Details
| Original language | English |
|---|---|
| Journal | Physical Review B - Condensed Matter and Materials Physics |
| Volume | 63 |
| Issue number | 16 |
| Publication status | Published - 4 Apr 2001 |
Abstract
Local fluctuations and fluctuation-induced transitions in catalytic CO oxidation are studied with field electron microscopy on the (112) facets of a [100]-oriented Pt field emitter tip. The reaction is investigated in the bistable range close to the cusp point (critical point) that terminates the bistability range in pCO, T-parameter space. The amplitude and the spatial coherence of the fluctuations increase on approaching the critical point. The fluctuations are spatially well correlated on each flat (112) facet, but their correlation decays rapidly across stepped regions that terminate the flat facets. On smaller (112) facets, an onset of fluctuation-induced transitions is observed earlier (i.e., further away from the critical point) than for larger (112) facets. The behavior of the reaction system near the cusp point appears to be similar to that of an equilibrium system near the critical point. The observed fluctuations are mimicked in a simple reaction model for CO oxidation on surfaces that incorporates both rapid diffusion of adsorbed CO, and superlattice ordering of adsorbed immobile oxygen. The steady states of the model exhibit a cusp bifurcation, from a regime of bistability to one of monostability. The fluctuations increase near this cusp point, as in experiment. This behavior is analyzed via kinetic Monte Carlo simulations and analytic procedures, focusing on the consequences for fluctuation-induced transitions.
ASJC Scopus subject areas
- Materials Science(all)
- Electronic, Optical and Magnetic Materials
- Physics and Astronomy(all)
- Condensed Matter Physics
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In: Physical Review B - Condensed Matter and Materials Physics, Vol. 63, No. 16, 04.04.2001.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Fluctuations and critical phenomena in catalytic CO oxidation on nanoscale Pt facets
AU - Suchorski, Yu
AU - Beben, J.
AU - Imbihl, R.
AU - James, E. W.
AU - Liu, Da Jiang
AU - Evans, J. W.
PY - 2001/4/4
Y1 - 2001/4/4
N2 - Local fluctuations and fluctuation-induced transitions in catalytic CO oxidation are studied with field electron microscopy on the (112) facets of a [100]-oriented Pt field emitter tip. The reaction is investigated in the bistable range close to the cusp point (critical point) that terminates the bistability range in pCO, T-parameter space. The amplitude and the spatial coherence of the fluctuations increase on approaching the critical point. The fluctuations are spatially well correlated on each flat (112) facet, but their correlation decays rapidly across stepped regions that terminate the flat facets. On smaller (112) facets, an onset of fluctuation-induced transitions is observed earlier (i.e., further away from the critical point) than for larger (112) facets. The behavior of the reaction system near the cusp point appears to be similar to that of an equilibrium system near the critical point. The observed fluctuations are mimicked in a simple reaction model for CO oxidation on surfaces that incorporates both rapid diffusion of adsorbed CO, and superlattice ordering of adsorbed immobile oxygen. The steady states of the model exhibit a cusp bifurcation, from a regime of bistability to one of monostability. The fluctuations increase near this cusp point, as in experiment. This behavior is analyzed via kinetic Monte Carlo simulations and analytic procedures, focusing on the consequences for fluctuation-induced transitions.
AB - Local fluctuations and fluctuation-induced transitions in catalytic CO oxidation are studied with field electron microscopy on the (112) facets of a [100]-oriented Pt field emitter tip. The reaction is investigated in the bistable range close to the cusp point (critical point) that terminates the bistability range in pCO, T-parameter space. The amplitude and the spatial coherence of the fluctuations increase on approaching the critical point. The fluctuations are spatially well correlated on each flat (112) facet, but their correlation decays rapidly across stepped regions that terminate the flat facets. On smaller (112) facets, an onset of fluctuation-induced transitions is observed earlier (i.e., further away from the critical point) than for larger (112) facets. The behavior of the reaction system near the cusp point appears to be similar to that of an equilibrium system near the critical point. The observed fluctuations are mimicked in a simple reaction model for CO oxidation on surfaces that incorporates both rapid diffusion of adsorbed CO, and superlattice ordering of adsorbed immobile oxygen. The steady states of the model exhibit a cusp bifurcation, from a regime of bistability to one of monostability. The fluctuations increase near this cusp point, as in experiment. This behavior is analyzed via kinetic Monte Carlo simulations and analytic procedures, focusing on the consequences for fluctuation-induced transitions.
UR - http://www.scopus.com/inward/record.url?scp=0034868923&partnerID=8YFLogxK
U2 - 10.1103/PhysRevB.63.165417
DO - 10.1103/PhysRevB.63.165417
M3 - Article
AN - SCOPUS:0034868923
VL - 63
JO - Physical Review B - Condensed Matter and Materials Physics
JF - Physical Review B - Condensed Matter and Materials Physics
SN - 1098-0121
IS - 16
ER -