A Cannibalistic Approach to Grand Canonical Crystal Growth

Authors: Tarak Karmakar1,2*, Pablo M. Piaggi3,2, Claudio Perego4,1,2, Michele Parrinello1,2*

  1. Department of Chemistry and Applied Biosciences, ETH Zürich, c/o USI Campus, Via Giuseppe Buffi 13, CH-6900, Lugano, Ticino, Switzerland
  2. Facoltà di Informatica, Istituto di Scienze Computationali, Università della Svizzera Italiana (USI), Via Giuseppe Buffi 13, CH-6900, Lugano, Ticino, Switzerland
  3. Theory and Simulation of Materials (THEOS), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland
  4. Polymer Theory Department, Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany
  • Corresponding authors emails: tarak.karmakar@phys.chem.ethz.ch, michele.parrinello@phys.chem.ethz.ch

DOI10.24435/materialscloud:2020.0015/v1 (version v1, submitted on 28 January 2020)

How to cite this entry

Tarak Karmakar, Pablo M. Piaggi, Claudio Perego, Michele Parrinello, A Cannibalistic Approach to Grand Canonical Crystal Growth, Materials Cloud Archive (2020), doi: 10.24435/materialscloud:2020.0015/v1.

Description

Canonical molecular dynamics simulations of crystal growth from solution suffer from severe finite-size effects. As the crystal grows, the solute molecules are drawn from the solution to the crystal, leading to a continuous drop in the solution concentration. This is in contrast to experiments in which the crystal grows at an approximately constant supersaturation of a bulk solution. Recently, Perego et al. [J. Chem. Phys.2015, 142, 144113] showed that in a periodic setup in which the crystal is represented as a slab, the concentration in the vicinity of the two surfaces can be kept constant while the molecules are drawn from a part of the solution that acts as a molecular reservoir. This method is quite effective in studying crystallization under controlled supersaturation conditions. However, once the reservoir is depleted, the constant supersaturation conditions cannot be maintained. We propose a variant of this method to tackle this depletion problem by simultaneously dissolving one side of the crystal while letting the other side grow. A continuous supply of particles to the solution due to the crystal dissolution maintains a steady solution concentration and avoids reservoir depletion. In this way, a constant supersaturation condition can be maintained for as long as necessary. We have applied this method to study the growth and dissolution of urea crystal from water solution under constant supersaturation and undersaturation conditions, respectively. The computed growth and dissolution rates are in good agreement with those obtained in previous studies.

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File name Size Description
README.txt
MD5MD5: 22563f9f1920f15bd36c1f3c89485f94
432 Bytes Description of the contents of cannibalistic.tar.gz
cannibalistic.tar.gz
MD5MD5: db9e69db2884b3875ffe35b4b7e928c4
303.9 MiB Plumed input and COLVAR files obtained from A and B type simulations.

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.

Keywords

ERC MARVEL/DD1 Solution crystallization Crystal nucleation and growth Constant chemical potential molecular dynamics simulations crystallization under realistic conditions

Version history

28 January 2020 [This version]