No abstract

Mesoscopic irregularly ordered and even amorphous self-assembled electronic structures were recently reported in two-dimensional metallic dichalcogenides (TMDs), created and manipulated with short light pulses or by charge injection. Apart from promising new all-electronic memory devices, such states are of great fundamental importance, since such aperiodic states cannot be described in terms of conventional charge-density-wave (CDW) physics. In this paper, we address the problem of metastable mesoscopic configurational charge ordering in TMDs with a sparsely filled charged lattice gas model in which electrons are subject only to screened Coulomb repulsion. The model correctly predicts commensurate CDW states corresponding to different TMDs at magic filling fractions = / / / / / f 1 3, 1 4, 1 9, 1 13, 1 16.mDoping away from f m results either in multiple neardegenerate configurational states, or an amorphous state at the correct density observed by scanning tunnelling microscopy. Quantum fluctuations between degenerate states predict a quantum charge liquid at low temperatures, revealing a new generalized viewpoint on both regular, irregular and amorphous charge ordering in transition metal dichalcogenides.

Metastable self-organized electronic states in quantum materials are of fundamental importance, displaying emergent dynamical properties that may be used in new generations of sensors and memory devices. Such states are typically formed through phase transitions under non-equilibrium conditions and the final state is reached through processes that span a large range of timescales. Conventionally, phase diagrams of materials are thought of as static, without temporal evolution. However, many functional properties of materials arise as a result of complex temporal changes in the material occurring on different timescales. Hitherto, such properties were not considered within the context of a temporally-evolving phase diagram, even though, under non-equilibrium conditions, different phases typically evolve on different timescales. Here, by using time-resolved optical techniques and femtosecond-pulse-excited scanning tunneling microscopy (STM), we track the evolution of the metastable states in a material that has been of wide recent interest, the quasi-two-dimensional dichalcogenide 1T-TaS2. We map out its temporal phase diagram using the photon density and temperature as control parameters on timescales ranging from 10−12 to 103 s. The introduction of a time-domain axis in the phase diagram enables us to follow the evolution of metastable emergent states created by different phase transition mechanisms on different timescales, thus enabling comparison with theoretical predictions of the phase diagram, and opening the way to understanding of the complex ordering processes in metastable materials.