اشترك بالحزمة الذهبية واحصل على وصول غير محدود شمرا أكاديميا
تسجيل مستخدم جديدFree Energy Barriers for Crystal Nucleation from Fluid Phases
183
0
0.0
(
0
)
اسأل ChatGPT حول البحث
ﻻ يوجد ملخص باللغة العربية
Monte Carlo simulations of crystal nuclei coexisting with the fluid phase in thermal equilibrium in finite volumes are presented and analyzed, for fluid densities from dense melts to the vapor. Generalizing the lever-rule for two-phase coexistence in the canonical ensemble to finite volume, measurements of the nucleus volume together with the pressure and chemical potential of the surrounding fluid allows to extract the surface free energy of the nucleus. Neither the knowledge of the (in general non-spherical) nucleus shape nor of the angle-dependent interface tension is required for this task. The feasibility of the approach is demonstrated for a variant of the Asakura-Oosawa model for colloid-polymer mixtures, which form face-centered cubic colloidal crystals. For a polymer to colloid size ratio of $0.15$, the colloid packing fraction in the fluid phase can be varied from melt values to zero by the variation of an effective attractive potential between the colloids. It is found that the approximation of spherical crystal nuclei often underestimates actual nucleation barriers significantly. Nucleation barriers are found to scale as $Delta F^*=(4pi/3)^{1/3}bar{gamma}(V^*)^{2/3}+const.$ with the nucleus volume $V^*$, and the effective surface tension $bar{gamma}$ that accounts implicitly for the nonspherical shape can be precisely estimated.
قيم البحث
اقرأ أيضاً
In this paper we discuss how the information contained in atomistic simulations of homogeneous nucleation should be used when fitting the parameters in macroscopic nucleation models. We show how the number of solid and liquid atoms in such simulation
s can be determined unambiguously by using a Gibbs dividing surface and how the free energy as a function of the number of solid atoms in the nucleus can thus be extracted. We then show that the parameters of a model based on classical nucleation theory can be fit using the information contained in these free-energy profiles but that the parameters in such models are highly correlated. This correlation is unfortunate as it ensures that small errors in the computed free energy surface can give rise to large errors in the extrapolated properties of the fitted model. To resolve this problem we thus propose a method for fitting macroscopic nucleation models that uses simulations of planar interfaces and simulations of three-dimensional nuclei in tandem. We show that when the parameters of the macroscopic model are fitted in this way the numerical errors for the final fitted model are smaller and that the extrapolated predictions for large nuclei are thus more reliable.
We consider singly-quantized vortex states in a condensate of 52Cr atoms in a pancake trap. We obtain the vortex solutions by numerically solving the Gross-Pitaevskii equation in the rotating frame with no further approximations. The behavior of the
condensate is studied under three different situations concerning the interactions: only s-wave, s-wave plus dipolar and only dipolar. The energy barrier for the nucleation of a vortex is calculated as a function of the vortex displacement from the rotation axis in the three cases. These results are compared to those obtained for contact interaction condensates in the Thomas-Fermi approximation, and to a pseudo-analytical model, showing this latter a very good agreement with the numerical calculation.
In this Letter we report a simulation study in which we compare the solid-liquid interfacial free energy of NaCl at coexistence, with the value that follows from the height of the homogeneous nucleation barrier. We find that the two estimates differ
by more than 100%. Similar, although smaller discrepancies are found for crystals of hard-sphere colloids and of Lennard-Jones (argon) particles. We consider a variety of possible causes for this discrepancy and are forced to conclude that it is due to a finite-size effect that cannot be corrected for by any simple thermodynamic procedure. Importantly, we find that the surface free energies that follow from real nucleation experiments should be subject to large finite size effects. Taking this in to account, we obtain quantitative agreement between the simulation data and the surface free energy of NaCl that follows from nucleation experiments. Our finding suggests that most published solid-liquid surface free energies derived from nucleation experiments will have to be revised.
The Sherrington-Kirkpatrick spin-glass model is investigated by means of Monte Carlo simulations employing a combination of the multi-overlap algorithm with parallel tempering methods. We investigate the finite-size scaling behaviour of the free-ener
gy barriers which are visible in the probability density of the Parisi overlap parameter. Assuming that the mean barrier height diverges with the number of spins N as N^alpha, our data show good agreement with the theoretical value alpha = 1/3.
The knowledge of vortex nucleation barriers is crucial for applications of superconductors, such as single-photon detectors and superconductor-based qubits. Contrarily to the problem of finding energy minima and critical fields, there are no controll
able methods to explore the energy landscape, identify saddle points, and compute associated barriers. Similar problems exist in high-energy physics where the saddle-point configurations are called sphalerons. Here, we present a generalization of the string method to gauge field theories, which allows the calculation of energy barriers in superconductors. We solve the problem of vortex nucleation, assessing the effects of the nonlinearity of the model, complicated geometry, surface roughness, and pinning.
سجل دخول لتتمكن من نشر تعليقات
التعليقات
جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
