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@ARTICLE{Dammann:623689,
author = {Dammann, Lars and Kohns, Richard and Huber, Patrick and
Meißner, Robert H.},
title = {{M}aximum {E}ntropy-{M}ediated {L}iquid-to-{S}olid
{N}ucleation and {T}ransition},
journal = {Journal of chemical theory and computation},
volume = {21},
number = {4},
issn = {1549-9618},
address = {Washington, DC},
publisher = {[Verlag nicht ermittelbar]},
reportid = {PUBDB-2025-00736},
pages = {1997 – 2011},
year = {2025},
abstract = {Molecular dynamics (MD) simulations are a powerful tool for
studying matter at the atomic scale. However, to simulate
solids, an initial atomic structure is crucial for the
successful execution of MD simulations but can be difficult
to prepare due to insufficient atomistic information. At the
same time, wide-angle X-ray scattering (WAXS) measurements
can determine the radial distribution function (RDF) of
atomic structures. However, the interpretation of RDFs is
often challenging. Here, we present an algorithm that can
bias MD simulations with RDFs by combining the information
on the MD atomic interaction potential and the RDF under the
principle of maximum relative entropy. We show that this
algorithm can be used to adjust the RDF of one liquid model,
e.g., the TIP3P water model, to reproduce the RDF and
improve the angular distribution function (ADF) of another
model, such as the TIP4P/2005 water model. In addition, we
demonstrate that the algorithm can initiate crystallization
in liquid systems, leading to both stable and metastable
crystalline states defined by the RDF, e.g., crystallization
of water to ice and liquid TiO2 to rutile or anatase.
Finally, we discuss how this method can be useful for
improving interaction models, studying crystallization
processes, interpreting measured RDFs, or training
machine-learned potentials.},
cin = {CIMMS},
ddc = {610},
cid = {I:(DE-H253)CIMMS-20211022},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / HIDSS-0002 - DASHH: Data Science in
Hamburg - Helmholtz Graduate School for the Structure of
Matter $(2019_IVF-HIDSS-0002)$ / GRK 2462 - GRK 2462:
Prozesse in natürlichen und technischen
Partikel-Fluid-Systemen (PintPFS) (390794421) / DFG project
G:(GEPRIS)192346071 - SFB 986: Maßgeschneiderte
Multiskalige Materialsysteme - M3 (192346071)},
pid = {G:(DE-HGF)POF4-632 / $G:(DE-HGF)2019_IVF-HIDSS-0002$ /
G:(GEPRIS)390794421 / G:(GEPRIS)192346071},
experiment = {EXP:(DE-MLZ)NOSPEC-20140101},
typ = {PUB:(DE-HGF)16},
pubmed = {39937968},
UT = {WOS:001419568600001},
doi = {10.1021/acs.jctc.4c01621},
url = {https://bib-pubdb1.desy.de/record/623689},
}