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Negative and Positive Anisotropic Thermal Expansion in 2D Fullerene Networks

Armaan Shaikh1,2, Jiaqi Wu3, and Bo Peng4,*

  • *Contact author: bp432@cam.ac.uk
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Phys. Rev. Lett. 135, 126103 – Published 18 September, 2025

DOI: https://doi.org/10.1103/tck2-78dx

Abstract

We find a design principle for tailoring thermal expansion properties in nearly spherical molecular networks. Using 2D fullerene networks as a representative system, we realize positive thermal expansion along intermolecular [2+2] cycloaddition bonds and negative thermal expansion along intermolecular C-C single bonds by varying the structural frameworks of molecules. The microscopic mechanism originates from a combination of the framework’s geometric flexibility and its transverse vibrational characteristics. Based on this insight, we find molecular networks beyond C60 with tunable thermal expansion. These findings shed light on the fundamental mechanisms governing thermal expansion in molecular networks towards rational materials design.

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Phys. Rev. Lett. 135, 126103– Published 18 September, 2025
  • Received 2 April 2025
  • Revised 13 July 2025
  • Accepted 28 August 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

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