Monatomic-Molecular Transition in Expanded Rubidium

S(Q,ω) for liquid rubidium measured along the liquid vapor coexistence line exhibits monatomic behavior from normal density down to twice the critical density. At this density we observe excitations characteristic of a harmonic oscillator. We interpret this as evidence for the passage of the fluid from a monatomic to a molecular state. First principle total energy calculations for lattices of ribidium at 0 K predict that expansion favors spin pairing and leads to a lattice of dimers with an increase in vibron energy with decreasing density. The excellent agreement of the calculated vibron energy with the experimental result provides theoretical support for the appearance of molecules.