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Unraveling the thermodynamic criteria for size-dependent spontaneous phase separation in soft porous crystals

Sven Rogge (UGent) , Michel Waroquier (UGent) and Veronique Van Speybroeck (UGent)
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Abstract
Soft porous crystals (SPCs) harbor a great potential as functional nanoporous materials owing to their stimuli-induced and tuneable morphing between different crystalline phases. These large-amplitude phase transitions are often assumed to occur cooperatively throughout the whole material, which thereby retains its perfect crystalline order. Here, we disprove this paradigm through mesoscale first-principles based molecular dynamics simulations, demonstrating that morphological transitions do induce spatial disorder under the form of interfacial defects and give rise to yet unidentified phase coexistence within a given sample. We hypothesize that this phase coexistence can be stabilized by carefully tuning the experimental control variables through, e.g., temperature or pressure quenching. The observed spatial disorder helps to rationalize yet elusive phenomena in SPCs, such as the impact of crystal downsizing on their flexible nature, thereby identifying the crystal size as a crucial design parameter for stimuli-responsive devices based on SPC nanoparticles and thin films.
Keywords
METAL-ORGANIC FRAMEWORKS, FORCE-FIELD, DYNAMICS, PRESSURE, DEFECTS, MIL-53, SIMULATIONS, BEHAVIOR, SYSTEMS, LIQUID

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Please use this url to cite or link to this publication:

MLA
Rogge, Sven, et al. “Unraveling the Thermodynamic Criteria for Size-Dependent Spontaneous Phase Separation in Soft Porous Crystals.” NATURE COMMUNICATIONS, vol. 10, 2019.
APA
Rogge, S., Waroquier, M., & Van Speybroeck, V. (2019). Unraveling the thermodynamic criteria for size-dependent spontaneous phase separation in soft porous crystals. NATURE COMMUNICATIONS, 10.
Chicago author-date
Rogge, Sven, Michel Waroquier, and Veronique Van Speybroeck. 2019. “Unraveling the Thermodynamic Criteria for Size-Dependent Spontaneous Phase Separation in Soft Porous Crystals.” NATURE COMMUNICATIONS 10.
Chicago author-date (all authors)
Rogge, Sven, Michel Waroquier, and Veronique Van Speybroeck. 2019. “Unraveling the Thermodynamic Criteria for Size-Dependent Spontaneous Phase Separation in Soft Porous Crystals.” NATURE COMMUNICATIONS 10.
Vancouver
1.
Rogge S, Waroquier M, Van Speybroeck V. Unraveling the thermodynamic criteria for size-dependent spontaneous phase separation in soft porous crystals. NATURE COMMUNICATIONS. 2019;10.
IEEE
[1]
S. Rogge, M. Waroquier, and V. Van Speybroeck, “Unraveling the thermodynamic criteria for size-dependent spontaneous phase separation in soft porous crystals,” NATURE COMMUNICATIONS, vol. 10, 2019.
@article{8635877,
  abstract     = {Soft porous crystals (SPCs) harbor a great potential as functional nanoporous materials owing to their stimuli-induced and tuneable morphing between different crystalline phases. These large-amplitude phase transitions are often assumed to occur cooperatively throughout the whole material, which thereby retains its perfect crystalline order. Here, we disprove this paradigm through mesoscale first-principles based molecular dynamics simulations, demonstrating that morphological transitions do induce spatial disorder under the form of interfacial defects and give rise to yet unidentified phase coexistence within a given sample. We hypothesize that this phase coexistence can be stabilized by carefully tuning the experimental control variables through, e.g., temperature or pressure quenching. The observed spatial disorder helps to rationalize yet elusive phenomena in SPCs, such as the impact of crystal downsizing on their flexible nature, thereby identifying the crystal size as a crucial design parameter for stimuli-responsive devices based on SPC nanoparticles and thin films.},
  articleno    = {4842},
  author       = {Rogge, Sven and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {2041-1723},
  journal      = {NATURE COMMUNICATIONS},
  keywords     = {METAL-ORGANIC FRAMEWORKS,FORCE-FIELD,DYNAMICS,PRESSURE,DEFECTS,MIL-53,SIMULATIONS,BEHAVIOR,SYSTEMS,LIQUID},
  language     = {eng},
  pages        = {10},
  title        = {Unraveling the thermodynamic criteria for size-dependent spontaneous phase separation in soft porous crystals},
  url          = {http://dx.doi.org/10.1038/s41467-019-12754-w},
  volume       = {10},
  year         = {2019},
}

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