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Origin of the Energy Barrier to Chemical Reactions of O2 on Al(111): Evidence for Charge Transfer, Not Spin Selection

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Physical Review Letters 2012年第19期109卷 198303-198303页

作者： Florian Libisch Chen Huang Peilin Liao Michele Pavone Emily A. Carter Departments of Mechanical and Aerospace Engineering and Chemistry Program in Applied and Computational Mathematics and Andlinger Center for Energy and the Environment Princeton University Princeton New Jersey 08544 USA Theoretical Division Los Alamos National Laboratory New Mexico 87544 USA

Dissociative adsorption of molecular oxygen on the Al(111) surface exhibits mechanistic complexity that remains surprisingly poorly understood in terms of the underlying physics. Experiments clearly indicate substantial energy barriers and a mysteriously large number of adsorbed single oxygen atoms instead of pairs. Conventional first principles quantum mechanics (density functional theory) predicts no energy barrier at all; instead, spin selection rules have been invoked to explain the barrier. In this Letter, we show that correct barriers arise naturally when embedded correlated electron wave functions are used to capture the physics of the interaction of O2 with the metal surface. The barrier originates from an abrupt charge transfer (from metal to oxygen), which is properly treated within correlated wave function theory but not within conventional density functional theory. Our potential energy surfaces also identify oxygen atom abstraction as the dominant reaction pathway at low incident energies, consistent with measurements, and show that charge transfer occurs in a stepwise fashion.

关键词： CHEMICAL reactions CHARGE transfer ADSORPTION SURFACE chemistry WAVE mechanics QUANTUM theory

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Multilayer thin film growth on crystalline and quasicrystalline surfaces: A phase-field crystal study

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Physical Review B 2012年第24期85卷 245428-245428页

作者： Srevatsan Muralidharan Raika Khodadad Ethan Sullivan Mikko Haataja Department of Mechanical and Aerospace Engineering Princeton Institute for the Science and Technology of Materials (PRISM) Program in Applied and Computational Mathematics (PACM) Princeton University Princeton New Jersey 08544 USA and School of Mathematics Institute for Advanced Study Princeton New Jersey 08540 USA

In this paper, we explore the effects of misfit strain fields on both heterogeneous nucleation behavior and anisotropic growth of islands at submonolayer coverages and compositional patterning at complete monolayer coverage via simulations of a phase-field crystal model. In particular, deposition on top of a herringbone structure and quasicrystalline (QC) substrate are considered, the former representing a system with spatially periodic misfit strain fields arising from the presence of surface dislocations, and the latter representing a system which inherently possesses a wide range of local, aperiodic misfit patterns. In the case of single-component systems, we demonstrate that misfit strain fields lead to heterogeneous nucleation behavior and anisotropic island growth. In the case of QC substrate, a wide range of morphologies, such as coexistence of locally hexagonally ordered atomic clusters within a larger scale arrangement with overall QC symmetry and so-called “starfish” aggregates, is observed in a pure system at submonolayer coverages when the adlayer-substrate interaction strength and lattice mismatch are tuned. In the case of bulk-immiscible binary systems at complete monolayer coverage, strain-stabilized compositional domains emerge at low line tension values for both substrates. Interestingly, the compositional domains on the QC substrate inherit their symmetries at sufficiently low line tension values, while at larger line tension values, the domain structure begins to resemble the classical spinodal microstructure. Such domain structures should be readily observable in colloidal systems in which attractive interparticle and particle-substrate interactions can be tuned.

关键词： THIN films CRYSTALS NUCLEATION DISLOCATIONS in crystals MICROSTRUCTURE

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Spectral Dynamics of Spatially Incoherent Modulation Instability

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Physical Review Letters 2012年第26期108卷 263902-263902页

作者： Can Sun Laura Waller Dmitry V. Dylov Jason W. Fleischer Department of Electrical Engineering Princeton University Princeton New Jersey 08544 USA General Electric Global Research Center Niskayuna New York 12309 USA Program in Applied and Computational Mathematics Princeton University Princeton New Jersey 08544 USA

To date, all experiments in nonlinear statistical optics have relied on beams whose transverse spatial statistics were Gaussian. Here, we present a new technique to generalize these studies by using a spatial light modulator to create spatially incoherent beams with arbitrary spectral distributions. As a specific example of the new dynamics possible, we consider the spatial modulation instability of a partially coherent beam. We show that, for statistical beams of uniform intensity and equal correlation length, the underlying spectral shape determines the threshold and visibility of intensity modulations as well as the spectral profile of the growing sidebands. We demonstrate the behavior using statistical light, but the results will hold for any wave-kinetic system, such as plasma, ultracold gases, and turbulent acoustic waves.

关键词： NONLINEAR optics MODULATION theory SPECTRUM analysis BEAM optics GAUSSIAN processes LIGHT modulators SOUND waves COLD gases

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Density-decomposed orbital-free density functional theory for covalently bonded molecules and materials

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Physical Review B 2012年第23期86卷 235109-235109页

作者： Junchao Xia Emily A. Carter Department of Mechanical and Aerospace Engineering Princeton University Princeton New Jersey 08544-5263 USA Program in Applied and Computational Mathematics and Andlinger Center for Energy and the Environment Princeton University Princeton New Jersey 08544-5263 USA

We propose a density decomposition scheme using a Wang-Govind-Carter- (WGC-) based kinetic energy density functional (KEDF) to accurately and efficiently simulate various covalently bonded molecules and materials within orbital-free (OF) density functional theory (DFT). By using a local, density-dependent scale function, the total density is decomposed into a highly localized density within covalent bond regions and a flattened delocalized density, with the former described by semilocal KEDFs and the latter treated by the WGC KEDF. The new model predicts reasonable equilibrium volumes, bulk moduli, and phase-ordering energies for various semiconductors compared to Kohn-Sham (KS) DFT benchmarks. The decomposition formalism greatly improves numerical stability and accuracy, while retaining computational speed compared to simply applying the original WGC KEDF to covalent materials. The surface energy of Si(100) and various diatomic molecule properties can be stably calculated and also agree well with KSDFT benchmarks. This linear-scaled, computationally efficient, density-partitioned, multi-KEDF scheme opens the door to large-scale simulations of molecules, semiconductors, and insulators with OFDFT.

关键词： PHYSICAL sciences research MOLECULES SEMICONDUCTORS BENCHMARKING (Management) CRYSTALS SURFACE energy COVALENT bonds (Chemistry)

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Density of States for a Specified Correlation Function and the Energy Landscape

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Physical Review Letters 2012年第8期108卷 080601-080601页

作者： C. J. Gommes Y. Jiao S. Torquato Department of Chemical Engineering University of Liège B-4000 Liège Belgium Department of Chemistry Princeton University Princeton New Jersey 08544 USA Program in Applied and Computational Mathematics and Princeton Center for Theoretical Science Princeton University Princeton New Jersey 08544 USA

The degeneracy of two-phase disordered microstructures consistent with a specified correlation function is analyzed by mapping it to a ground-state degeneracy. We determine for the first time the associated density of states via a Monte Carlo algorithm. Our results are explained in terms of the roughness of an energy landscape, defined on a hypercubic configuration space. The use of a Hamming distance in this space enables us to define a roughness metric, which is calculated from the correlation function alone and related quantitatively to the structural degeneracy. This relation is validated for a wide variety of disordered structures.

关键词： ENERGY levels (Quantum mechanics) CORRELATION (Statistics) MICROSTRUCTURE GROUND state (Quantum mechanics) MONTE Carlo method CONFIGURATION space QUANTITATIVE research

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Singularities of quantum control landscapes

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Physical Review A 2012年第1期86卷 013405-013405页

作者： Re-Bing Wu Ruixing Long Jason Dominy Tak-San Ho Herschel Rabitz Department of Automation Tsinghua University Beijing 100084 China and Center for Quantum Information Science and Technology TNList Beijing 100084 China Department of Chemistry Princeton University Princeton New Jersey 08544 USA Program in Applied and Computational Mathematics Princeton University Princeton New Jersey 08544 USA

Quantum control landscape theory was formulated to assess the ease of finding optimal control fields in simulations and in the laboratory. The landscape is the observable as a function of the controls, and a primary goal of the theory is the analysis of landscape features. In what is referred to as the kinematic picture of the landscape, prior work showed that the landscapes are generally free of traps that could halt the search for an optimal control at a suboptimal observable value. The present paper considers the dynamical picture of the landscape, seeking the existence of singular controls, especially of a nonkinematic nature along with an assessment of whether they correspond to traps. We analyze the necessary and sufficient conditions for singular controls to be kinematic or nonkinematic critical solutions and the likelihood of their being encountered while maximizing an observable. An algorithm is introduced to seek singular controls on the landscape in simulations along with an associated Hessian landscape analysis. Simulations are performed for a large number of model finite-level quantum systems, showing that all the numerically identified kinematic and nonkinematic singular critical controls are not traps, in support of the prior empirical observations on the ease of finding high-quality optimal control fields.

关键词： QUANTUM theory LANDSCAPES COMPUTER simulation OPTIMAL control theory ALGORITHMS

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Importance of reference Hamiltonians containing exact exchange for accurate one-shot GW calculations of Cu2O

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Physical Review B 2012年第23期85卷 235142-235142页

作者： Leah Y. Isseroff Emily A. Carter Department of Chemical and Biological Engineering Princeton University Princeton New Jersey 08544-5263 USA Department of Mechanical and Aerospace Engineering Program in Applied and Computational Mathematics and Andlinger Center for Energy and the Environment Princeton University Princeton New Jersey 08544-5263 USA

We show that a “one-shot” GW approach (denoted G0W0) can accurately calculate the photoemission/inverse-photoemission properties of Cu2O. As the results of any perturbative method are heavily dependent on the reference state, the appropriate reference Hamiltonian for G0W0 is identified by evaluating the performance of density-functional-theory-based input wave functions and eigenvalues generated with selected exchange-correlation functionals. It is shown that a reference Hamiltonian employing the hybrid Heyd-Scuseria-Ernzerhof functional used in conjunction with G0W0 produces an accurate photoemission/inverse-photoemission band gap and photoemission spectrum whose character is then further analyzed. The physical origin of why a hybrid functional is required for the zeroth-order wave function is discussed, giving insight into the unique electronic structure of Cu2O in comparison to other transition-metal oxides.

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Efficient coarse simulation of a growing avascular tumor

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Physical Review E 2012年第3期85卷 031912-031912页

作者： Michail E. Kavousanakis Ping Liu Andreas G. Boudouvis John Lowengrub Ioannis G. Kevrekidis School of Chemical Engineering National Technical University of Athens 9 Heroon Polytechniou St. Zographos Athens GR-15780 Greece Department of Chemical and Biological Engineering Princeton University Princeton New Jersey 08544 USA Department of Mathematics University of California 103 MSTB Irvine California 92697 USA Program in Applied and Computational Mathematics Princeton University Princeton New Jersey 08544 USA

The subject of this work is the development and implementation of algorithms which accelerate the simulation of early stage tumor growth models. Among the different computational approaches used for the simulation of tumor progression, discrete stochastic models (e.g., cellular automata) have been widely used to describe processes occurring at the cell and subcell scales (e.g., cell-cell interactions and signaling processes). To describe macroscopic characteristics (e.g., morphology) of growing tumors, large numbers of interacting cells must be simulated. However, the high computational demands of stochastic models make the simulation of large-scale systems impractical. Alternatively, continuum models, which can describe behavior at the tumor scale, often rely on phenomenological assumptions in place of rigorous upscaling of microscopic models. This limits their predictive power. In this work, we circumvent the derivation of closed macroscopic equations for the growing cancer cell populations; instead, we construct, based on the so-called “equation-free” framework, a computational superstructure, which wraps around the individual-based cell-level simulator and accelerates the computations required for the study of the long-time behavior of systems involving many interacting cells. The microscopic model, e.g., a cellular automaton, which simulates the evolution of cancer cell populations, is executed for relatively short time intervals, at the end of which coarse-scale information is obtained. These coarse variables evolve on slower time scales than each individual cell in the population, enabling the application of forward projection schemes, which extrapolate their values at later times. This technique is referred to as coarse projective integration. Increasing the ratio of projection times to microscopic simulator execution times enhances the computational savings. Crucial accuracy issues arising for growing tumors with radial symmetry are addressed by applying th

关键词： SIMULATION methods & models TUMORS -- Growth MATHEMATICAL models CANCER invasiveness STOCHASTIC models computational biology BIONICS PHENOMENOLOGY

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Model reduction for agent-based social simulation: Coarse-graining a civil violence model

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Physical Review E 2012年第6期85卷 066106-066106页

作者： Yu Zou Vladimir A. Fonoberov Maria Fonoberova Igor Mezic Ioannis G. Kevrekidis Department of Chemical and Biological Engineering and Program in Applied and Computational Mathematics Princeton University Princeton New Jersey 08544 USA Aimdyn Inc. 1919 State Street Suite 207 Santa Barbara California 93101 USA Department of Mechanical Engineering University of California Santa Barbara Santa Barbara California 93106 USA

Agent-based modeling (ABM) constitutes a powerful computational tool for the exploration of phenomena involving emergent dynamic behavior in the social sciences. This paper demonstrates a computer-assisted approach that bridges the significant gap between the single-agent microscopic level and the macroscopic (coarse-grained population) level, where fundamental questions must be rationally answered and policies guiding the emergent dynamics devised. Our approach will be illustrated through an agent-based model of civil violence. This spatiotemporally varying ABM incorporates interactions between a heterogeneous population of citizens [active (insurgent), inactive, or jailed] and a population of police officers. Detailed simulations exhibit an equilibrium punctuated by periods of social upheavals. We show how to effectively reduce the agent-based dynamics to a stochastic model with only two coarse-grained degrees of freedom: the number of jailed citizens and the number of active ones. The coarse-grained model captures the ABM dynamics while drastically reducing the computation time (by a factor of approximately 20).

关键词： VIOLENCE SOCIAL dynamics STOCHASTIC models CITIZENS SOCIAL interaction DEGREES of freedom

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Seismic Probes of Solar Interior Magnetic Structure

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Physical Review Letters 2012年第10期109卷 101101-101101页

作者： Shravan Hanasoge Aaron Birch Laurent Gizon Jeroen Tromp Department of Geosciences Princeton University New Jersey 08544 USA Max-Planck Institut für Sonnensystemforschung 37191 Kalenburg-Lindau Germany Georg-August-Universität Institut für Astrophysik D-37077 Göttingen Germany Program for Applied and Computational Mathematics Princeton University New Jersey 08544 USA

Sun spots are prominent manifestations of solar magnetoconvection, and imaging their subsurface structure is an outstanding problem of wide physical importance. Travel times of seismic waves that propagate through these structures are typically used as inputs to inversions. Despite the presence of strongly anisotropic magnetic waveguides, these measurements have always been interpreted in terms of changes to isotropic wave speeds and flow-advection-related Doppler shifts. Here, we employ partial-differential-equation-constrained optimization to determine the appropriate parametrization of the structural properties of the magnetic interior. Seven different wave speeds fully characterize helioseismic wave propagation: the isotropic sound speed, a Doppler-shifting flow-advection velocity, and an anisotropic magnetic velocity. The structure of magnetic media is sensed by magnetoacoustic slow and fast modes and Alfvén waves, each of which propagates at a different wave speed. We show that even in the case of weak magnetic fields, significant errors may be incurred if these anisotropies are not accounted for in inversions. Translation invariance is demonstrably lost. These developments render plausible the accurate seismic imaging of magnetoconvection in the Sun.

关键词： SEISMIC waves -- Speed MAGNETIC structure PARTIAL differential equations DOPPLER effect THEORY of wave motion SUN INTERNAL structure

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