Jakob Birkedal Wagner

Bio: Jakob Birkedal Wagner is an academic researcher from Technical University of Denmark. The author has contributed to research in topics: Nanowire & Catalysis. The author has an hindex of 51, co-authored 221 publications receiving 8579 citations. Previous affiliations of Jakob Birkedal Wagner include Odense University & Lund University.

Atom-Resolved Imaging of Dynamic Shape Changes in Supported Copper Nanocrystals

Abstract: In situ transmission electron microscopy is used to obtain atom-resolved images of copper nanocrystals on different supports. These are catalysts for methanol synthesis and hydrocarbon conversion processes for fuel cells. The nanocrystals undergo dynamic reversible shape changes in response to changes in the gaseous environment. For zinc oxide-supported samples, the changes are caused both by adsorbate-induced changes in surface energies and by changes in the interfacial energy. For copper nanocrystals supported on silica, the support has negligible influence on the structure. Nanoparticle dynamics must be included in the description of catalytic and other properties of nanomaterials. In situ microscopy offers possibilities for obtaining the relevant atomic-scale insight.

Atomic-Resolution in Situ Transmission Electron Microscopy of a Promoter of a Heterogeneous Catalyst

Abstract: Insight into the location, state, and function of a promoter in heterogeneous catalysis was obtained through atomic-resolution in situ transmission electron microscopy. In the most active ruthenium catalyst for ammonia synthesis known so far, the barium promoter is shown to be located in two different phases in the catalyst. The increased activity is suggested to be related to a two-dimensional barium-oxygen overlayer on the ruthenium crystals. The possibility for conducting such studies for other reactions could add substantially to our current understanding of heterogeneous catalysis. Heterogeneous catalysis plays an increasingly important role in environmental protection processes, in fuel upgrading, and in providing the majority of the chemical building blocks required by contemporary society. Most heterogeneous catalysts of industrial importance are multicomponent materials that are designed by trial-and-error experimentation. Application of even the most sophisticated physical-chemical characterization techniques is usually not sufficient to obtain a complete understanding of the structure of the active site, the reaction mechanism and kinetics, the structural dynamics, and the specific roles of all catalyst components.

Optical properties of rotationally twinned InP nanowire heterostructures.

Abstract: We have developed a technique so that both transmission electron microscopy and microphotoluminescence can be performed on the same semiconductor nanowire over a large range of optical power, thus allowing us to directly correlate structural and optical properties of rotationally twinned zinc blende InP nanowires. We have constructed the energy band diagram of the resulting multiquantum well heterostructure and have performed detailed quantum mechanical calculations of the electron and hole wave functions. The excitation power dependent blue-shift of the photoluminescence can be explained in terms of the predicted staggered band alignment of the rotationally twinned zinc blende/wurzite InP heterostructure and of the concomitant diagonal transitions between localized electron and hole states responsible for radiative recombination. The ability of rotational twinning to introduce a heterostructure in a chemically homogeneous nanowire material and alter in a major way its optical properties opens new possibilities for band-structure engineering.

Giant, level-dependent g factors in InSb nanowire quantum dots.

Abstract: We report on magnetotransport measurements on InSb nanowire quantum dots. The measurements show that the quantum levels of the InSb quantum dots have giant g factors, with absolute values up to approximately 70, the largest value ever reported for semiconductor quantum dots. We also observe that the values of these g factors are quantum level dependent and can differ strongly between different quantum levels. The presence of giant g factors indicates that considerable contributions from the orbital motion of electrons are preserved in the measured InSb nanowire quantum dots, while the level-to-level fluctuations arise from spin-orbit interaction. We have deduced a value of Delta(SO) = 280 mueV for the strength of spin-orbit interaction from an avoided level crossing between the ground state and first excited state of an InSb nanowire quantum dot with a fixed number of electrons.

Strain mapping in free-standing heterostructured wurtzite InAs/InP nanowires

Abstract: The strain distribution in heterostructured wurtzite InAs/InP nanowires is measured by a peak finding technique using high resolution transmission electron microscopy images. We find that nanowires with a diameter of about 20 nm show a 10 nm strained area over the InAs/InP interface and the rest of the wire has a relaxed lattice structure. The lattice parameters and elastic properties for the wurtzite structure of InAs and InP are calculated and a nanowire interface is simulated using finite element calculations. Both the method and the experimental results are validated using a combination of finite element calculations and image simulations.

Bounding the role of black carbon in the climate system: A scientific assessment

Abstract: Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr−1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2 with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2 with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (−0.50 to +1.08) W m−2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (−0.06 W m−2 with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

Signatures of Majorana Fermions in Hybrid Superconductor-Semiconductor Nanowire Devices

Abstract: Majorana fermions are particles identical to their own antiparticles. They have been theoretically predicted to exist in topological superconductors. Here, we report electrical measurements on indium antimonide nanowires contacted with one normal (gold) and one superconducting (niobium titanium nitride) electrode. Gate voltages vary electron density and define a tunnel barrier between normal and superconducting contacts. In the presence of magnetic fields on the order of 100 millitesla, we observe bound, midgap states at zero bias voltage. These bound states remain fixed to zero bias, even when magnetic fields and gate voltages are changed over considerable ranges. Our observations support the hypothesis of Majorana fermions in nanowires coupled to superconductors.

Engineering Metal Organic Frameworks for Heterogeneous Catalysis

Abstract: 2.2. MOFs with Metal Active Sites 4614 2.2.1. Early Studies 4614 2.2.2. Hydrogenation Reactions 4618 2.2.3. Oxidation of Organic Substrates 4620 2.2.4. CO Oxidation to CO2 4626 2.2.5. Phototocatalysis by MOFs 4627 2.2.6. Carbonyl Cyanosilylation 4630 2.2.7. Hydrodesulfurization 4631 2.2.8. Other Reactions 4632 2.3. MOFs with Reactive Functional Groups 4634 2.4. MOFs as Host Matrices or Nanometric Reaction Cavities 4636

Towards the computational design of solid catalysts

Abstract: Over the past decade the theoretical description of surface reactions has undergone a radical development. Advances in density functional theory mean it is now possible to describe catalytic reactions at surfaces with the detail and accuracy required for computational results to compare favourably with experiments. Theoretical methods can be used to describe surface chemical reactions in detail and to understand variations in catalytic activity from one catalyst to another. Here, we review the first steps towards using computational methods to design new catalysts. Examples include screening for catalysts with increased activity and catalysts with improved selectivity. We discuss how, in the future, such methods may be used to engineer the electronic structure of the active surface by changing its composition and structure.