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Lithium and calcium carbides with polymeric carbon structures.

Daryn Benson1, Yanling Li, Wei Luo

  • 1Department of Physics, Arizona State University, Tempe, Arizona 85287-1504, USA.

Inorganic Chemistry
|May 16, 2013
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Summary

High pressure transforms lithium and calcium carbides into semimetallic and metallic phases with novel polyanionic carbon structures. These new forms exhibit unique electronic properties and potential superconductivity.

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Area of Science:

  • Materials Science
  • Solid State Physics
  • Computational Chemistry

Background:

  • At ambient conditions, lithium carbide (Li2C2) and calcium carbide (CaC2) exist as salt-like acetylides with C2(2-) dumbbell anions.
  • Understanding the high-pressure behavior of these binary carbides is crucial for exploring novel carbon allotropes and their properties.

Purpose of the Study:

  • To investigate the crystal structure and electronic properties of Li2C2 and CaC2 systems under high pressure.
  • To explore the formation of polyanionic carbon structures and their impact on material properties.

Main Methods:

  • Employed an evolutionary and ab initio random structure search methodology for crystal structure prediction.
  • Utilized high-pressure computational simulations to analyze structural and electronic phase transitions.

Main Results:

  • Observed phase transitions to semimetallic (P3m1-Li2C2) and metallic (Cmcm-Li2C2, Cmcm-CaC2, Immm-CaC2) phases below 20 GPa.
  • Identified the formation of polymeric carbon anions (chains, layers, strands) stabilized by cations.
  • The semimetallic P3m1-Li2C2 phase shows electronic structure similarities to graphene, with hybridized Li-sp states affecting the π* band.

Conclusions:

  • High pressure induces significant structural and electronic changes in Li2C2 and CaC2, leading to polyanionic carbon forms.
  • The predicted metallic phases are potential superconductors, with calculated critical temperatures potentially exceeding 10 K.