Orbital-free density functional theory simulation of collective dynamics coupling in liquid Sn

Abstract

The appearance of a second excitation mode in the longitudinal and transverse collective dynamics of a series of liquid metals has been observed recently, either by inelastic X-ray scattering (IXS) or by first-principles molecular dynamics (FPMD). The phenomenon’s origin is still uncertain, although some theories have been used with relative success to reproduce the FPMD results as a means to find an explanation for it (e.g., mode-coupling (MC) theory in liquid zinc [B. G. del Rio and L. E. González, Phys. Rev. B 95, 224201 (2017)]). For liquid tin (l-Sn), the second excitation mode in the dynamic structure factor and longitudinal current spectrum was observed by IXS [S. Hosokawa et al., J. Phys.: Condens. Matter 25, 112101 (2013)]. By performing orbital-free density functional theory MD simulations of l-Sn, we confirm the existence of a second excitation mode in the longitudinal and transverse collective dynamics and provide a theoretical explanation based on MC theory. Moreover, we introduce a new binary term in MC theory to better capture the negative minima present in the memory functions of the collective dynamics. These results confirm that the origin of the second excitation mode exhibited by the longitudinal and transverse collective dynamics in some liquid metals involves an indirect coupling of the longitudinal and transverse modes.