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P. A. Rikvold

Publications and source records attributed to P. A. Rikvold.

At least 37 records · Page 2Linked to original sources
arXiv2006

First-order Reversal Curve Analysis of Phase Transitions in Electrochemical Adsorption: A New Experimental Technique Suggested by Computer Simulations

The first-order reversal curve (FORC) method for analysis of systems undergoing hysteresis is applied to dynamical models of electrochemical adsorption. In this setting, the method can not only differentiate between discontinuous and continuous phase transitions, but can also quite accurately recover equilibrium behavior from dynamic analysis for systems with a continuous phase transition. Discontinuous and continuous phase transitions in a two-dimensional lattice-gas model are compared using the FORC method. The FORC diagram for a discontinuous phase transition is characterized by a negative (unstable) region separating two positive (stable) regions, while such a negative region does not exist for continuous phase transitions. Experimental data for FORC analysis could easily be obtained by simple reprogramming of a potentiostat designed for cyclic-voltammetry experiments.

cond-mat.mtrl-sci↗
arXiv2006

Reply to ``Remarks on the simulation of Cl electrosorption on Ag(100) reported in Electrochimica Acta 50 (2005) 5518"

We reply to remarks by Lang and Horanyi on the meaning of the notion of "electrosorption valency" used in I. Abou Hamad et al., Electrochim. Acta 50 (2005) 5518. It is concluded that, contrary to the assertion of Lang and Horanyi, the magnitude of the current in the external circuit upon adsorption of an ion of charge ze with partial charge transfer is indeed given by an electrosorption valency gamma such that |gamma e| < |ze|. We believe the conclusion of Lang and Horanyi to the contrary is the result of an excessively severe charge-neutrality requirement.

physics.chem-ph↗
arXiv2006

Response of a Model of CO Oxidation with CO Desorption and Diffusion to a Periodic External CO Pressure

We present a study of the dynamical behavior of a Ziff-Gulari-Barshad model with CO desorption and lateral diffusion. Depending on the values of the desorption and diffusion parameters, the system presents a discontinuous phase transition between low and high CO coverage phases. We calculate several points on the coexistence curve between these phases. Inclusion of the diffusion term produces a significant increase in the CO_2 production rate. We further applied a square-wave periodic pressure variation of the partial CO pressure with parameters that can be tuned to modify the catalytic activity. Contrary to the diffusion-free case, this driven system does not present a further enhancement of the catalytic activity, beyond the increase induced by the diffusion under constant CO pressure.

cond-mat.mtrl-sci↗
arXiv2006

Finite-temperature Simulations for Magnetic Nanostructures

We examine different models and methods for studying finite-temperature magnetic hysteresis in nanoparticles and ultrathin films. This includes micromagnetic results for the hysteresis of a single magnetic nanoparticle which is misaligned with respect to the magnetic field. We present results from both a representation of the particle as a one-dimensional array of magnetic rotors, and from full micromagnetic simulations. The results are compared with the Stoner-Wohlfarth model. Results of kinetic Monte Carlo simulations of ultrathin films are also presented. In addition, we discuss other topics of current interest in the modeling of magnetic hysteresis in nanostructures, including kinetic Monte Carlo simulations of dynamic phase transitions and First-Order Reversal Curves.

cond-mat.mtrl-sci↗
arXiv2006

Microstructure and velocity of field-driven solid-on-solid interfaces moving under stochastic dynamics with local energy barriers

We study the microscopic structure and the stationary propagation velocity of (1+1)-dimensional solid-on-solid interfaces in an Ising lattice-gas model, which are driven far from equilibrium by an applied force, such as a magnetic field or a difference in (electro)chemical potential. We use an analytic nonlinear-response approximation [P.A. Rikvold and M. Kolesik, J. Stat. Phys. 100, 377 (2000)] together with kinetic Monte Carlo simulations. Here we consider interfaces that move under Arrhenius dynamics, which include a microscopic energy barrier between the allowed Ising/lattice-gas states. Two different dynamics are studied: the standard one-step dynamic (OSD) [H.C. Kang and W. Weinberg, J. Chem. Phys. 90, 2824 (1992)] and the two-step transition-dynamics approximation (TDA) [T. Ala-Nissila, J. Kjoll, and S.C. Ying, Phys. Rev. B 46, 846 (1992)]. In the OSD the effects of the applied force and the interaction energies in the model factorize in the transition rates (a soft dynamic), while in the TDA such factorization is not possible (a hard dynamic). In full agreement with previous general theoretical results we find that the local interface width under the TDA increases dramatically with the applied force. In contrast, the interface structure with the OSD is only weakly influenced by the force, in qualitative agreement with the theoretical expectations. Results are also obtained for the force-dependence and anisotropy of the interface velocity, which also show differences in good agreement with the theoretical expectations for the differences between soft and hard dynamics. Our results confirm that different stochastic interface dynamics that all obey detailed balance and the same conservation laws nevertheless can lead to radically different interface responses to an applied force.

cond-mat.mtrl-sci↗
arXiv2005

Field-driven solid-on-solid interfaces moving under a stochastic Arrhenius dynamic: effects of the barrier height

We present analytical results and kinetic Monte Carlo simulations for the mobility and microscopic structure of solid-on-solid (SOS) interfaces driven far from equilibrium by an external force, such as an applied field or (electro)chemical potential difference. The interfaces evolve under a specific stochastic dynamic with a local energy barrier (an Arrhenius dynamic), known as the transition dynamics approximation (TDA). We calculate the average height of steps on the interface, the average interface velocity, and the skewness of the interface as functions of the driving force and the height of the energy barrier. We find that the microscopic interface structure depends quite strongly on the barrier height. As the barrier becomes higher, the local interface width decreases and the skewness increases, suggesting increasing short-range correlations between the step heights.

cond-mat.mtrl-sci↗
arXiv2005

Decay of Metastable Nonequilibrium Phases, Enhanced Reaction Rate, and Dynamic Phase Transition in a Model of CO Oxidation with CO Desorption

We present a computational study of the dynamic behavior of a Ziff-Gulari-Barshad model of CO oxidation with CO desorption on a catalytic surface. Our results provide further evidence that below a critical desorption rate the model exhibits a non-equilibrium, first-order phase transition between low and high CO coverage phases. Our kinetic Monte Carlo simulations indicate that the transition process between these phases follows a decay mechanism very similar to the one described by the classic Kolmogorov-Johnson-Mehl-Avrami theory of phase transformation by nucleation and growth. We measure the lifetimes of the metastable phases on each side of the transition line and find that they are strongly dependent on the direction of the transformation, i.e., from low to high coverage or vice versa. Inspired by this asymmetry, we introduce a square-wave periodic external forcing, whose two parameters can be tuned to enhance the catalytic activity. At CO desorption rates below the critical value, we find that this far-from-equilibrium system undergoes a dynamic phase transition between a CO_2 productive phase and a nonproductive one. In the space of the parameters of the periodic external forcing, this nonequilibrium phase transition defines a line of critical points. The maximum enhancement rate for the CO_2 production rate occurs near this critical line.

cond-mat.mtrl-sci↗
arXiv2005

Cl electrosorption on Ag(100): Lateral interactions and electrosorption valency from comparison of Monte Carlo simulations with chronocoulometry experiments

We present Monte Carlo Simulations using an equilibrium lattice-gas model for the electrosorption of Cl on Ag(100) single-crystal surfaces. Fitting the simulated isotherms to chronocoulometry experiments, we extract parameters such as the electrosorption valency gamma and the next-nearest-neighbor lateral interaction energy phi_nnn. Both coverage-dependent and coverage independent gamma were previously studied assuming a constant phi_nnn [I. Abou Hamad, Th. Wandlowski, G. Brown, P.A. Rikvold, J. Electroanal. Chem. 554-555 (2003) 211]. Here, a self-consistent, entirely electrostatic picture of the lateral interactions with a coverage-dependent phi_nnn is developed, and a relationship between phi_nnn and gamma is investigated for Cl on Ag(100).

cond-mat.mtrl-sci↗
arXiv2005

Decay of metastable phases in a model for the catalytic oxidation of CO

We study by kinetic Monte Carlo simulations the dynamic behavior of a Ziff-Gulari-Barshad model with CO desorption for the reaction CO + O $\to$ CO$_2$ on a catalytic surface. Finite-size scaling analysis of the fluctuations and the fourth-order order-parameter cumulant show that below a critical CO desorption rate, the model exhibits a nonequilibrium first-order phase transition between low and high CO coverage phases. We calculate several points on the coexistence curve. We also measure the metastable lifetimes associated with the transition from the low CO coverage phase to the high CO coverage phase, and {\it vice versa}. Our results indicate that the transition process follows a mechanism very similar to the decay of metastable phases associated with {\it equilibrium} first-order phase transitions and can be described by the classic Kolmogorov-Johnson-Mehl-Avrami theory of phase transformation by nucleation and growth. In the present case, the desorption parameter plays the role of temperature, and the distance to the coexistence curve plays the role of an external field or supersaturation. We identify two distinct regimes, depending on whether the system is far from or close to the coexistence curve, in which the statistical properties and the system-size dependence of the lifetimes are different, corresponding to multidroplet or single-droplet decay, respectively. The crossover between the two regimes approaches the coexistence curve logarithmically with system size, analogous to the behavior of the crossover between multidroplet and single-droplet metastable decay near an equilibrium first-order phase transition.

cond-mat.stat-mech↗
arXiv2004

FORC Analysis of homogeneous nucleation in the two-dimensional kinetic Ising model

The first-order reversal curve (FORC) method is applied to the two-dimensional kinetic Ising model. For the system size and magnetic field chosen, the system reverses by the homogeneous nucleation and growth of many droplets. This makes the dynamics of reversal nearly deterministic, in contrast to the strongly disordered systems previously studied by the FORC method. Consequently, the FORC diagrams appear different from those obtained in previous studies. The Kolmogorov-Johnson-Mehl-Avrami (KJMA) theory of phase transformation by nucleation and growth is applied to the system. Reasonable agreement with the Monte Carlo simulations is found, and the FORC method suggests how the KJMA theory could be extended.

cond-mat.stat-mech↗
arXiv2004

Determination of the basic timescale in kinetic Monte Carlo simulations by comparison with cyclic-voltammetry experiments

While kinetic Monte Carlo simulations can provide long-time simulations of the dynamics of physical and chemical systems, it is not yet possible in general to identify the inverse Monte Carlo attempt frequency with a physical timescale. Here we demonstrate such an identification by comparing simulations with experimental data. Using a dynamic lattice-gas model for the electrosorption of Br on Ag(100), we measure the scan-rate dependence of the separation between positive-and negative-going peaks in cyclic-voltammetry (CV) and compare simulated and experimental peak separations. By adjusting the Monte Carlo attempt frequency, good agreement between simulated and experimental peak separations is achieved. It is also found that the uniqueness of such a determination is dependent on the relative values of the adsorption/desorption and diffusion free-energy barriers.

cond-mat.mtrl-sci↗
arXiv2004

Reversal Modes of Simulated Iron Nanopillars in an Obliquely Oriented Field

Stochastic micromagnetic simulations are employed to study switching in three-dimensional magnetic nanopillars exposed to highly misaligned fields. The switching appears to proceed through two different decay modes, characterized by very different average lifetimes and different average values of the transverse magnetization components.

cond-mat.stat-mech↗
arXiv2004

First-principles calculations for the adsorption of water molecules on the Cu(100) surface

First-principles density-functional theory and supercell models are employed to calculate the adsorption of water molecules on the Cu(100) surface. In agreement with the experimental observations, the calculations show that a H2O molecule prefers to bond at a one-fold on-top (T1) surface site with a tilted geometry. At low temperatures, rotational diffusion of the molecular axis of the water molecules around the surface normal is predicted to occur at much higher rates than lateral diffusion of the molecules. In addition, the calculated binding energy of an adsorbed water molecule on the surfaces is significantly smaller than the water sublimation energy, indicating a tendency for the formation of water clusters on the Cu(100) surface.

cond-mat.mtrl-sci↗
arXiv2004

Projective Dynamics in Realistic Models of Nanomagnets

The free-energy extrema governing the magnetization-reversal process for a model of an iron nanopillar are investigated using the projective dynamics method. Since the time evolution of the model is computationally intensive, one could question whether sufficient statistics can be generated, with current resources, to evaluate the position of the metastable configuration. Justification for the fine-grained discretization of the model that we use here is given, and it is shown that tractable results can be obtained for this system on realistic time scales.

cond-mat.stat-mech↗
arXiv2003

Angular Dependence of Switching Properties in Single Fe Nanopillars

The continued increase in areal densities in magnetic recording makes it crucial to understand magnetization reversal in nanoparticles. We present finite-temperature micromagnetic simulations of hysteresis in Fe nanopillars with the long axis tilted at angles from 0 degrees to 90 degrees to the applied sinusoidal field. The field period is 15 ns, and the particle size is 9 x 9 x 150 nm. The system is discretized into a rectangular pillar of 7 x 7 x 101 spins each with uniform magnetization. At low angles, reversal begins at the endcaps and proceeds toward the center of the particle. At ninety degrees, reversal proceeds along the entire length of the particle (save at the ends). The switching field was observed to increase over the entire range of angles, consistent with recent experimental observations. A second, lower-resolution micromagnetic simulation with 1 x 1 x 17 spins, does not agree with experiment, but shows behavior very similar to that of the Stoner-Wohlfarth model of coherent rotation.

cond-mat.mtrl-sci↗
arXiv2003

Projective Dynamics Analysis of Magnetization Reversal

The computational Projective Dynamics method is used to analyze simulations of magnetization reversal in nanoscale magnetic pillars. It is shown that this method can be used to determine the magnetizations corresponding to the metastable minimum and saddle point in the free energy, and the free-energy barrier associated with those points. For the nanopillars studied here, entropy is found to provide a significant contribution to the free-energy barrier which determines the reversal time scale.

cond-mat.stat-mech↗
arXiv2003

Electron Paramagnetic Resonance Linewidths and Lineshapes for the Molecular Magnets Fe8 and Mn12

We study theoretically Electron Paramagentic Resonance (EPR) linewidths for single crystals of the molecular magnets Fe$_8$ and Mn$_{12}$ as functions of energy eigenstates $M_s$, frequency, and temperature when a magnetic field along the easy axis is swept at fixed excitation frequency. This work was motivated by recent EPR experiments. To calculate the linewidths, we use density-matrix equations, including dipolar interactions and distributions of the uniaxial anisotropy parameter $D$ and the Landé $g$ factor. Our calculated linewidths agree well with the experimental data. We also examine the lineshapes of the EPR spectra due to local rotations of the magnetic anisotropy axes caused by defects in samples. Our preliminary results predict that this effect leads to asymmetry in the EPR spectra.

cond-mat↗