Search for: All records

Abstract Solid–liquid phase transitions are basic physical processes, but atomically resolved microscopy has yet to capture their full dynamics. A new technique is developed for controlling the melting and freezing of self‐assembled molecular structures on a graphene field‐effect transistor (FET) that allows phase‐transition behavior to be imaged using atomically resolved scanning tunneling microscopy. This is achieved by applying electric fields to 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane‐decorated FETs to induce reversible transitions between molecular solid and liquid phases at the FET surface. Nonequilibrium melting dynamics are visualized by rapidly heating the graphene substrate with an electrical current and imaging the resulting evolution toward new 2D equilibrium states. An analytical model is developed that explains observed mixed‐state phases based on spectroscopic measurement of solid and liquid molecular energy levels. The observed nonequilibrium melting dynamics are consistent with Monte Carlo simulations. 

Abstract When a three-dimensional material is constructed by stacking different two-dimensional layers into an ordered structure, new and unique physical properties can emerge. An example is the delafossite PdCoO 2 , which consists of alternating layers of metallic Pd and Mott-insulating CoO 2 sheets. To understand the nature of the electronic coupling between the layers that gives rise to the unique properties of PdCoO 2 , we revealed its layer-resolved electronic structure combining standing-wave X-ray photoemission spectroscopy and ab initio many-body calculations. Experimentally, we have decomposed the measured VB spectrum into contributions from Pd and CoO 2 layers. Computationally, we find that many-body interactions in Pd and CoO 2 layers are highly different. Holes in the CoO 2 layer interact strongly with charge-transfer excitons in the same layer, whereas holes in the Pd layer couple to plasmons in the Pd layer. Interestingly, we find that holes in states hybridized across both layers couple to both types of excitations (charge-transfer excitons or plasmons), with the intensity of photoemission satellites being proportional to the projection of the state onto a given layer. This establishes satellites as a sensitive probe for inter-layer hybridization. These findings pave the way towards a better understanding of complex many-electron interactions in layered quantum materials.