Mixing effects in the crystallization of supercooled quantum binary liquids.

Mixing effects in the crystallization of supercooled quantum binary liquids.
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DOI:
10.1063/1.4928280
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发表时间:
2015-04
期刊:
The Journal of chemical physics
影响因子:
--
通讯作者:
M. Kühnel;J. Fernández;F. Tramonto;G. Tejeda;E. Moreno;A. Kalinin;M. Nava;D. Galli;S. Montero;R. Grisenti
M. Kühnel;J. Fernández;F. Tramonto;G. Tejeda;E. Moreno;A. Kalinin;M. Nava;D. Galli;S. Montero;R. Grisenti
中科院分区:
其他
文献类型:
--
作者:
M. Kühnel;J. Fernández;F. Tramonto;G. Tejeda;E. Moreno;A. Kalinin;M. Nava;D. Galli;S. Montero;R. Grisenti

文献摘要

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通过液体微射流拉曼光谱,我们研究了用少量氖稀释的仲氢(pH2)或正氘(oD2)组成的过冷量子液体混合物的结晶过程。我们表明,Ne 杂质的引入会影响结晶动力学,导致测得的 pH2 和 oD2 晶体生长速率显着降低,这与我们之前在过冷 pH2-oD2 液体混合物的工作中发现的情况类似 [Kühnel 等人,Phys.修订版 B 89, 180201(R) (2014)]。我们的实验结果与过冷液体混合物的路径积分模拟相结合,特别表明了测量的生长速率与源自量子离域效应的有效粒径之比之间的相关性。我们进一步表明,混合物的晶体结构在很大程度上也受到氖杂质的存在的影响,这可能通过形成富氖微晶来引发冷冻过程。
By means of Raman spectroscopy of liquid microjets, we have investigated the crystallization process of supercooled quantum liquid mixtures composed of parahydrogen (pH2) or orthodeuterium (oD2) diluted with small amounts of neon. We show that the introduction of the Ne impurities affects the crystallization kinetics in terms of a significant reduction of the measured pH2 and oD2 crystal growth rates, similarly to what found in our previous work on supercooled pH2-oD2 liquid mixtures [Kühnel et al., Phys. Rev. B 89, 180201(R) (2014)]. Our experimental results, in combination with path-integral simulations of the supercooled liquid mixtures, suggest in particular a correlation between the measured growth rates and the ratio of the effective particle sizes originating from quantum delocalization effects. We further show that the crystalline structure of the mixtures is also affected to a large extent by the presence of the Ne impurities, which likely initiate the freezing process through the formation of Ne-rich crystallites.