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.

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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. By using time-resolved optical techniques and femtosecond-pulse-excited scanning tunneling microscopy (STM), the evolution of the metastable states in the quasi-two-dimensional dichalcogenide 1T-TaS2 is mapped out on a 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.

Progress in high-performance computing demands significant advances in memory technology. Among novel memory technologies that promise efficient device operation on a sub-ns timescale, resistance switching between charge ordered phases of 1 T-TaS2 has shown to be potentially useful for development of high-speed, energy efficient nonvolatile memory devices. Measurement of the electrical operation of such devices in the picosecond regime is technically challenging and hitherto still largely unexplored. Here, we use an optoelectronic “laboratory-on-a-chip” experiment for measurement of ultrafast memory switching, enabling accurate measurement of electrical switching parameters with 100 fs temporal resolution. Photoexcitation and electro-optic sampling on a (Cd,Mn)Te substrate are used to generate and, subsequently, measure electrical pulse propagation with intra-band excitation and sub-gap probing, respectively. We demonstrate high contrast nonvolatile resistance switching from high to low resistance states of a 1 T-TaS2 device using single sub-2 ps electrical pulses. Using detailed modeling, we find that the switching energy density per unit area is exceptionally small, [Formula: see text] 9.4 fJ/ μm2. The speed and energy efficiency of an electronic “write” process place the 1 T-TaS2 devices into a category of their own among new generation nonvolatile memory devices.

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