Graphite intercalation compounds under pressure: A first-principles density functional theory study

Abstract

Motivated by recent experimental work, we use first-principles density functional theory methods to conduct an extensive search for low enthalpy structures of ${\mathrm{C}}_{6}\mathrm{Ca}$ under pressure. As well as a range of buckled structures, which are energetically competitive over an intermediate range of pressures, we show that the high-pressure system $(\ensuremath{\gtrsim}18\phantom{\rule{0.3em}{0ex}}\mathrm{GPa})$ is unstable toward the formation of a class of layered structures, with the most stable compound involving carbon sheets containing five- and eight-membered rings. As well as discussing the energetics of the different classes of low enthalpy structures, we comment on the electronic structure of the high-pressure compound and its implications for superconductivity.