---
_id: '9666'
abstract:
- lang: eng
  text: Predicting phase stabilities of crystal polymorphs is central to computational
    materials science and chemistry. Such predictions are challenging because they
    first require searching for potential energy minima and then performing arduous
    free-energy calculations to account for entropic effects at finite temperatures.
    Here, we develop a framework that facilitates such predictions by exploiting all
    the information obtained from random searches of crystal structures. This framework
    combines automated clustering, classification and visualisation of crystal structures
    with machine-learning estimation of their enthalpy and entropy. We demonstrate
    the framework on the technologically important system of TiO2, which has many
    polymorphs, without relying on prior knowledge of known phases. We find a number
    of new phases and predict the phase diagram and metastabilities of crystal polymorphs
    at 1600 K, benchmarking the results against full free-energy calculations.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Aleks
  full_name: Reinhardt, Aleks
  last_name: Reinhardt
- first_name: Chris J.
  full_name: Pickard, Chris J.
  last_name: Pickard
- first_name: Bingqing
  full_name: Cheng, Bingqing
  id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
  last_name: Cheng
  orcid: 0000-0002-3584-9632
citation:
  ama: Reinhardt A, Pickard CJ, Cheng B. Predicting the phase diagram of titanium
    dioxide with random search and pattern recognition. <i>Physical Chemistry Chemical
    Physics</i>. 2020;22(22):12697-12705. doi:<a href="https://doi.org/10.1039/d0cp02513e">10.1039/d0cp02513e</a>
  apa: Reinhardt, A., Pickard, C. J., &#38; Cheng, B. (2020). Predicting the phase
    diagram of titanium dioxide with random search and pattern recognition. <i>Physical
    Chemistry Chemical Physics</i>. Royal Society of Chemistry. <a href="https://doi.org/10.1039/d0cp02513e">https://doi.org/10.1039/d0cp02513e</a>
  chicago: Reinhardt, Aleks, Chris J. Pickard, and Bingqing Cheng. “Predicting the
    Phase Diagram of Titanium Dioxide with Random Search and Pattern Recognition.”
    <i>Physical Chemistry Chemical Physics</i>. Royal Society of Chemistry, 2020.
    <a href="https://doi.org/10.1039/d0cp02513e">https://doi.org/10.1039/d0cp02513e</a>.
  ieee: A. Reinhardt, C. J. Pickard, and B. Cheng, “Predicting the phase diagram of
    titanium dioxide with random search and pattern recognition,” <i>Physical Chemistry
    Chemical Physics</i>, vol. 22, no. 22. Royal Society of Chemistry, pp. 12697–12705,
    2020.
  ista: Reinhardt A, Pickard CJ, Cheng B. 2020. Predicting the phase diagram of titanium
    dioxide with random search and pattern recognition. Physical Chemistry Chemical
    Physics. 22(22), 12697–12705.
  mla: Reinhardt, Aleks, et al. “Predicting the Phase Diagram of Titanium Dioxide
    with Random Search and Pattern Recognition.” <i>Physical Chemistry Chemical Physics</i>,
    vol. 22, no. 22, Royal Society of Chemistry, 2020, pp. 12697–705, doi:<a href="https://doi.org/10.1039/d0cp02513e">10.1039/d0cp02513e</a>.
  short: A. Reinhardt, C.J. Pickard, B. Cheng, Physical Chemistry Chemical Physics
    22 (2020) 12697–12705.
date_created: 2021-07-15T12:37:27Z
date_published: 2020-06-14T00:00:00Z
date_updated: 2023-02-23T14:04:16Z
day: '14'
ddc:
- '530'
doi: 10.1039/d0cp02513e
extern: '1'
external_id:
  arxiv:
  - '1909.08934'
  pmid:
  - '32459228'
file:
- access_level: open_access
  checksum: 0a6872972b1b2e60f9095d39b01753fa
  content_type: application/pdf
  creator: asandaue
  date_created: 2021-07-15T12:43:51Z
  date_updated: 2021-07-15T12:43:51Z
  file_id: '9667'
  file_name: 202_PhysicalChemistryChemicalPhysics_Reinhardt.pdf
  file_size: 3151206
  relation: main_file
  success: 1
file_date_updated: 2021-07-15T12:43:51Z
has_accepted_license: '1'
intvolume: '        22'
issue: '22'
language:
- iso: eng
license: https://creativecommons.org/licenses/by/3.0/
month: '06'
oa: 1
oa_version: Published Version
page: 12697-12705
pmid: 1
publication: Physical Chemistry Chemical Physics
publication_identifier:
  eissn:
  - 1463-9084
  issn:
  - 1463-9076
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: Predicting the phase diagram of titanium dioxide with random search and pattern
  recognition
tmp:
  image: /images/cc_by.png
  legal_code_url: https://creativecommons.org/licenses/by/3.0/legalcode
  name: Creative Commons Attribution 3.0 Unported (CC BY 3.0)
  short: CC BY (3.0)
type: journal_article
user_id: 6785fbc1-c503-11eb-8a32-93094b40e1cf
volume: 22
year: '2020'
...
---
_id: '9668'
abstract:
- lang: eng
  text: Estimating the homogeneous ice nucleation rate from undercooled liquid water
    is crucial for understanding many important physical phenomena and technological
    applications, and challenging for both experiments and theory. From a theoretical
    point of view, difficulties arise due to the long time scales required, as well
    as the numerous nucleation pathways involved to form ice nuclei with different
    stacking disorders. We computed the homogeneous ice nucleation rate at a physically
    relevant undercooling for a single-site water model, taking into account the diffuse
    nature of ice–water interfaces, stacking disorders in ice nuclei, and the addition
    rate of particles to the critical nucleus. We disentangled and investigated the
    relative importance of all the terms, including interfacial free energy, entropic
    contributions and the kinetic prefactor, that contribute to the overall nucleation
    rate. Breaking down the problem into pieces not only provides physical insights
    into ice nucleation, but also sheds light on the long-standing discrepancy between
    different theoretical predictions, as well as between theoretical and experimental
    determinations of the nucleation rate. Moreover, we pinpoint the main shortcomings
    and suggest strategies to systematically improve the existing simulation methods.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Bingqing
  full_name: Cheng, Bingqing
  id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
  last_name: Cheng
  orcid: 0000-0002-3584-9632
- first_name: Christoph
  full_name: Dellago, Christoph
  last_name: Dellago
- first_name: Michele
  full_name: Ceriotti, Michele
  last_name: Ceriotti
citation:
  ama: 'Cheng B, Dellago C, Ceriotti M. Theoretical prediction of the homogeneous
    ice nucleation rate: Disentangling thermodynamics and kinetics. <i>Physical Chemistry
    Chemical Physics</i>. 2018;20(45):28732-28740. doi:<a href="https://doi.org/10.1039/c8cp04561e">10.1039/c8cp04561e</a>'
  apa: 'Cheng, B., Dellago, C., &#38; Ceriotti, M. (2018). Theoretical prediction
    of the homogeneous ice nucleation rate: Disentangling thermodynamics and kinetics.
    <i>Physical Chemistry Chemical Physics</i>. Royal Society of Chemistry. <a href="https://doi.org/10.1039/c8cp04561e">https://doi.org/10.1039/c8cp04561e</a>'
  chicago: 'Cheng, Bingqing, Christoph Dellago, and Michele Ceriotti. “Theoretical
    Prediction of the Homogeneous Ice Nucleation Rate: Disentangling Thermodynamics
    and Kinetics.” <i>Physical Chemistry Chemical Physics</i>. Royal Society of Chemistry,
    2018. <a href="https://doi.org/10.1039/c8cp04561e">https://doi.org/10.1039/c8cp04561e</a>.'
  ieee: 'B. Cheng, C. Dellago, and M. Ceriotti, “Theoretical prediction of the homogeneous
    ice nucleation rate: Disentangling thermodynamics and kinetics,” <i>Physical Chemistry
    Chemical Physics</i>, vol. 20, no. 45. Royal Society of Chemistry, pp. 28732–28740,
    2018.'
  ista: 'Cheng B, Dellago C, Ceriotti M. 2018. Theoretical prediction of the homogeneous
    ice nucleation rate: Disentangling thermodynamics and kinetics. Physical Chemistry
    Chemical Physics. 20(45), 28732–28740.'
  mla: 'Cheng, Bingqing, et al. “Theoretical Prediction of the Homogeneous Ice Nucleation
    Rate: Disentangling Thermodynamics and Kinetics.” <i>Physical Chemistry Chemical
    Physics</i>, vol. 20, no. 45, Royal Society of Chemistry, 2018, pp. 28732–40,
    doi:<a href="https://doi.org/10.1039/c8cp04561e">10.1039/c8cp04561e</a>.'
  short: B. Cheng, C. Dellago, M. Ceriotti, Physical Chemistry Chemical Physics 20
    (2018) 28732–28740.
date_created: 2021-07-15T12:51:44Z
date_published: 2018-12-07T00:00:00Z
date_updated: 2021-08-09T12:36:47Z
day: '07'
doi: 10.1039/c8cp04561e
extern: '1'
external_id:
  arxiv:
  - '1807.05551'
  pmid:
  - '30412211'
intvolume: '        20'
issue: '45'
language:
- iso: eng
main_file_link:
- open_access: '1'
  url: https://arxiv.org/abs/1807.05551
month: '12'
oa: 1
oa_version: Preprint
page: 28732-28740
pmid: 1
publication: Physical Chemistry Chemical Physics
publication_identifier:
  eissn:
  - 1463-9084
  issn:
  - 1463-9076
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Theoretical prediction of the homogeneous ice nucleation rate: Disentangling
  thermodynamics and kinetics'
type: journal_article
user_id: 6785fbc1-c503-11eb-8a32-93094b40e1cf
volume: 20
year: '2018'
...