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Super-expansive thermo-reversible interstitial solid solution of nanocrystal superlattices with mesogens

Nature Materials volume 25, pages 294–301 (2026)Cite this article

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Abstract

Designing superlattices of nanocrystals to mimic and extend the properties of atomic crystals has been a long-standing motivation in materials chemistry. Interstitial solid solutions, such as steel, are well-studied atomic lattices in which mobile components move among the interstices. These materials exhibit unique properties, including reversible structural changes and phase transitions. Interstitial solid solutions possess unique dynamic structures and reversible responses, which motivate the creation of their colloidal equivalents. Here we report a fully thermo-reversible colloidal interstitial solid solution by combining liquid crystals and nanocrystals functionalized with promesogenic ligands. Mesogen molecules fill and diffuse among the interstices of a superlattice, resulting in a super-large thermal expansivity. The approach uses a modular design of interparticle interactions, allowing control of interparticle distance, microstructure and transition between crystallographic forms.

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Fig. 1: Colloidal solid solutions.
Fig. 2: Simulation of interstitial 5CB mesogens in NCSL for inter-NC distance of 11 nm: Au–L2 (top) and Au–L3 (bottom).
Fig. 3: Tailoring NCSL structure and NC–LC interaction by tuning ligands and mesogens.
Fig. 4: Phase transition of NCSL ISSs.

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Data availability

All data and information needed to evaluate the conclusions in the paper are presented in the Article or Supplementary Information. These data are also publicly available via Zenodo at https://doi.org/10.5281/zenodo.16666571 (ref. 56). Source data are provided with this paper.

Code availability

The simulation-related data supporting the findings of this study—including input parameters, model source code, simulation settings and representative output configurations—are publicly available via Zenodo at https://doi.org/10.5281/zenodo.16666571 (ref. 56).

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Acknowledgements

The primary experiments in this work were supported by the National Science Foundation (NSF) STC-IMOD under award DMR2019444 (S.Y., Y.N. and C.B.M.), and partial characterizations were supported by the Office of Naval Research Multidisciplinary University Research Initiative (MURI) award ONR N00014-18-1-2497 (S.Y., Y.N. and C.B.M.). Simulation and modelling were supported by the US Department of Energy (DOE) award DE-SC0019282 (J.G.S.) and John G. Miller Fellowship from the University of Pennsylvania (D.-B.Y.). Ligand synthesis and magnetic measurement were supported by the NSF University of Pennsylvania Materials Research Science and Engineering Center (MRSEC) under award DMR-1720530 (Y.N. and J.M.K.). C.B.M. also acknowledges the Richard Perry University Professorship at the University of Pennsylvania. This research used resources from the Center for Functional Nanomaterials and the CMS beamline (11-BM) and SMI beamline (12-ID) of the National Synchrotron Light Source II, both supported by the DOE Office of Science Facilities at Brookhaven National Laboratory under contract no. DE-SC0012704. We thank R. Li and H. Zhang for the discussions and help at the beamline. This work was carried out in part at the Singh Center for Nanotechnology, which is supported by the NSF National Nanotechnology Coordinated Infrastructure Program under grant NNCI-2025608. Simulations and modelling were performed using allocation TG-CHE110041 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) programme, which is supported by NSF grant nos 1548562, 2138259, 2138286, 2138307, 2137603 and 2138296.

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Author notes

  1. These authors contributed equally: Shengsong Yang, Dai-Bei Yang, Yifan Ning.

Authors and Affiliations

  1. Department of Chemistry, University of Pennsylvania, Philadelphia, PA, USA

    Shengsong Yang, Dai-Bei Yang, Yifan Ning, Jeffery G. Saven & Christopher B. Murray

  2. Center for Functional Nanomaterials, Brookhaven National Laboratories, Upton, NY, USA

    Yugang Zhang

  3. Department of Physics, University of Pennsylvania, Philadelphia, PA, USA

    James M. Kikkawa

  4. Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA, USA

    Christopher B. Murray

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  1. Shengsong Yang
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Contributions

S.Y. and Y.N. performed and designed the experiments, analysed data and co-wrote the paper under supervision from C.B.M.; D.-B.Y. performed simulations, analysed data and co-wrote the paper under supervision from J.G.S.; S.Y., Y.N. and Y.Z. designed and performed beamtime synchrotron studies. S.Y. and J.M.K. performed magnetic measurements. J.G.S. and C.B.M. supervised the project, analysed data, co-wrote the paper and acquired the funding. All authors discussed the results and commented on the manuscript.

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Correspondence to Jeffery G. Saven or Christopher B. Murray.

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Nature Materials thanks Jan Lagerwall, Monica Olvera de la Cruz, Alex Travesset and Asaph Widmer-Cooper for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information (download PDF )

Supplementary Schemes 1 and 2, Figs. 1–50, Table 1, captions for Videos 1–5, text and references.

Supplementary Video 1 (download MP4 )

Coarse-grained simulation of mesogens gradually penetrating the trilayer of NCSL.

Supplementary Video 2 (download MP4 )

In situ SAXS experiment of Au–L2 in 5CB system under heating and cooling cycles.

Supplementary Video 3 (download MP4 )

In situ SAXS experiment of Au–L3 in 5CB system under heating and cooling cycles.

Supplementary Video 4 (download MP4 )

Coarse-grained simulation of mesogens diffusing among the interstices of NCSL, with one mesogen emphasized in white.

Supplementary Video 5 (download MP4 )

In situ SAXS experiment of Fe3O4–L2 in 7CB system under heating and cooling cycles with reversible FCC to BCT Martensitic transition.

Source data

Source Data Fig. 1 (download XLSX )

Statistical source data for Fig. 1c,e,f.

Source Data Fig. 4 (download XLSX )

Statistical source data for Fig. 4b,c.

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Yang, S., Yang, DB., Ning, Y. et al. Super-expansive thermo-reversible interstitial solid solution of nanocrystal superlattices with mesogens. Nat. Mater. 25, 294–301 (2026). https://doi.org/10.1038/s41563-025-02388-3

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