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.
Hydrogen-air mixtures are highly flammable. Hydrogen sensors are therefore of paramount importance for timely leak detection during handling. However, existing solutions do not meet the stringent performance targets set by stakeholders, while deactivation due to poisoning, for example by carbon monoxide, is a widely unsolved problem. Here we present a plasmonic metal-polymer hybrid nanomaterial concept, where the polymer coating reduces the apparent activation energy for hydrogen transport into and out of the plasmonic nanoparticles, while deactivation resistance is provided via a tailored tandem polymer membrane. In concert with an optimized volume-to-surface ratio of the signal transducer uniquely offered by nanoparticles, this enables subsecond sensor response times. Simultaneously, hydrogen sorption hysteresis is suppressed, sensor limit of detection is enhanced, and sensor operation in demanding chemical environments is enabled, without signs of long-term deactivation. In a wider perspective, our work suggests strategies for next-generation optical gas sensors with functionalities optimized by hybrid material engineering.
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.
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.
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