Simple reflection anisotropy microscopy set-up for CO oxidation studies

Reflection anisotropy microscopy (RAM) is a tool to monitor the optical anisotropy of surfaces with spatial resolution (Rotermund et al 1995 Science 270 608–10). It has been applied to pattern formation during CO oxidation on Pt(110), where it provides a high sensitivity for surface reconstruction and partially also for the coverage with reaction educts (Heumann 2000 Dissertation TU-Berlin). However, the spatial resolution of RAM and the alignment procedure of the optical components were not satisfactory. Here, we give a detailed description of a new set-up, which employs a simple polarizing beam splitter cube as an analyser instead of a Foster prism, offering a higher spatial resolution (<10 μm) and easier alignment of the optical components while retaining the high sensitivity for surface structure. Polarization contrast and spatial resolution of the new set-up are systematically measured, and applications to CO oxidation on uniform and microstructured Pt(110) single crystals are presented

Control of spatiotemporal chaos in catalytic CO oxidation by laser-induced pacemakers

Control of spatiotemporal chaos is achieved in the catalytic oxidation of CO on Pt(110) by localized modification of the kinetic properties of the surface chemical reaction. In the experiment, a small temperature heterogeneity is created on the surface by a focused laser beam. This heterogeneity constitutes a pacemaker and starts to emit target waves. These waves slowly entrain the medium and suppress the spatiotemporal chaos that is present in the absence of control. We compare this experimental result with a numerical study of the Krischer–Eiswirth–Ertl model for CO oxidation on Pt(110). We confirm the experimental findings and identify regimes where complete and partial controls are possible

Geometry-induced pulse instability in microdesigned catalysts: the effect of boundary curvature

We explore the effect of boundary curvature on the instability of reactive pulses in the catalytic oxidation of CO on microdesigned Pt catalysts. Using ring-shaped domains of various radii, we find that the pulses disappear (decollate from the inert boundary) at a turning point bifurcation, and trace this boundary in both physical and geometrical parameter space. These computations corroborate experimental observations of pulse decollation.Comment: submitted to Phys. Rev.

Enhancement of surface activity in CO oxidation on Pt(110) through spatiotemporal laser actuation

We explore the effect of spatiotemporally varying substrate temperature profiles on the dynamics and resulting reaction rate enhancement for the catalytic oxidation of CO on Pt(110). The catalytic surface is "addressed" by a focused laser beam whose motion is computer-controlled. The averaged reaction rate is observed to undergo a characteristic maximum as a function of the speed of this moving laser spot. Experiments as well as modelling are used to explore and rationalize the existence of such an optimal laser speed.Comment: 9 pages, 12 figures, submitted to Phys. Rev.

Guiding chemical pulses through geometry: Y-junctions

We study computationally and experimentally the propagation of chemical pulses in complex geometries.The reaction of interest, CO oxidation, takes place on single crystal Pt(110) surfaces that are microlithographically patterned; they are also addressable through a focused laser beam, manipulated through galvanometer mirrors, capable of locally altering the crystal temperature and thus affecting pulse propagation. We focus on sudden changes in the domain shape (corners in a Y-junction geometry) that can affect the pulse dynamics; we also show how brief, localized temperature perturbations can be used to control reactive pulse propagation.The computational results are corroborated through experimental studies in which the pulses are visualized using Reflection Anisotropy Microscopy.Comment: submitted to Phys. Rev.

Pattern formation in 4:1 resonance of the periodically forced CO oxidation on Pt(110)

Periodically forced oscillatory reaction-diffusion systems may show complex spatiotemporal patterns. At high-frequency resonant forcing, multiple-phase patterns can be found. In the present work, the dynamics of turbulent CO oxidation on Pt(110), forced with the fourth harmonic of the system's natural frequency, is investigated. Experiments result in subharmonic entrainment, where the system locks to a quarter of the forcing frequency. Cluster patterns are observed, where different parts of the pattern show a defined phase difference. The experimental results are compared with numerical simulations using the realistic Krischer-Eiswirth-Ertl model for catalytic CO oxidation. Using the fourth harmonic of an uncoupled surface element's natural frequency, we find 3:1 entrainment with three-phase cluster patterns in a wide parameter range of forcing amplitudes and frequency detuning. Numerical analysis of the spatially extended, turbulent system reveals a remarkable upshift of the mean oscillation frequency compared to homogeneous oscillations. Using the fourth harmonic of the most prominent frequency found in the turbulent system results in four-phase patterns with partial or full 4:1 entrainment, depending on the forcing parameters chosen

High frequency periodic forcing of the oscillatory catalytic CO oxidation on Pt(110)

Resonant periodic forcing is applied to catalytic CO oxidation on platinum (110) in the oscillatory regime. The external parameters are chosen such that the unperturbed system spontaneously develops chemical turbulence. By periodically modulating the CO partial pressure, changes in the spatiotemporal behaviour of the system can be induced: the turbulent behaviour is suppressed and frequency locked patterns with sub-harmonic entrainment develop. A novel gas-driving compressor has been implemented to perform the experimental work

A Roadmap for Transforming Research to Invent the Batteries of the Future Designed within the European Large Scale Research Initiative BATTERY 2030+

This roadmap presents the transformational research ideas proposed by “BATTERY 2030+,” the European large-scale research initiative for future battery chemistries. A “chemistry-neutral” roadmap to advance battery research, particularly at low technology readiness levels, is outlined, with a time horizon of more than ten years. The roadmap is centered around six themes: 1) accelerated materials discovery platform, 2) battery interface genome, with the integration of smart functionalities such as 3) sensing and 4) self-healing processes. Beyond chemistry related aspects also include crosscutting research regarding 5) manufacturability and 6) recyclability. This roadmap should be seen as an enabling complement to the global battery roadmaps which focus on expected ultrahigh battery performance, especially for the future of transport. Batteries are used in many applications and are considered to be one technology necessary to reach the climate goals. Currently the market is dominated by lithium-ion batteries, which perform well, but despite new generations coming in the near future, they will soon approach their performance limits. Without major breakthroughs, battery performance and production requirements will not be sufficient to enable the building of a climate-neutral society. Through this “chemistry neutral” approach a generic toolbox transforming the way batteries are developed, designed and manufactured, will be created

Optical imaging of pattern formation: reflection anisotropy microscopy applied to globally coupled oscillatory CO-oxidation

A reflection anisotropy microscope (RAM) creates the contrast in its images from a change in the polarization orientation of reflected light from a surface. This may stem from local variations of the reconstruction of a surface, being initiated by changes in an adsorption layer. The advantages and disadvantages of a recently improved RAM versus other optical imaging techniques are discussed. We demonstrate the unique features of RAM and present the first experimental findings of so called 2π phase kinks in the globally coupled CO-oxidation on Pt(110)