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	Author	Mueller, K.; Krause, F.F.; Béché, A.; Schowalter, M.; Galioit, V.; Loeffler, S.; Verbeeck, J.; Zweck, J.; Schattschneider, P.; Rosenauer, A.
	Title	Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction			Type	A1 Journal article
	Year	2014	Publication	Nature communications	Abbreviated Journal	Nat Commun
	Volume	5	Issue		Pages	5653
	Keywords	A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
	Abstract	By focusing electrons on probes with a diameter of 50 pm, aberration-corrected scanning transmission electron microscopy (STEM) is currently crossing the border to probing subatomic details. A major challenge is the measurement of atomic electric fields using differential phase contrast (DPC) microscopy, traditionally exploiting the concept of a field- induced shift of diffraction patterns. Here we present a simplified quantum theoretical interpretation of DPC. This enables us to calculate the momentum transferred to the STEM probe from diffracted intensities recorded on a pixel array instead of conventional segmented bright- field detectors. The methodical development yielding atomic electric field, charge and electron density is performed using simulations for binary GaN as an ideal model system. We then present a detailed experimental study of SrTiO3 yielding atomic electric fields, validated by comprehensive simulations. With this interpretation and upgraded instrumentation, STEM is capable of quantifying atomic electric fields and high-contrast imaging of light atoms.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000347227700003	Publication Date	2014-12-15
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	2041-1723;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	12.124	Times cited	197	Open Access
	Notes	246791 COUNTATOMS; 278510 VORTEX; Hercules; 312483 ESTEEM2; esteem2ta; ECASJO;			Approved	Most recent IF: 12.124; 2014 IF: 11.470
	Call Number	UA @ lucian @ c:irua:122835UA @ admin @ c:irua:122835			Serial	166
Permanent link to this record



	Author	Zhou, K.-G.; Vasu, K.S.; Cherian, C.T.; Neek-Amal, M.; Zhang, J.C.; Ghorbanfekr-Kalashami, H.; Huang, K.; Marshall, O.P.; Kravets, V.G.; Abraham, J.; Su, Y.; Grigorenko, A.N.; Pratt, A.; Geim, A.K.; Peeters, F.M.; Novoselov, K.S.; Nair, R.R.
	Title	Electrically controlled water permeation through graphene oxide membranes			Type	A1 Journal article
	Year	2018	Publication	Nature	Abbreviated Journal	Nature
	Volume	559	Issue	7713	Pages	236-+
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	Controlled transport of water molecules through membranes and capillaries is important in areas as diverse as water purification and healthcare technologies(1-7). Previous attempts to control water permeation through membranes (mainly polymeric ones) have concentrated on modulating the structure of the membrane and the physicochemical properties of its surface by varying the pH, temperature or ionic strength(3,8). Electrical control over water transport is an attractive alternative; however, theory and simulations(9-14) have often yielded conflicting results, from freezing of water molecules to melting of ice(14-16) under an applied electric field. Here we report electrically controlled water permeation through micrometre-thick graphene oxide membranes(17-21). Such membranes have previously been shown to exhibit ultrafast permeation of water(17,22) and molecular sieving properties(18,21), with the potential for industrial-scale production. To achieve electrical control over water permeation, we create conductive filaments in the graphene oxide membranes via controllable electrical breakdown. The electric field that concentrates around these current-carrying filaments ionizes water molecules inside graphene capillaries within the graphene oxide membranes, which impedes water transport. We thus demonstrate precise control of water permeation, from ultrafast permeation to complete blocking. Our work opens up an avenue for developing smart membrane technologies for artificial biological systems, tissue engineering and filtration.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication	London	Editor
	Language		Wos	000438240900052	Publication Date	2018-07-05
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	0028-0836	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	40.137	Times cited	216	Open Access
	Notes	; This work was supported by the Royal Society, Engineering and Physical Sciences Research Council, UK (EP/K016946/1, EP/N013670/1 and EP/P00119X/1), British Council (award reference number 279336045), European Research Council (contract 679689) and Lloyd's Register Foundation. We thank J. Waters for assisting with X-ray measurements and G. Yu for electrical measurements. ;			Approved	Most recent IF: 40.137
	Call Number	UA @ lucian @ c:irua:152420UA @ admin @ c:irua:152420			Serial	5096
Permanent link to this record



	Author	Goris, B.; Bals, S.; van den Broek, W.; Carbó-Argibay, E.; Gómez-Graña, S.; Liz-Marzán, L.M.; Van Tendeloo, G.
	Title	Atomic-scale determination of surface facets in gold nanorods			Type	A1 Journal article
	Year	2012	Publication	Nature materials	Abbreviated Journal	Nat Mater
	Volume	11	Issue	11	Pages	930-935
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract	It is widely accepted that the physical properties of nanostructures depend on the type of surface facets1, 2. For Au nanorods, the surface facets have a major influence on crucial effects such as reactivity and ligand adsorption and there has been controversy regarding facet indexing3, 4. Aberration-corrected electron microscopy is the ideal technique to study the atomic structure of nanomaterials5, 6. However, these images correspond to two-dimensional (2D) projections of 3D nano-objects, leading to an incomplete characterization. Recently, much progress was achieved in the field of atomic-resolution electron tomography, but it is still far from being a routinely used technique. Here we propose a methodology to measure the 3D atomic structure of free-standing nanoparticles, which we apply to characterize the surface facets of Au nanorods. This methodology is applicable to a broad range of nanocrystals, leading to unique insights concerning the connection between the structure and properties of nanostructures.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication	London	Editor
	Language		Wos	000310434600015	Publication Date	2012-10-19
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1476-1122;1476-4660;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	39.737	Times cited	261	Open Access
	Notes	262348 ESMI; Hercules 3; 24691 COUNTATOMS; 267867 PLASMAQUO			Approved	Most recent IF: 39.737; 2012 IF: 35.749
	Call Number	UA @ lucian @ c:irua:101778			Serial	182
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	Author	Liao, Z.; Huijben, M.; Zhong, Z.; Gauquelin, N.; Macke, S.; Green, R.J.; Van Aert, S.; Verbeeck, J.; Van Tendeloo, G.; Held, K.; Sawatzky, G.A.; Koster, G.; Rijnders, G.
	Title	Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling			Type	A1 Journal article
	Year	2016	Publication	Nature materials	Abbreviated Journal	Nat Mater
	Volume	15	Issue	15	Pages	425-431
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract	Controlled in-plane rotation of the magnetic easy axis in manganite heterostructures by tailoring the interface oxygen network could allow the development of correlated oxide-based magnetic tunnelling junctions with non-collinear magnetization, with possible practical applications as miniaturized high-switching-speed magnetic random access memory (MRAM) devices. Here, we demonstrate how to manipulate magnetic and electronic anisotropic properties in manganite heterostructures by engineering the oxygen network on the unit-cell level. The strong oxygen octahedral coupling is found to transfer the octahedral rotation, present in the NdGaO3 (NGO) substrate, to the La2/3Sr1/3MnO3 (LSMO) film in the interface region. This causes an unexpected realignment of the magnetic easy axis along the short axis of the LSMO unit cell as well as the presence of a giant anisotropic transport in these ultrathin LSMO films. As a result we possess control of the lateral magnetic and electronic anisotropies by atomic-scale design of the oxygen octahedral rotation.
	Address	MESA+ Institute for Nanotechnology, University of Twente, PO Box 217, 7500 AE Enschede, The Netherlands
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language	English	Wos	000372591700017	Publication Date	2016-03-07
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1476-1122	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	39.737	Times cited	273	Open Access
	Notes	We would like to acknowledge Dr. Evert Houwman for stimulated discussion. M.H., G.K. and G.R. acknowledge funding from DESCO program of the Dutch Foundation for Fundamental Research on Matter (FOM) with financial support from the Netherlands Organization for Scientific Research (NWO). This work was funded by the European Union Council under the 7th Framework Program (FP7) grant nr NMP3-LA-2010- 246102 IFOX. J.V. and S.V.A. acknowledges funding from FWO project G.0044.13N and G. 0368.15N. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. N.G. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Starting Grant 278510 VORTEX. N.G., S.V.A., J.V. and G.V.T. acknowledge financial support from the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative (Reference No. 312483-ESTEEM2). The Canadian work was supported by NSERC and the Max Planck-UBC Centre for Quantum Materials. Some experiments for this work were performed at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, NSERC, the National Research Council of Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. Z.Z. acknowledges funding from the SFB ViCoM (Austrian Science Fund project ID F4103- N13), and Calculations have been done on the Vienna Scientific Cluster (VSC).; esteem2jra2; esteem2jra3 ECASJO_;			Approved	Most recent IF: 39.737
	Call Number	c:irua:133190 c:irua:133190UA @ admin @ c:irua:133190			Serial	4041
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	Author	Mefford, J.T.; Rong, X.; Abakumov, A.M.; Hardin, W.G.; Dai, S.; Kolpak, A.M.; Johnston, K.P.; Stevenson, K.J.
	Title	Water electrolysis on La_1-xSr_xCoO_3-\delta perovskite electrocatalysts			Type	A1 Journal article
	Year	2016	Publication	Nature communications	Abbreviated Journal	Nat Commun
	Volume	7	Issue	7	Pages	11053
	Keywords	A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
	Abstract	Perovskite oxides are attractive candidates as catalysts for the electrolysis of water in alkaline energy storage and conversion systems. However, the rational design of active catalysts has been hampered by the lack of understanding of the mechanism of water electrolysis on perovskite surfaces. Key parameters that have been overlooked include the role of oxygen vacancies, B-O bond covalency, and redox activity of lattice oxygen species. Here we present a series of cobaltite perovskites where the covalency of the Co-O bond and the concentration of oxygen vacancies are controlled through Sr2+ substitution into La1 – xSrxCoO3 – delta. We attempt to rationalize the high activities of La1 – xSrxCoO3 – delta through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling. Using this approach, we report a material, SrCoO2.7, with a high, room temperature-specific activity and mass activity towards alkaline water electrolysis.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000372721700001	Publication Date	2016-03-23
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	2041-1723	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	12.124	Times cited	278	Open Access
	Notes	Financial support for this work was provided by the R.A. Welch Foundation (grants F-1529 and F-1319). X.R. and A.M.K. acknowledge support from the Skoltech-MIT Center for Electrochemical Energy Storage. Computations were performed using computational resources from XSEDE and NERSC. S.D. was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. We thank D.W. Redman for help with the RHE measurements.			Approved	Most recent IF: 12.124
	Call Number	UA @ lucian @ c:irua:133242			Serial	4276
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	Author	Huijben, M.; Rijnders, G.; Blank, D.H.A.; Bals, S.; Van Aert, S.; Verbeeck, J.; Van Tendeloo, G.; Brinkman, A.; Hilgenkamp, H.
	Title	Electronically coupled complementary interfaces between perovskite band insulators			Type	A1 Journal article
	Year	2006	Publication	Nature materials	Abbreviated Journal	Nat Mater
	Volume	5	Issue		Pages	556-560
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication	London	Editor
	Language		Wos	000238708900021	Publication Date	2006-06-18
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1476-1122;1476-4660;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	39.737	Times cited	315	Open Access
	Notes	Fwo			Approved	Most recent IF: 39.737; 2006 IF: 19.194
	Call Number	UA @ lucian @ c:irua:59713UA @ admin @ c:irua:59713			Serial	1019
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	Author	Van Aert, S.; Batenburg, K.J.; Rossell, M.D.; Erni, R.; Van Tendeloo, G.
	Title	Three-dimensional atomic imaging of crystalline nanoparticles			Type	A1 Journal article
	Year	2011	Publication	Nature	Abbreviated Journal	Nature
	Volume	470	Issue	7334	Pages	374-377
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
	Abstract	Determining the three-dimensional (3D) arrangement of atoms in crystalline nanoparticles is important for nanometre-scale device engineering and also for applications involving nanoparticles, such as optoelectronics or catalysis. A nanoparticles physical and chemical properties are controlled by its exact 3D morphology, structure and composition1. Electron tomography enables the recovery of the shape of a nanoparticle from a series of projection images2, 3, 4. Although atomic-resolution electron microscopy has been feasible for nearly four decades, neither electron tomography nor any other experimental technique has yet demonstrated atomic resolution in three dimensions. Here we report the 3D reconstruction of a complex crystalline nanoparticle at atomic resolution. To achieve this, we combined aberration-corrected scanning transmission electron microscopy5, 6, 7, statistical parameter estimation theory8, 9 and discrete tomography10, 11. Unlike conventional electron tomography, only two images of the targeta silver nanoparticle embedded in an aluminium matrixare sufficient for the reconstruction when combined with available knowledge about the particles crystallographic structure. Additional projections confirm the reliability of the result. The results we present help close the gap between the atomic resolution achievable in two-dimensional electron micrographs and the coarser resolution that has hitherto been obtained by conventional electron tomography.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication	London	Editor
	Language		Wos	000287409100037	Publication Date	2011-02-02
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	0028-0836;1476-4687;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	40.137	Times cited	341	Open Access
	Notes	Esteem 026019			Approved	Most recent IF: 40.137; 2011 IF: 36.280
	Call Number	UA @ lucian @ c:irua:86745			Serial	3644
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	Author	Geim, A.K.; Grigorieva, I.V.; Dubonos, S.V.; Lok, J.G.S.; Maan, J.C.; Filippov, A.E.; Peeters, F.M.
	Title	Phase transitions in individual sub-micrometre superconductors			Type	A1 Journal article
	Year	1997	Publication	Nature	Abbreviated Journal	Nature
	Volume	390	Issue		Pages	259-262
	Keywords	A1 Journal article; Condensed Matter Theory (CMT)
	Abstract
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	A1997YG66700054	Publication Date	2002-07-26
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	0028-0836;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	40.137	Times cited	370	Open Access
	Notes				Approved	Most recent IF: 40.137; 1997 IF: 27.368
	Call Number	UA @ lucian @ c:irua:19265			Serial	2595
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	Author	Sathiya, M.; Abakumov, A.M.; Foix, D.; Rousse, G.; Ramesha, K.; Saubanère, M.; Doublet, M. .; Vezin, H.; Laisa, C.P.; Prakash, A.S.; Gonbeau, D.; Van Tendeloo, G.; Tarascon, J.M.
	Title	Origin of voltage decay in high-capacity layered oxide electrodes			Type	A1 Journal article
	Year	2015	Publication	Nature materials	Abbreviated Journal	Nat Mater
	Volume	14	Issue	14	Pages	230-238
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract	Although Li-rich layered oxides (Li1+xNiyCozMn1−x−y−zO2 > 250 mAh g−1) are attractive electrode materials providing energy densities more than 15% higher than todays commercial Li-ion cells, they suffer from voltage decay on cycling. To elucidate the origin of this phenomenon, we employ chemical substitution in structurally related Li2RuO3 compounds. Li-rich layered Li2Ru1−yTiyO3 phases with capacities of ~240 mAh g−1 exhibit the characteristic voltage decay on cycling. A combination of transmission electron microscopy and X-ray photoelectron spectroscopy studies reveals that the migration of cations between metal layers and Li layers is an intrinsic feature of the chargedischarge process that increases the trapping of metal ions in interstitial tetrahedral sites. A correlation between these trapped ions and the voltage decay is established by expanding the study to both Li2Ru1−ySnyO3 and Li2RuO3; the slowest decay occurs for the cations with the largest ionic radii. This effect is robust, and the finding provides insights into new chemistry to be explored for developing high-capacity layered electrodes that evade voltage decay.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication	London	Editor
	Language		Wos	000348600200024	Publication Date	2014-12-01
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1476-1122;1476-4660;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	39.737	Times cited	395	Open Access
	Notes	246791 Countatoms; 312483 Esteem2; esteem2_ta			Approved	Most recent IF: 39.737; 2015 IF: 36.503
	Call Number	c:irua:132555 c:irua:132555			Serial	2528
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	Author	Loquet, J.-P.; Perret, J.; Fompeyrine, J.; Mächler, E.; Seo, J.W.; Van Tendeloo, G.
	Title	Doubling the critical temperature of La1.9Sr0.1CuO4 using epitaxial strain			Type	A1 Journal article
	Year	1998	Publication	Nature	Abbreviated Journal	Nature
	Volume	394	Issue		Pages	453-456
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000075080400044	Publication Date	2002-07-26
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	0028-0836;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	40.137	Times cited	404	Open Access
	Notes				Approved	Most recent IF: 40.137; 1998 IF: 28.833
	Call Number	UA @ lucian @ c:irua:25676			Serial	757
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	Author	Godefroo, S.; Hayne, M.; Jivanescu, M.; Stesmans, A.; Zacharias, M.; Lebedev, O.I.; Van Tendeloo, G.; Moshchalkov, V.V.
	Title	Classification and control of the origin of photoluminescence from Si nanocrystals			Type	A1 Journal article
	Year	2008	Publication	Nature nanotechnology	Abbreviated Journal	Nat Nanotechnol
	Volume	3	Issue	3	Pages	174-178
	Keywords	A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
	Abstract	Silicon dominates the electronics industry, but its poor optical properties mean that III-V compound semiconductors are preferred for photonics applications. Photoluminescence at visible wavelengths was observed from porous Si at room temperature in 1990, but the origin of these photons (do they arise from highly localized defect states or quantum confinement effects?) has been the subject of intense debate ever since. Attention has subsequently shifted from porous Si to Si nanocrystals, but the same fundamental question about the origin of the photoluminescence has remained. Here we show, based on measurements in high magnetic fields, that defects are the dominant source of light from Si nanocrystals. Moreover, we show that it is possible to control the origin of the photoluminescence in a single sample: passivation with hydrogen removes the defects, resulting in photoluminescence from quantum-confined states, but subsequent ultraviolet illumination reintroduces the defects, making them the origin of the light again.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000254743600017	Publication Date	2008-03-02
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1748-3387;1748-3395;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	38.986	Times cited	426	Open Access
	Notes	Fwo			Approved	Most recent IF: 38.986; 2008 IF: 20.571
	Call Number	UA @ lucian @ c:irua:102630			Serial	373
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	Author	Verbeeck, J.; Tian, H.; Schattschneider, P.
	Title	Production and application of electron vortex beams			Type	A1 Journal article
	Year	2010	Publication	Nature	Abbreviated Journal	Nature
	Volume	467	Issue	7313	Pages	301-304
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract	Vortex beams (also known as beams with a phase singularity) consist of spiralling wavefronts that give rise to angular momentum around the propagation direction. Vortex photon beams are widely used in applications such as optical tweezers to manipulate micrometre-sized particles and in micro-motors to provide angular momentum1, 2, improving channel capacity in optical3 and radio-wave4 information transfer, astrophysics5 and so on6. Very recently, an experimental realization of vortex beams formed of electrons was demonstrated7. Here we describe the creation of vortex electron beams, making use of a versatile holographic reconstruction technique in a transmission electron microscope. This technique is a reproducible method of creating vortex electron beams in a conventional electron microscope. We demonstrate how they may be used in electron energy-loss spectroscopy to detect the magnetic state of materials and describe their properties. Our results show that electron vortex beams hold promise for new applications, in particular for analysing and manipulating nanomaterials, and can be easily produced.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication	London	Editor
	Language		Wos	000281824900033	Publication Date	2010-09-14
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	0028-0836;1476-4687;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	40.137	Times cited	626	Open Access
	Notes	Esteem 026019; Fwo			Approved	Most recent IF: 40.137; 2010 IF: 36.104
	Call Number	UA @ lucian @ c:irua:84878UA @ admin @ c:irua:84878			Serial	2720
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	Author	Zhou, Y.; Che, F.; Liu, M.; Zou, C.; Liang, Z.; De Luna, P.; Yuan, H.; Li, J.; Wang, Z.; Xie, H.; Li, H.; Chen, P.; Bladt, E.; Quintero-Bermudez, R.; Sham, T.-K.; Bals, S.; Hofkens, J.; Sinton, D.; Chen, G.; Sargent, E.H.
	Title	Dopant-induced electron localization drives CO₂ reduction to C₂ hydrocarbons			Type	A1 Journal article
	Year	2018	Publication	Nature chemistry	Abbreviated Journal	Nat Chem
	Volume	10	Issue	10	Pages	974-980
	Keywords	A1 Journal article; Electron microscopy for materials research (EMAT)
	Abstract	The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C-2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C-2 products. Here, we use boron to tune the ratio of Cu delta+ to Cu-0 active sites and improve both stability and C-2-product generation. Simulations show that the ability to tune the average oxidation state of copper enables control over CO adsorption and dimerization, and makes it possible to implement a preference for the electrosynthesis of C-2 products. We report experimentally a C-2 Faradaic efficiency of 79 +/- 2% on boron-doped copper catalysts and further show that boron doping leads to catalysts that are stable for in excess of similar to 40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons.
	Address
	Corporate Author				Thesis
	Publisher		Place of Publication		Editor
	Language		Wos	000442395200013	Publication Date	2018-07-13
	Series Editor		Series Title		Abbreviated Series Title
	Series Volume		Series Issue		Edition
	ISSN	1755-4330; 1755-4349	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	25.87	Times cited	700	Open Access	OpenAccess
	Notes	; This work was supported financially by funding from TOTAL S.A., the Ontario Research Fund: Research Excellence Program, the Natural Sciences and Engineering Research Council of Canada, the CIFAR Bio-Inspired Solar Energy programme, a University of Toronto Connaught grant, the Ministry of Science, Natural Science Foundation of China (21471040, 21271055 and 21501035), the Innovation-Driven Plan in Central South University project (2017CX003), a project from State Key Laboratory of Powder Metallurgy in Central South University, the Thousand Youth Talents Plan of China and Hundred Youth Talents Program of Hunan and the China Scholarship Council programme. This work benefited from the soft X-ray microcharacterization beamline at CLS, sector 20BM at the APS and the Ontario Centre for the Characterisation of Advanced Materials at the University of Toronto. H.Y. acknowledges financial support from the Research Foundation-Flanders (FWO postdoctoral fellowship). C.Z. acknowledges support from the International Academic Exchange Fund for Joint PhD Students from Tianjin University. P.D.L. acknowledges financial support from the Natural Sciences and Engineering Research Council in the form of the Canada Graduate Scholarship-Doctoral award. S.B. and E.B. acknowledge financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS). The authors thank B. Zhang, N. Wang, C. T. Dinh, T. Zhuang, J. Li and Y. Zhao for fruitful discussions, as well as Y. Hu and Q. Xiao from CLS, and Z. Finfrock and M. Ward from APS for their help during the course of study. Computations were performed on the SOSCIP Consortium's Blue Gene/Q computing platform. SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada, Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. ; ecas_sara			Approved	Most recent IF: 25.87
	Call Number	UA @ lucian @ c:irua:153693UA @ admin @ c:irua:153693			Serial	5091
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	Author	Tongay, S.; Sahin, H.; Ko, C.; Luce, A.; Fan, W.; Liu, K.; Zhou, J.; Huang, Y.S.; Ho, C.H.; Yan, J.; Ogletree, D.F.; Aloni, S.; Ji, J.; Li, S.; Li, J.; Peeters, F.M.; Wu, J.;
	Title	Monolayer behaviour in bulk ReS₂ due to electronic and vibrational decoupling			Type	A1 Journal article
	Year	2014	Publication	Nature communications	Abbreviated Journal	Nat Commun
	Volume	5	Issue		Pages	3252
	Keywords	A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
	Abstract	Semiconducting transition metal dichalcogenides consist of monolayers held together by weak forces where the layers are electronically and vibrationally coupled. Isolated monolayers show changes in electronic structure and lattice vibration energies, including a transition from indirect to direct bandgap. Here we present a new member of the family, rhenium disulphide (ReS2), where such variation is absent and bulk behaves as electronically and vibrationally decoupled monolayers stacked together. From bulk to monolayers, ReS2 remains direct bandgap and its Raman spectrum shows no dependence on the number of layers. Interlayer decoupling is further demonstrated by the insensitivity of the optical absorption and Raman spectrum to interlayer distance modulated by hydrostatic pressure. Theoretical calculations attribute the decoupling to Peierls distortion of the 1T structure of ReS2, which prevents ordered stacking and minimizes the interlayer overlap of wavefunctions. Such vanishing interlayer coupling enables probing of two-dimensional-like systems without the need for monolayers.
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	Publisher		Place of Publication		Editor
	Language		Wos	000332666700010	Publication Date	2014-02-06
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	ISSN	2041-1723;	ISBN		Additional Links	UA library record; WoS full record; WoS citing articles
	Impact Factor	12.124	Times cited	806	Open Access
	Notes	; This work was supported by the United States Department of Energy Early Career Award DE-FG02-11ER46796. The high pressure part of this work was supported by COMPRES, the Consortium for Materials Properties Research in Earth Sciences, under National Science Foundation Cooperative Agreement EAR 11-577758. The electron microscopy and nano-Auger measurements were supported by the user programme at the Molecular Foundry, which was supported by the Office of Science, Office of Basic Energy Sciences, of the United States Department of Energy under contract no. DE-AC02-05CH11231. S. A. gratefully acknowledges Dr Virginia Altoe of the Molecular Foundry for help with the TEM data acquisition and analysis. J.L. acknowledges support from the Natural Science Foundation of China for Distinguished Young Scholar (grant nos. 60925016 and 91233120). Y.-S.H. and C.-H. H. acknowledge support from the National Science Council of Taiwan under project nos. NSC 100-2112-M-011-001-MY3 and NSC 101-2221-E-011-052-MY3. H. S. was supported by the FWO Pegasus Marie Curie Long Fellowship programme. The DFT work was supported by the Flemish Science Foundation (FWO-Vl) and the Methusalem programme of the Flemish government. Computational resources were partially provided by TUBITAK ULAKBIM, High Performance and Grid Computing Centre. ;			Approved	Most recent IF: 12.124; 2014 IF: 11.470
	Call Number	UA @ lucian @ c:irua:119247			Serial	2192
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