Abstract

Solids in nature can be generally classified into crystalline and non-crystalline states1-7, depending on whether long-range lattice periodicity is present in the material. The differentiation of the two states, however, could face fundamental challenges if the degree of long-range order in crystals is significantly reduced. Here we report a paracrystalline state of diamond that is distinct from either crystalline or amorphous diamond8-10. The paracrystalline diamond reported in this work, consisting of sub-nanometre-sizedparacrystallites that possess a well-defined crystalline medium-range order up to a few atomic shells4,5,11-13, was synthesized in high-pressure high-temperature conditions (for example, 30 GPa and 1,600 K) employing face-centred cubic C60 as a precursor. The structural characteristics of the paracrystalline diamond were identified through a combination of X-ray diffraction, high-resolution transmission microscopy and advanced molecular dynamics simulation.The formation of paracrystalline diamond is a result of densely distributed nucleation sites developed in compressed C60 as well as pronounced second-nearest-neighbour short-range order in amorphous diamond due to strong sp3 bonding. The discovery of paracrystalline diamond adds an unusual diamond form to the enriched carbon family14-16, which exhibits distinguishing physical properties and can be furthered exploited to develop new materials. Furthermore, this work reveals the missing link in the length scale between amorphous and crystalline states across the structural landscape, having profound implications for recognizing complex structures arising from amorphous materials.

Highlights

  • Version of Record: A version of this preprint was published at Nature on November 24th, 2021

  • Due to decades of research effort, it is understood that structural ordering on the atomic level of amorphous solids is ubiquitous, as manifested by the short-to-medium-range ordering in metallic glasses[5,6,7] and the continuousrandom networks (CRN) of amorphous semiconductors[1,2,3]

  • A crucial question to answer is, in the configurational space, are we able to identify a state of matter that is fully packed with tiny paracrystals possessing only medium range order (MRO) but devoid of long-range order (LRO)? The identification of such a material state is essential to obtaining much-needed structural information differentiating amorphous solids with and without crystalline MRO

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Summary

Introduction

Version of Record: A version of this preprint was published at Nature on November 24th, 2021. Hu Tang Center for High Pressure Science and Technology Advanced Research https://orcid.org/0000-0003-

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