Quantum jamming transition to a correlated electron glass in 1T-TaS2.

Distinct many-body states may be created under non-equilibrium conditions through different ordering paths, even when their constituents are subjected to the same fundamental interactions. The phase-transition mechanism to such states remains poorly understood. Here, we show that controlled optical or electromagnetic perturbations can lead to an amorphous metastable state of strongly correlated electrons in a quasi-two-dimensional dichalcogenide. Scanning tunnelling microscopy reveals a hyperuniform pattern of localized charges, whereas multitip surface nanoscale conductivity measurements and tunnelling spectroscopy show an electronically gapless conducting state that is different from conventional Coulomb glasses and many-body localized systems. The state is stable up to room temperature and shows no signs of either local charge order or phase separation. The mechanism for its formation is attributed to a dynamical localization of electrons through mutual interactions. Theoretical calculations confirm the correlations between localized charges to be crucial for the state's unusual stability.

Mottness collapse without metallization in the domain wall of the triangular-lattice Mott insulator 1T-TaS_{2}.

1T-TaS_{2} is a charge-density-wave (CDW) compound with a Mott-insulating ground state. The metallic state obtained by doping, substitution, or pulsed charge injection is characterized by an emergent CDW domain-wall network, while single domain walls can be found in the pristine Mott state. Here we study whether and how the single walls become metallic. Tunneling spectroscopy reveals partial suppression of the Mott gap and the presence of in-gap states strongly localized at the domain-wall sites. Using the real-space dynamical mean field theory description of the strongly correlated quantum-paramagnet ground state, we show that the local gap suppression follows from the increased hopping along the connected zigzag chain of lattice sites forming the domain wall. Furthermore, we show that full metallization is preempted by the splitting of the quasiparticle band into bonding and antibonding subbands due to the structural dimerization of the wall, explaining the presence of the in-gap states and the low density of states at the Fermi level.

Non-equilibrium quantum domain reconfiguration dynamics in a two-dimensional electronic crystal and a quantum annealer.

Relaxation dynamics of complex many-body quantum systems trapped into metastable states is a very active field of research from both the theoretical and experimental point of view with implications in a wide array of topics from macroscopic quantum tunnelling and nucleosynthesis to non-equilibrium superconductivity and energy-efficient memory devices. In this work, we investigate quantum domain reconfiguration dynamics in the electronic superlattice of a quantum material using time-resolved scanning tunneling microscopy and unveil a crossover from temperature to noisy quantum fluctuation dominated dynamics. The process is modeled using a programmable superconducting quantum annealer in which qubit interconnections correspond directly to the microscopic interactions between electrons in the quantum material. Crucially, the dynamics of both the experiment and quantum simulation is driven by spectrally similar pink noise. We find that the simulations reproduce the emergent time evolution and temperature dependence of the experimentally observed electronic domain dynamics.

Manipulation of fractionalized charge in the metastable topologically entangled state of a doped Wigner crystal.

Metastability of many-body quantum states is rare and still poorly understood. An exceptional example is the low-temperature metallic state of the layered dichalcogenide 1T-TaS2 in which electronic order is frozen after external excitation. Here we visualize the microscopic dynamics of injected charges in the metastable state using a multiple-tip scanning tunnelling microscope. We observe non-thermal formation of a metastable network of dislocations interconnected by domain walls, that leads to macroscopic robustness of the state to external thermal perturbations, such as small applied currents. With higher currents, we observe annihilation of dislocations following topological rules, accompanied with a change of macroscopic electrical resistance. Modelling carrier injection into a Wigner crystal reveals the origin of formation of fractionalized, topologically entangled networks, which defines the spatial fabric through which single particle excitations propagate. The possibility of manipulating topological entanglement of such networks suggests the way forward in the search for elusive metastable states in quantum many body systems.

Coherent light control of a metastable hidden state.

Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.

Quantum billiards with correlated electrons confined in triangular transition metal dichalcogenide monolayer nanostructures.

Forcing systems through fast non-equilibrium phase transitions offers the opportunity to study new states of quantum matter that self-assemble in their wake. Here we study the quantum interference effects of correlated electrons confined in monolayer quantum nanostructures, created by femtosecond laser-induced quench through a first-order polytype structural transition in a layered transition-metal dichalcogenide material. Scanning tunnelling microscopy of the electrons confined within equilateral triangles, whose dimensions are a few crystal unit cells on the side, reveals that the trajectories are strongly modified from free-electron states both by electronic correlations and confinement. Comparison of experiments with theoretical predictions of strongly correlated electron behaviour reveals that the confining geometry destabilizes the Wigner/Mott crystal ground state, resulting in mixed itinerant and correlation-localized states intertwined on a length scale of 1 nm. The work opens the path toward understanding the quantum transport of electrons confined in atomic-scale monolayer structures based on correlated-electron-materials.

A time-domain phase diagram of metastable states in a charge ordered quantum material.

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.

Strain-Induced Metastable Topological Networks in Laser-Fabricated TaS2 Polytype Heterostructures for Nanoscale Devices.

The stacking of layered materials into heterostructures offers diverse possibilities for generating deformed moiré states arising from their mutual interaction. Here we report self-assembled two-dimensional nanoscale strain networks formed within a single prismatic (H) polytype monolayer of TaS2 created in situ on the surface of an orthorhombic 1T-TaS2 single crystal by a low-temperature laser-induced polytype transformation. The networks revealed by scanning tunneling microscopy (STM) take on diverse configurations at different temperatures, including extensive double stripes and a twisted 3-gonal mesh of connected 6-pronged vertices. The resulting phase diagram can be understood to be a consequence of thermally driven minimization of discommensurations between the H and 1T layers. Nontrivial dislocation defects of embedded 2- and 4-gonal structures are shown to be associated with local inhomogeneous strains. The creation of metastable heterostructures by laser quench at cryogenic temperatures in combination with STM manipulation of local strain demonstrates nanoscale control of topological defects in transition metal dichalcogenide heterostructures may be utilized in the fabrication of nanoscale electronic devices and neural networks.