Department of Chemistry and Biochemistry, California State University at Northridge, 18111 Nordhoff St., Northridge, California 91330, USA.
J Chem Phys. 2013 May 28;138(20):204307. doi: 10.1063/1.4807382.
Laser ablation of copper and silver targets immersed in bulk normal and superfluid (4)He was studied through time-resolved shadowgraph photography. In normal fluid, only a sub-millimeter cavitation bubble is created and immediate formation of metal clusters is observed within a few hundred microseconds. The metal clusters remain spatially tightly focused up to 15 ms, and it is proposed that this observation may find applications in particle image velocimetry. In superfluid helium, the cavitation bubble formation process is distinctly different from the normal fluid. Due to the high thermal conductivity and an apparent lag in the breakdown of superfluidity, about 20% of the laser pulse energy was transferred directly into the liquid and a large gas bubble, up to several millimeters depending on laser pulse energy, is created. The internal temperature of the gas bubble is estimated to exceed 9 K and the following bubble cool down period therefore includes two separate phase transitions: gas-normal liquid and normal liquid-superfluid. The last stage of the cool down process was assigned to the superfluid lambda transition where a sudden formation of large metal clusters is observed. This is attributed to high vorticity created in the volume where the gas bubble previously resided. As shown by theoretical bosonic density functional theory calculations, quantized vortices can trap atoms and dimers efficiently, exhibiting static binding energies up to 22 K. This, combined with hydrodynamic Bernoulli attraction, yields total binding energies as high as 35 K. For larger clusters, the static binding energy increases as a function of the volume occupied in the liquid to minimize the surface tension energy. For heliophobic species an energy barrier develops as a function of the cluster size, whereas heliophilics show barrierless entry into vortices. The present theoretical and experimental observations are used to rationalize the previously reported metal nanowire assembly in both superfluid bulk liquid helium and helium droplets, both of which share the common element of a rapid passage through the lambda point. The origin of vorticity is tentatively assigned to the Zurek-Kibble mechanism. Implications of the large gas bubble formation by laser ablation to previous experiments aimed at implanting atomic and dimeric species in bulk superfluid helium are also discussed, and it is proposed that the developed visualization method should be used as a diagnostic tool in such experiments to avoid measurements in dense gaseous environments.
通过时间分辨阴影摄影研究了浸入体正常和超流(4)He 中的铜和银靶材的激光烧蚀。在正常流体中,仅形成亚毫米空化泡,并在几百微秒内立即观察到金属团簇的形成。金属团簇在 15 毫秒内保持空间上的紧密聚焦,据推测,这一观察结果可能在粒子图像测速法中有应用。在超流氦中,空化泡形成过程与正常流体明显不同。由于高热导率和超流性的明显滞后,约 20%的激光脉冲能量直接传递到液体中,并形成一个大的气泡,其直径取决于激光脉冲能量,可达数毫米。估计气泡内的温度超过 9 K,因此随后的冷却过程包括两个单独的相变:气体-正常液体和正常液体-超流。冷却过程的最后阶段归因于超流λ相变,在此过程中观察到大量金属团簇的突然形成。这归因于先前存在气泡的体积中产生的高涡度。正如理论玻色密度泛函理论计算所示,量子涡旋可以有效地捕获原子和二聚体,表现出高达 22 K 的静态结合能。这与流体力学伯努利吸引力相结合,产生高达 35 K 的总结合能。对于较大的团簇,静态结合能随着在液体中占据的体积增加而增加,以最小化表面张力能。对于疏氦物质,随着团簇尺寸的增加,会形成能量势垒,而亲氦物质则无势垒进入涡旋。目前的理论和实验观察结果用于合理化先前报道的在超流体 bulk 液体氦和氦滴中形成的金属纳米线组装,两者都具有快速通过λ点的共同元素。涡度的起源被暂时归因于 Zurek-Kibble 机制。还讨论了激光烧蚀形成大气体泡对先前旨在将原子和二聚体植入体超流氦中的实验的影响,并提出应将开发的可视化方法用作此类实验中的诊断工具,以避免在密集的气体环境中进行测量。