The interplay of diffusion and heterogeneity in nucleation of the networked Ising model

Nucleation underlies the dynamics of most first-order phase transitions in natural and man-made systems. However, most of the systems of interest are out of equilibrium. Little is known on the effect of nonequilibrium factors on the dynamics of nucleation. Here, we use the forward flux sampling method to investigate the effect of nonequilibrium diffusion on nucleation in small-world Ising networks, wherein spins can be exchanged between nearest-neighboring nodes. We introduce a parameter α to quantify the difference of nucleation rate with and without diffusion. We find that α shows a nonmonotonic dependence on the rewiring probability p of small-world networks. In particular, for different diffusion probability D, a crossover happens at p ≃ 0.17, below which the nucleation rate decreases as D increases, suggesting that the diffusion is against nucleation; while above which the nucleation rate increases with D, indicating that the diffusion is in favor of nucleation. By identifying the distinct features of nucleating clusters along the pathways for different randomness of networks, we reveal the underlying mechanism of such a nontrivial dependence.     

On the nucleation of hadronic domains in the quark-hadron transition

We present numerical results on bubble profiles, nucleation rates and time evolution for a weakly first-order quark-hadron phase transition in different expansion scenarios. We confirm the standard picture of a cosmological first-order phase transition, in which the phase transition is entirely dominated by nucleation. We also show that, even for expansion rates much lower than those expected in heavy-ion collisions nucleation is very unlikely, indicating that the main phase conversion mechanism is spinodal decomposition.     

Nonequilibrium critical behavior in unidirectionally coupled stochastic processes

Phase transitions from an active into an absorbing, inactive state are generically described by the critical exponents of directed percolation (DP), with upper critical dimension d(c)=4. In the framework of single-species reaction-diffusion systems, this universality class is realized by the combined processes A-->A+A, A+A-->A, and A-->0. We study a hierarchy of such DP processes for particle species A,B,..., unidirectionally coupled via the reactions A-->B, ...(with rates mu(AB),...). When the DP critical points at all levels coincide, multicritical behavior emerges, with density exponents beta(i) which are markedly reduced at each hierarchy level i> or =2. This scenario can be understood on the basis of the mean-field rate equations, which yield beta(i)=1/2(i-1) at the multicritical point. Using field-theoretic renormalization-group techniques in d=4-epsilon dimensions, we identify a new crossover exponent phi, and compute phi=1+O(epsilon(2)) in the multicritical regime (for small mu(AB)) of the second hierarchy level. In the active phase, we calculate the fluctuation correction to the density exponent on the second hierarchy level, beta(2)=1/2-epsilon/8+O(epsilon(2)). Outside the multicritical region, we discuss the crossover to ordinary DP behavior, with the density exponent beta(1)=1-epsilon/6+O(epsilon(2)). Monte Carlo simulations are then employed to confirm the crossover scenario, and to determine the values for the new scaling exponents in dimensions d< or =3, including the critical initial slip exponent. Our theory is connected to specific classes of growth processes and to certain cellular automata, and the above ideas are also applied to unidirectionally coupled pair annihilation processes. We also discuss some technical as well as conceptual problems of the loop expansion, and suggest some possible interpretations of these difficulties.     

Sharp Asymptotics for Stochastic Dynamics with Parallel Updating Rule

In this paper we study the metastability problem for a stochastic dynamics with a parallel updating rule; in particular we consider a finite volume Probabilistic Cellular Automaton (PCA) in a small external field at low temperature regime. We are interested in the nucleation of the system, i.e., the typical excursion from the metastable phase (the configuration with all minuses) to the stable phase (the configuration with all pluses), triggered by the formation of a critical droplet. The main result of the paper is the sharp estimate of the nucleation time: we show that the nucleation time divided by its average converges to an exponential random variable and that the rate of the exponential random variable is an exponential function of the inverse temperature β times a prefactor that does not scale with β. Our approach combines geometric and potential theoretic arguments.     

Transition of β to α phase in isotactic polypropylene

In samples of isotactic polypropylene, the influence of the nucleation agent chinacridine permanent red E3B on the crystallization rate and content of α and β modifications and on the rate and mechanism of the β → α transition was investigated using x-ray diffraction, DSC microcalorimetry, and electron microscopy. It was found that, though E3B increases the content of the β phase, it is also a very efficient nucleation agent for the α-phase crystallization. The β → α transition occurring above 140°C could be characterized by a gradual melting and annealing of the β phase, accompanied by a surface crystallization of the α phase on lateral faces of β lamellae by a mechanism similar to cross-branching of α lamellae.     

Nonlinearity in the dynamics of photoinduced nucleation process

Coherent nonlinear dynamics of photoinduced cooperative phenomena at 0 K is studied by numerical calculations on a model of molecular crystals. We found that the photoinduced nucleation process is triggered only when a certain amount of excitation energy is supplied in a narrow part of the system; i.e., there exists the smallest size of the cluster of excited molecules which makes the nucleation possible. As a result, the portion of the cooperatively converted molecules is nonlinearly dependent on the photoexcitation strength, which has been observed in various materials.     

Absence of kinetic effects in reaction-diffusion processes in scale-free networks

We show that the chemical reactions of the model systems of A+A-->0 and A+B-->0 when performed on scale-free networks exhibit drastically different behavior as compared to the same reactions in normal spaces. The exponents characterizing the density evolution as a function of time are considerably higher than 1, implying that both reactions occur at a much faster rate. This is due to the fact that the discerning effects of the generation of a depletion zone (A+A) and the segregation of the reactants (A+B) do not occur at all as in normal spaces. Instead we observe the formation of clusters of A (A+A reaction) and of mixed A and B (A+B reaction) around the hubs of the network. Only at the limit of very sparse networks is the usual behavior recovered.     

Domain coalescence-induced nucleation and anomalous growth of holes in thin polymer blend film

The phase evolution of a thin polymer blend film of polystyrene (PS) and poly(2-vinyl pyridine) (P2VP) triggered by solvent annealing is examined at both the bulk and single-(macro)molecule levels using wide-field microscopy (WFM). The transitions between different evolutionary stages in the nucleation and growth process are clearly visualized in real time and without intermittent breaks. The nucleation of PS holes arises from the coalescence and growth of P2VP domains and the holes expand in a complex manner involving the dewetting of PS and the absorption of P2VP domains into the holes.     

Kinetic Monte Carlo simulations of electrodeposition: Crossover from continuous to instantaneous homogeneous nucleation within Avrami’s law

The influence of lateral adsorbate diffusion on the dynamics of the first-order phase transition in a two-dimensional Ising lattice gas with attractive nearest-neighbor interactions is investigated by means of kinetic Monte Carlo simulations. For example, electrochemical underpotential deposition proceeds by this mechanism. One major difference from adsorption in vacuum surface science is that under control of the electrode potential and in the absence of mass-transport limitations, local adsorption equilibrium is approximately established. We analyze our results using the theory of Kolmogorov, Johnson and Mehl, and Avrami (KJMA), which we extend to an exponentially decaying nucleation rate. Such a decay may occur due to a suppression of nucleation around existing clusters in the presence of lateral adsorbate diffusion. Correlation functions prove the existence of such exclusion zones. By comparison with microscopic results for the nucleation rate I and the interface velocity of the growing clusters v, we can show that the KJMA theory yields the correct order of magnitude for Iv². This is true even though the spatial correlations mediated by diffusion are neglected. The decaying nucleation rate causes a gradual crossover from continuous to instantaneous nucleation, which is complete when the decay of the nucleation rate is very fast on the time scale of the phase transformation. Hence, instantaneous nucleation can be homogeneous, producing negative minima in the two-point correlation functions. We also present in this paper an n-fold way Monte Carlo algorithm for a square lattice gas with adsorption/desorption and lateral diffusion.     

Dynamics of congestion transition triggered by multiple walkers on complex networks

The congestion transition triggered by multiple walkers walking along the shortest path on complex networks is numerically investigated. These networks are composed of nodes that have a finite capacity in analogy to the buffer memory of a computer. It is found that a transition from free-flow phase to congestion phase occurs at a critical walker density f_c, which varies for complex networks with different topological structures. The dynamic pictures of congestion for networks with different topological structures show that congestion on scale-free networks is a percolation process of congestion clusters, while the dynamics of congestion transition on non-scale-free networks is mainly a process of nucleation.     

QCD phase transition in the inhomogeneous universe

We investigate a new mechanism for the cosmological QCD phase transition: inhomogeneous nucleation. The primordial temperature fluctuations, measured to be deltaT/T approximately 10(-5), are larger than the tiny temperature interval in which bubbles would form in the standard picture of homogeneous nucleation. Thus the bubbles nucleate at cold spots. We find the typical distance between bubble centers to be a few meters. This exceeds the estimates from homogeneous nucleation by 2 orders of magnitude. The resulting baryon inhomogeneities may affect primordial nucleosynthesis.     

Controlled multibubble surface cavitation

Heterogeneous bubble nucleation at surfaces has been notorious because of its irreproducibility. Here controlled multibubble surface cavitation is achieved by using a hydrophobic surface patterned with microcavities. The expansion of the nuclei in the microcavities is triggered by a fast lowering of the liquid pressure. The procedure allows us to control and fix the bubble distance within the bubble cluster. We observe a perfect quantitative reproducibility of the cavitation events where the inner bubbles in the two-dimensional cluster are shielded by the outer ones, reflected by their later expansion and their delayed collapse. Apart from the final bubble collapse phase (when jetting flows directed towards the cluster's center develop), the bubble dynamics can be quantitatively described by an extended Rayleigh-Plesset equation, taking pressure modification through the surrounding bubbles into account.     

Heterogeneous nucleation in and out of pores

We study the nucleation of a new thermodynamic phase in pores and find that the nucleation often proceeds via two steps: nucleation of pore filling, and nucleation out of the pore. These two rates have opposing dependencies on pore size, resulting in a pore size at which the nucleation rate of the new phase is maximal. This finding is relevant to attempts to design and use porous media to crystallize proteins.     

The growth mechanism of pentacene-fullerene heteroepitaxial films

The growth of pentacene on C₆₀ film has been studied in real-time by low energy electron microscope. The standing-up phase overgrows on the lying-down phase at room temperature with increasing film thickness. At intermediate temperature we observed two distinct types of nucleation: an earlier nucleation of lying-down phase and a delayed nucleation of standing-up phase on the bare C₆₀ surface between islands of lying-down phase. Further thermal activation control enabled us to tune the types of nucleation and the standing-up phase without co-presence of the lying-down phase could be achieved above ∼70 °C.     

Real-time X-Ray diffraction measurements of the phase transition in KCl shocked along

We have directly imaged subcritical fluctuations during the nucleation phase of three-dimensional islands in strained layer epitaxy. The fluctuations are defect mediated and are found to be large even at low growth temperatures. We attribute the existence of large fluctuations to the time dependence of the supersaturation. This indicates classical nucleation concepts are relevant, even at low growth temperatures.     

Spin-precession vortex and spin-precession supercurrent stability in 3He-B

The stability of the spin-precession currents in superfluid ³He-B is analyzed for the precession angle very close to 104°. In this limit, a spin-precession vortex has a very large core, and the barrier that blocks motion of these large-core vortices across the current streamlines (phase slip) disappears at precession-phase gradients much smaller than critical gradients estimated from the Landau criterion. Nevertheless, spin-precession currents remain stable up to the Landau-critical gradients, since, in this case, there is a barrier, which blocks the phase slip at a very early stage of the vortex-core nucleation. The second-order phase transition between the parity-symmetric and parity-asymmetric spin-precession vortex cores at the precession angle of 126.5° is also predicted. The text was submitted by the author in English.     

Dragon-Kings in rock fracturing: Insights gained from rock fracture tests in the laboratory

In order to shed some lights to the “dragon-kings” concept, this paper re-examines experimental results on rock fracture tests in the laboratory, obtained from acoustic emission monitoring. The fracture of intact rocks as well as rocks containing natural structures (joints, faults, foliations) under constant stress rate loading or creep conditions is generally characterized by typical stages with different underlying physics. The primary phase reflects the initial rupture of pre-existing microcrack population in the sample or in the fault zone. Sub-critical growth dominates the secondary phase. The third phases termed nucleation phase corresponds to the initiation and accelerated growth of the ultimate fracture. The secondary and nucleation phases in both intact rock and faulted rock show power-law (of time-to-failure) increasing event rate and moment release. Samples containing planar structures such as foliations and faults demonstrate very similar features to natural earthquakes including: 1) small number of immediate foreshocks by which fault nucleation zones could be mapped; 2) the critical nucleation zone size is normally a fraction of the sample dimension; 3) a lot of aftershocks concentrated on the fault ruptured during the main event; 4) stress drop due to the main rupture is of the order from a few tens to a few hundreds MPa; 5) b-value drops during foreshocks and recovers during the aftershocks. All these results agree with the suggestion that laboratory measurements require no scaling but can be applied directly to the Earth to represent local fault behavior. The ultimate failure of the sample, or fracture of major asperities on the fault surface, normally lead to extreme events, i.e., dragon-kings, which has a magnitude significantly greater than that expected by the Gutenberg-Richter power-law relation in the magnitude-frequency distribution for either foreshocks or aftershocks. There are at least two mechanisms that may lead to dragon-kings: 1) The power-law increasing event rate and moment release; and 2) Hierarchical fracturing behavior resulting from hierarchical inhomogeneities in the sample. In the 1st mechanism, the final failure corresponds to the end point of the progressive occurrence of events and thus the resulted dragon-king event can be interpreted as a superposition of many small events. While for the 2nd mechanism an event of extreme size is the result of fracture growth stepping from a lower hierarchy into a higher hierarchy on fault surface having asperities characterized by hierarchical distribution (of size or strength) rather than simple fractal distribution. In both mechanisms the underlying physics is that fracture in rocks is hard to stop beyond certain threshold corresponding to the critical nucleation zone size.     

非晶一次晶化过程微观组织演化和生长动力学的相场法研究

在晶化物理模型中添加扩散系数对晶化过程的影响, 采用相场方法研究初始形核率和初始形核半径对一次晶化过程中微观组织和生长动力学的影响。结果表明: 随着初始形核率的增加, 相同时间内非晶一次晶化的晶粒数量逐渐增加, 晶粒尺寸逐渐减小。晶化分数随着演化时间和初始形核率的增加逐渐增大, 初始形核率越大, 相同演化时间内的晶化分数越高。不同初始形核半径情况下, 非晶一次晶化过程中的晶粒数量和尺寸随着演化时间的增加基本保持不变。晶化分数随着演化时间的增加而增大。不同初始形核率和初始形核半径情况下所对应的生长指数均小于1, 表明初始形核率和初始形核半径对晶化方式无影响, 均为一次晶化。改变初始形核率和初始形核半径可调控一次晶化微观组织结构, 而晶粒尺寸及晶化分数直接关系到合金性能。