Single-bubble dynamics in nanopores: Transition between homogeneous and heterogeneous nucleation
Single-bubble dynamics in nanopores: Transition between homogeneous and heterogeneous nucleation
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DOI：
10.1103/physrevresearch.2.043400
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发表时间：
2020-12-21
影响因子：
4.2
通讯作者：
Daiguji, Hirofumi
中科院分区：
文献类型：
--
作者：
Paul, Soumyadeep;Hsu, Wei-Lun;Daiguji, Hirofumi
当在薄纳米孔上施加偏置电压时，局部焦耳加热可以导致单泡成核，为研究纳米级气泡行为提供了一个独特的平台，这一点仍然知之甚少。因此，我们研究了填充电解质溶液的固态纳米孔内的气泡成核和崩溃，发现同质/非均质气泡成核与孔径之间存在明显的相关性。当孔径从280 nm增加到525 nm时，成核模式由主要的周期性均匀成核转变为均匀和非均匀成核的非周期性混合成核。通过考虑簇形成的相对自由能成本，定义了均相和非均相成核体系之间的过渡屏障。建立了考虑过渡势垒和接触线在曲面上钉住的热力学模型，确定了非均相成核的可能性。结果表明，我们的热力学分析很好地捕捉到了实验气泡的生成行为，为控制纳米孔中气泡的周期性均匀成核提供了重要的信息。
When applying a voltage bias across a thin nanopore, localized Joule heating can lead to single-bubble nucleation, offering a unique platform for studying nanoscale bubble behavior, which is still poorly understood. Accordingly, we investigate bubble nucleation and collapse inside solid-state nanopores filled with electrolyte solutions and find that there exists a clear correlation between homo/heterogeneous bubble nucleation and the pore diameter. As the pore diameter is increased from 280 to 525 nm, the nucleation regime transitions from predominantly periodic homogeneous nucleation to a nonperiodic mixture of homogeneous and heterogeneous nucleation. A transition barrier between the homogeneous and heterogeneous nucleation regimes is defined by considering the relative free-energy costs of cluster formation. A thermodynamic model considering the transition barrier and contact-line pinning on curved surfaces is constructed, which determines the possibility of heterogeneous nucleation. It is shown that the experimental bubble generation behavior is closely captured by our thermodynamic analysis, providing important information for controlling the periodic homogeneous nucleation of bubbles in nanopores.