论文标题

部分可观测时空混沌系统的无模型预测

Surface-directed and bulk spinodal decomposition compete to decide the morphology of bimetallic nanoparticles

论文作者

Pankaj, P., Bhattacharyya, Saswata, Chatterjee, Subhradeep

论文摘要

嵌入式域相形形式主义用于研究双金属纳米颗粒(BNP)中的相变途径。散装和表面指导的双旋分解过程及其与毛细血管的相互作用的竞争被确定为BNP形态的主要决定因素。前者的特征是有效的散装驱动力$δ\ tilde {f} $随温度降低而增加,而后者通过通过触点角$θ$捕获的界面能量来表现出来。模拟的形态,即核心壳,janus和逆核壳,将其聚集到$δ\ tilde {f} $ - $θ$ space的不同区域。 Ag-Cu合金系统中使用$δ\ tilde {f} $的$θ$的变化是使用calphad方法计算的,该方法是通过calphad方法来计算的,其中从修改后的管家方程中估算了表面能量。当在形态图上叠加时,此$θ-δ\ tilde {f} $轨迹在形态图上叠加时,可以预测不同的形态转变作为温度的函数。因此,该研究建立了一个独特的热力学框架以及相位模拟,用于通过加工温度的变化来预测和调整纳米颗粒形态。

An embedded-domain phase-field formalism is used for studying phase transformation pathways in bimetallic nanoparticles (BNPs). Competition of bulk and surface-directed spinodal decomposition processes and their interplay with capillarity are identified as the main determinants of BNP morphology. The former is characterized by an effective bulk driving force $Δ\tilde{f}$ which increases with decreasing temperature, while the latter manifests itself through a balance of interfacial energies captured by the contact angle $θ$. The simulated morphologies, namely, core-shell, Janus and inverse core-shell, cluster into distinct regions of the $Δ\tilde{f}$-$θ$ space. Variation of $θ$ with $Δ\tilde{f}$ in the Ag-Cu alloy system is computed as a function of temperature using a CALPHAD approach in which surface energies are estimated from a modified Butler equation. This $θ-Δ\tilde{f}$ trajectory for Ag-Cu, when superimposed on the morphology map, enables the prediction of different morphological transitions as a function of temperature. Therefore, the study establishes a unique thermodynamic framework coupled with phase-field simulations for predicting and tailoring nanoparticle morphology through a variation of processing temperature.

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