A few-layer covalent network of fullerenes

Elena Meirzadeh¹, Austin M Evans^{2

3}, Mehdi Rezaee⁴, Milena Milich⁵, Connor J Dionne⁶, Thomas P Darlington⁷, Si Tong Bao², Amymarie K Bartholomew², Taketo Handa², Daniel J Rizzo⁸, Ren A Wiscons⁹, Mahniz Reza¹⁰, Amirali Zangiabadi¹¹, Natalie Fardian-Melamed⁷, Andrew C Crowther¹⁰, P James Schuck⁷, D N Basov⁸, Xiaoyang Zhu², Ashutosh Giri⁶, Patrick E Hopkins^{5

12

13}, Philip Kim¹⁴, Michael L Steigerwald¹⁵, Jingjing Yang¹⁶, Colin Nuckolls¹⁷, Xavier Roy¹⁸

Affiliations

¹ Department of Chemistry, Columbia University, New York, NY, USA. em3428@columbia.edu.
² Department of Chemistry, Columbia University, New York, NY, USA.
³ George and Josephine Butler Polymer Research Laboratory, Center for Macromolecular Science and Engineering, Department of Chemistry, University of Florida, Gainesville, FL, USA.
⁴ School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
⁵ Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA, USA.
⁶ Department of Mechanical, Industrial and Systems Engineering, University of Rhode Island, Kingston, RI, USA.
⁷ Department of Mechanical Engineering, Columbia University, New York, NY, USA.
⁸ Department of Physics, Columbia University, New York, NY, USA.
⁹ Department of Chemistry, Amherst College, Amherst, MA, USA.
¹⁰ Department of Chemistry, Barnard College, New York, NY, USA.
¹¹ Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY, USA.
¹² Department of Materials Science and Engineering, University of Virginia, Charlottesville, VA, USA.
¹³ Department of Physics, University of Virginia, Charlottesville, VA, USA.
¹⁴ Department of Physics, Harvard University, Cambridge, MA, USA.
¹⁵ Department of Chemistry, Columbia University, New York, NY, USA. mls2064@columbia.edu.
¹⁶ Department of Chemistry, Columbia University, New York, NY, USA. yjj0412@berkeley.edu.
¹⁷ Department of Chemistry, Columbia University, New York, NY, USA. cn37@columbia.edu.
¹⁸ Department of Chemistry, Columbia University, New York, NY, USA. xr2114@columbia.edu.

PMID: 36600065
DOI: 10.1038/s41586-022-05401-w

A few-layer covalent network of fullerenes

Elena Meirzadeh et al. Nature. 2023 Jan.

. 2023 Jan;613(7942):71-76.

doi: 10.1038/s41586-022-05401-w. Epub 2023 Jan 4.

Authors

Affiliations

¹ Department of Chemistry, Columbia University, New York, NY, USA. em3428@columbia.edu.
² Department of Chemistry, Columbia University, New York, NY, USA.
³ George and Josephine Butler Polymer Research Laboratory, Center for Macromolecular Science and Engineering, Department of Chemistry, University of Florida, Gainesville, FL, USA.
⁴ School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
⁵ Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA, USA.
⁶ Department of Mechanical, Industrial and Systems Engineering, University of Rhode Island, Kingston, RI, USA.
⁷ Department of Mechanical Engineering, Columbia University, New York, NY, USA.
⁸ Department of Physics, Columbia University, New York, NY, USA.
⁹ Department of Chemistry, Amherst College, Amherst, MA, USA.
¹⁰ Department of Chemistry, Barnard College, New York, NY, USA.
¹¹ Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY, USA.
¹² Department of Materials Science and Engineering, University of Virginia, Charlottesville, VA, USA.
¹³ Department of Physics, University of Virginia, Charlottesville, VA, USA.
¹⁴ Department of Physics, Harvard University, Cambridge, MA, USA.
¹⁵ Department of Chemistry, Columbia University, New York, NY, USA. mls2064@columbia.edu.
¹⁶ Department of Chemistry, Columbia University, New York, NY, USA. yjj0412@berkeley.edu.
¹⁷ Department of Chemistry, Columbia University, New York, NY, USA. cn37@columbia.edu.
¹⁸ Department of Chemistry, Columbia University, New York, NY, USA. xr2114@columbia.edu.

PMID: 36600065
DOI: 10.1038/s41586-022-05401-w

Abstract

The two natural allotropes of carbon, diamond and graphite, are extended networks of sp³-hybridized and sp²-hybridized atoms, respectively¹. By mixing different hybridizations and geometries of carbon, one could conceptually construct countless synthetic allotropes. Here we introduce graphullerene, a two-dimensional crystalline polymer of C₆₀ that bridges the gulf between molecular and extended carbon materials. Its constituent fullerene subunits arrange hexagonally in a covalently interconnected molecular sheet. We report charge-neutral, purely carbon-based macroscopic crystals that are large enough to be mechanically exfoliated to produce molecularly thin flakes with clean interfaces-a critical requirement for the creation of heterostructures and optoelectronic devices². The synthesis entails growing single crystals of layered polymeric (Mg₄C₆₀)_∞ by chemical vapour transport and subsequently removing the magnesium with dilute acid. We explore the thermal conductivity of this material and find it to be much higher than that of molecular C₆₀, which is a consequence of the in-plane covalent bonding. Furthermore, imaging few-layer graphullerene flakes using transmission electron microscopy and near-field nano-photoluminescence spectroscopy reveals the existence of moiré-like superlattices³. More broadly, the synthesis of extended carbon structures by polymerization of molecular precursors charts a clear path to the systematic design of materials for the construction of two-dimensional heterostructures with tunable optoelectronic properties.

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References

1. Hirsch, A. The era of carbon allotropes. Nat. Mater. 9, 868–871 (2010). - DOI
1. Liu, X. & Hersam, M. C. Interface characterization and control of 2D materials and heterostructures. Adv. Mater. 30, 1801586 (2018). - DOI
1. Andrei, E. Y. et al. The marvels of moiré materials. Nat. Rev. Mater. 6, 201–206 (2021). - DOI
1. Kroto, H. W., Heath, J. R., O’Brien, S. C., Curl, R. F. & Smalley, R. E. C₆₀: buckminsterfullerene. Nature 318, 162–163 (1985). - DOI
1. David, W. I. F. et al. Crystal structure and bonding of ordered C₆₀. Nature 353, 147–149 (1991). - DOI

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A few-layer covalent network of fullerenes

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A few-layer covalent network of fullerenes

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