the experiment and by hardware such that resulting image distortions are below 80 pm. Consequently, the imaging can be aberration-free to this extent. The resolution enhancement results from increased electrical and mechanical stability of the instrument coupled with a low spherical aberration coefficient of 0.595 + 0.005 mm.
- Published
- 2001
- Full Text
- View/download PDF
90. Sub-Angstrom high-resolution transmission electron microscopy at 300 keV.
- Author
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O'Keefe MA, Hetherington CJ, Wang YC, Nelson EC, Turner JH, Kisielowski C, Malm JO, Mueller R, Ringnalda J, Pan M, and Thust A
- Abstract
Sub-Angstrom transmission electron microscopy has been achieved at the National Center for Electron Microscopy (NCEM) by a one-Angstrom microscope (OAM) project using software and enhanced hardware developed within a Brite-Euram project (Ultramicroscopy 64 (1996) 1). The NCEM OAM provides materials scientists with transmission electron microscopy at a resolution better than 1 A by using extensive image reconstruction to exploit the significantly higher information limit of an FEG-TEM over its Scherzer resolution limit. Reconstruction methods chosen used off-axis holograms and focal series of underfocused images. Measured values of coherence parameters predict an information limit of 0.78 A. Images from a [1 1 0] diamond test specimen show that sub-Angstrom resolution of 0.89 A has been achieved with the OAM using focal series reconstruction.
- Published
- 2001
- Full Text
- View/download PDF
91. Strain-related phenomena in GaN thin films.
- Author
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Kisielowski C, Krüger J, Ruvimov S, Suski T, Ager JW 3rd, Jones E, Liliental-Weber Z, Rubin M, Weber ER, Bremser MD, and Davis RF
- Published
- 1996
- Full Text
- View/download PDF
92. Mapping projected potential, interfacial roughness, and composition in general crystalline solids by quantitative transmission electron microscopy.
- Author
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Schwander P, Kisielowski C, Seibt M, Baumann FH, Kim Y, and Ourmazd A
- Published
- 1993
- Full Text
- View/download PDF
93. Inhomogeneities in plastically deformed silicon single crystals. I. ESR and photo-ESR investigations of p- and n-doped silicon.
- Author
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Kisielowski C, Palm J, Bollig B, and Alexander H
- Published
- 1991
- Full Text
- View/download PDF
94. Inhomogeneities in plastically deformed silicon single crystals. II. Deep-level transient spectroscopy investigations of p- and n-doped silicon.
- Author
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Kisielowski C and Weber ER
- Published
- 1991
- Full Text
- View/download PDF
95. Scanning tunneling microscopy of crystal dislocations in gallium arsenide.
- Author
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Cox G, Szynka D, Poppe U, Graf KH, Urban K, Kisielowski-Kemmerich C, Krüger J, and Alexander H
- Published
- 1990
- Full Text
- View/download PDF
96. Dissociation-width-dependent radiative recombination of electrons and holes at widely split partial dislocations in silicon.
- Author
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Sauer R, Kisielowski-Kemmerich C, and Alexander H
- Published
- 1986
- Full Text
- View/download PDF
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