Nonexponential decay of velocity correlations in surface diffusion: The role of interactions and ordering

We study the diffusive dynamics of adparticles in two model systems with strong interactions by considering the decay of the single-particle velocity correlation function φ(t). In accordance with previous studies, we find φ(t) to decay nonexponentially and follow a power-law φ(t)∼t−x at intermediate times t, while at long times there is a crossover to an exponential decay. We characterize the behavior of the decay exponent x in detail in various ordered phases and in the vicinity of phase boundaries. We find that within the disordered phase, the behavior of x can be rationalized in terms of interaction effects. Namely, x is typically larger than two in cases where repulsive adparticle–adparticle interactions dominate, while attractive interactions lead to x<2. In ordered phases, our results suggest that the behavior of x is mainly governed by ordering effects that determine the local structure in which adatoms diffuse. Then the decay is characterized by 1

[1]  Pedersen,et al.  Diffusion of N adatoms on the Fe(100) surface , 2000, Physical review letters.

[2]  T. Ala‐Nissila,et al.  Velocity correlations and memory functions in surface diffusion , 2000 .

[3]  T. Ala‐Nissila,et al.  Comment on “Surface diffusion near the points corresponding to continuous phase transitions” [J. Chem. Phys. 109, 3197 (1998)] , 1999 .

[4]  L. Lauhon,et al.  Single molecule thermal rotation and diffusion: Acetylene on Cu(001) , 1999 .

[5]  Steffen Renisch,et al.  Dynamics of adatom motion under the influence of mutual interactions: O/Ru(0001) , 1999 .

[6]  T. Ala‐Nissila,et al.  Memory effects and coverage dependence of surface diffusion in a model adsorption system , 1999 .

[7]  Riccardo Ferrando,et al.  Leapfrog Diffusion Mechanism for One-Dimensional Chains on Missing-Row Reconstructed Surfaces , 1999 .

[8]  R. Ferrando,et al.  Jumps and concerted moves in Cu, Ag, and Au(110) adatom self-diffusion , 1999 .

[9]  I. Vattulainen Memory effects in Arrhenius barriers for surface diffusion , 1998 .

[10]  T. Ala‐Nissila,et al.  Memory expansion for diffusion coefficients , 1998 .

[11]  T. Ala‐Nissila,et al.  Dynamical mean field theory: an efficient method to study surface diffusion coefficients , 1998 .

[12]  T. Ala‐Nissila,et al.  Dynamics of chainlike molecules on surfaces. , 1998, cond-mat/9805394.

[13]  T. Ala‐Nissila,et al.  Adatom dynamics and diffusion in a model of O/W(110) , 1998 .

[14]  T. Ala‐Nissila,et al.  Effect of kinks and concerted diffusion mechanisms on mass transport and growth on stepped metal surfaces , 1997 .

[15]  M. Rao,et al.  Kumar and Rao Reply , 1997 .

[16]  E. Scalas,et al.  LATTICE-GAS THEORY OF COLLECTIVE DIFFUSION IN ADSORBED LAYERS , 1997 .

[17]  B. Swartzentruber Si ad-dimer interactions with steps and islands on Si(001) , 1997 .

[18]  Ying,et al.  Memory effects in the frictional damping of diffusive and vibrational motion of adatoms. , 1996, Physical review. B, Condensed matter.

[19]  K. Fichthorn Diffusion of short-chain molecules on metal surfaces , 1996 .

[20]  G. Kellogg,et al.  Field ion microscope studies of single-atom surface diffusion and cluster nucleation on metal surfaces , 1994 .

[21]  Chen,et al.  Dynamics of adatoms on solid surfaces. , 1994, Physical review. B, Condensed matter.

[22]  V. Zhdanov,et al.  Kinetic phase transitions in simple reactions on solid surfaces , 1994 .

[23]  Wilson,et al.  Effects of adsorption site and surface stress on ordered structures of oxygen adsorbed on W(110). , 1993, Physical review letters.

[24]  T. Ala‐Nissila,et al.  Theory of classical surface diffusion , 1992 .

[25]  R. Gomer Diffusion of adsorbates on metal surfaces , 1990 .

[26]  Kurt Kremer,et al.  The bond fluctuation method: a new effective algorithm for the dynamics of polymers in all spatial dimensions , 1988 .

[27]  A. Naumovets,et al.  Surface diffusion of adsorbates , 1985 .

[28]  D. Chaturvedi Exact solution of continued fraction for tracer diffusion in solids , 1984 .

[29]  J. Ross The chemical physics of solid surfaces and heterogeneous catalysis , 1983 .

[30]  D. A. King,et al.  The Chemical Physics of Solid Surfaces and Heterogeneous Catalysis , 1981 .

[31]  M. Lagally,et al.  Phase transitions in the chemisorbed layer W(110) p (2×1)–O as a function of coverage. I. Experimental , 1978 .

[32]  D. Lévesque,et al.  Long-Time Behavior of the Velocity Autocorrelation Function for a Fluid of Soft Repulsive Particles , 1974 .

[33]  D. Frenkel,et al.  Algebraic decay of velocity fluctuations near a wall , 1998 .

[34]  K. Binder Monte Carlo and molecular dynamics simulations in polymer science , 1995 .

[35]  A. Barabasi,et al.  Fractal concepts in surface growth , 1995 .

[36]  N. H. March,et al.  Atomic dynamics in liquids , 1976 .