Density-wave instability in α-(BEDT-TTF)2KHg(SCN)4 studied by x-ray diffuse scattering and by first-principles calculations

alpha-(BEDT-TTF)(2)KHg(SCN)(4) develops a density wave ground state below 8 K whose origin is still debated. Here we report a combined x-ray diffuse scattering and first-principles density functional theory study supporting the charge density wave (CDW) scenario. In particular, we observe a triply incommensurate anharmonic lattice modulation with intralayer wave vector components which coincide within experimental errors to the maximum of the calculated Lindhard response function. A detailed study of the structural aspects of the modulation shows that the CDW instability in alpha-(BEDT-TTF)(2)KHg(SCN)(4) is considerably more involved than those following a standard Peierls mechanism. We thus propose a microscopic mechanism where the CDW instability of the BEDT- TTF layer is triggered by the anion sublattice. Our mechanism also emphasizes the key role of the coupling of the BEDT- TTF and anion layers via the hydrogen bond network to set the global modulation.