article published yes Michael Wassermair author 23d132c4-4e98-11ef-b275-9e8d4cd8c9170009-0003-6339-4051 Gerhard Kahl author Roland Roth author Andrew J. Archer author GradSch department We investigate the phase ordering (pattern formation) of systems of two-dimensional core–shell particles using Monte Carlo (MC) computer simulations and classical density functional theory (DFT). The particles interact via a pair potential having a hard core and a repulsive square shoulder. Our simulations show that on cooling, the liquid state structure becomes increasingly characterized by long wavelength density modulations and on further cooling forms a variety of other phases, including clustered, striped, and other patterned phases. In DFT, the hard core part of the potential is treated using either fundamental measure theory or a simple local density approximation, whereas the soft shoulder is treated using the random phase approximation. The different DFTs are benchmarked using large-scale grand-canonical-MC and Gibbs-ensemble-MC simulations, demonstrating their predictive capabilities and shortcomings. We find that having the liquid state static structure factor S(k) for wavenumber k is sufficient to identify the Fourier modes governing both the liquid and solid phases. This allows us to identify from easier-to-obtain liquid state data the wavenumbers relevant to the periodic phases and to predict roughly where in the phase diagram these patterned phases arise. https://research-explorer.ista.ac.at/download/18174/18185/2024_JourChemicalPhysics_Wassermair.pdf application/pdfno AIP Publishing2024 eng 1089-7690 2409.06447 39344889 00132526830000410.1063/5.0226954 16112 Wassermair, Michael, Gerhard Kahl, Roland Roth, and Andrew J. Archer. “Fingerprints of Ordered Self-Assembled Structures in the Liquid Phase of a Hard-Core, Square-Shoulder System.” <i>The Journal of Chemical Physics</i>. AIP Publishing, 2024. <a href="https://doi.org/10.1063/5.0226954">https://doi.org/10.1063/5.0226954</a>. Wassermair, Michael, et al. “Fingerprints of Ordered Self-Assembled Structures in the Liquid Phase of a Hard-Core, Square-Shoulder System.” <i>The Journal of Chemical Physics</i>, vol. 161, no. 12, 124503, AIP Publishing, 2024, doi:<a href="https://doi.org/10.1063/5.0226954">10.1063/5.0226954</a>. Wassermair M, Kahl G, Roth R, Archer AJ. Fingerprints of ordered self-assembled structures in the liquid phase of a hard-core, square-shoulder system. <i>The Journal of chemical physics</i>. 2024;161(12). doi:<a href="https://doi.org/10.1063/5.0226954">10.1063/5.0226954</a> M. Wassermair, G. Kahl, R. Roth, A.J. Archer, The Journal of Chemical Physics 161 (2024). Wassermair M, Kahl G, Roth R, Archer AJ. 2024. Fingerprints of ordered self-assembled structures in the liquid phase of a hard-core, square-shoulder system. The Journal of chemical physics. 161(12), 124503. M. Wassermair, G. Kahl, R. Roth, and A. J. Archer, “Fingerprints of ordered self-assembled structures in the liquid phase of a hard-core, square-shoulder system,” <i>The Journal of chemical physics</i>, vol. 161, no. 12. AIP Publishing, 2024. Wassermair, M., Kahl, G., Roth, R., &#38; Archer, A. J. (2024). Fingerprints of ordered self-assembled structures in the liquid phase of a hard-core, square-shoulder system. <i>The Journal of Chemical Physics</i>. AIP Publishing. <a href="https://doi.org/10.1063/5.0226954">https://doi.org/10.1063/5.0226954</a> 181742024-10-06T22:01:12Z2026-10-02T11:10:03Z