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Solid-liquid phase transitions are fundamental physical processes, butatomically-resolved microscopy has yet to capture both the solid and liquiddynamics for such a transition. We have developed a new technique forcontrolling the melting and freezing of 2D molecular layers on a graphenefield-effect transistor (FET) that allows us to image phase transition dynamicsvia atomically-resolved scanning tunneling microscopy. Back-gate voltagesapplied to a F4TCNQ-decorated graphene FET induce reversible transitionsbetween a charge-neutral solid phase and a negatively charged liquid phase.Nonequilibrium molecular melting dynamics are visualized by rapidly heating thegraphene surface with electrical current and imaging the resulting evolutiontoward new equilibrium states. An analytical model has been developed thatexplains the observed equilibrium mixed-state phases based on spectroscopicmeasurement of both solid and liquid molecular energy levels. Observednon-equilibrium melting dynamics are consistent with Monte Carlo simulations.

Imaging gate-induced molecular melting on a graphene field-effect transistor