纳米团簇碰撞生长中的过剩热能和潜热
Excess Thermal Energy and Latent Heat in Nanocluster Collisional Growth
摘要：
纳米团簇可以通过纳米团簇-单体（凝聚）和纳米团簇-纳米团簇（凝聚）碰撞形成和生长。在生长过程中，由于碰撞后的势能和热能交换，产物纳米团簇具有升高的热能。尽管纳米团簇碰撞加热可能是显著的并且强烈地依赖于尺寸，但是没有先前的理论描述这样的现象。我们推导出一个模型来描述过剩的热能，动能增加的产品集群，和潜热，释放到背景的非平衡集群热化，碰撞增长的热量。这两个量都是由一个与势能最小差有关的熵项和一个与尺寸有关的熵项组成的，熵项取决于热容和能量分配。使用金纳米团簇的实例计算表明，碰撞加热可以是重要的和强烈的尺寸依赖性，特别是对于涉及由14-20个原子组成的纳米团簇的反应性碰撞。过多的潜热释放可能对团簇形成和生长有相当大的影响。
英文摘要：
Nanoclusters can form and grow by nanocluster-monomer (condensation) and nanocluster-nanocluster (coagulation) collisions. During growth, product nanoclusters have elevated thermal energies due to potential and thermal energy exchange following a collision. Even though nanocluster collisional heating may be significant and strongly-size dependent, no prior theory describes such phenomenon. We derive a model to describe the excess thermal energy, the kinetic energy increase of the product cluster, and latent heat, the heat released to the background upon thermalization of the non-equilibrium cluster, of collisional growth. Both quantities are composed of an enthalpic term, related to potential energy minimum differences, and a size-dependent entropic term, which hinges upon heat capacity and energy partitioning. Example calculations using gold nanoclusters demonstrate that collisional heating can be important and strongly size dependent, particularly for reactive collisions involving nanoclusters composed of 14-20 atoms. Excessive latent heat release may have considerable implications in cluster formation and growth.
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