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Title: Mixing effects in the crystallization of supercooled quantum binary liquids

By means of Raman spectroscopy of liquid microjets, we have investigated the crystallization process of supercooled quantum liquid mixtures composed of parahydrogen (pH{sub 2}) or orthodeuterium (oD{sub 2}) 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 pH{sub 2} and oD{sub 2} crystal growth rates, similarly to what found in our previous work on supercooled pH{sub 2}-oD{sub 2} 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.
Authors:
;  [1] ; ; ; ;  [2] ; ;  [3] ;  [3] ;  [4] ;  [1] ;  [5]
  1. Institut für Kernphysik, J. W. Goethe-Universität, Max-von-Laue-Str. 1, 60438 Frankfurt am Main (Germany)
  2. Laboratory of Molecular Fluid Dynamics, Instituto de Estructura de la Materia, CSIC, Serrano 121, 28006 Madrid (Spain)
  3. Laboratorio di Calcolo Parallelo e di Simulazioni di Materia Condensata, Dipartimento di Fisica, Università degli Studi di Milano, Via Celoria 16, 20133 Milano (Italy)
  4. (Switzerland)
  5. (Germany)
Publication Date:
OSTI Identifier:
22493511
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 6; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CORRELATIONS; CRYSTAL GROWTH; CRYSTALLIZATION; DEUTERIUM; FREEZING; HYDROGEN; IMPURITIES; LIQUIDS; MIXTURES; NEON; PARTICLE SIZE; PATH INTEGRALS; RAMAN SPECTROSCOPY; REDUCTION