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A nontrivial balance between Coulomb repulsion and kinematic effects determines the electronic structure of correlated electron materials. The use of electromagnetic fields strong enough to rival these native microscopic interactions allows us to study the electronic response as well as the time scales and energies involved in using quantum effects for possible applications. We use element-specific transient x-ray absorption spectroscopy and high-harmonic generation to measure the response to ultrashort off-resonant optical fields in the prototypical correlated electron insulator NiO. Surprisingly, fields of up to 0.22 V/Å lead to no detectable changes in the correlated Ni 3d orbitals contrary to previous predictions. A transient directional charge transfer is uncovered, a behavior that is captured by first-principles theory. Our results highlight the importance of retardation effects in electronic screening and pinpoints a key challenge in functionalizing correlated materials for ultrafast device operation.

The control of a material's state via external stimuli is the basis of modern information storage technology. Here, the authors use pulsed currents to induce fast switching between Mott insulator and metallic states in the charge density wave system 1T-TaS2, presenting an all-electronic storage mechanism.

The spinel-structure CuIr _2 S _4 compound displays a rather unusual orbitally-driven three-dimensional Peierls-like insulator–metal transition. The low- T symmetry-broken insulating state is especially interesting due to the existence of a metastable irradiation-induced disordered weakly conducting state. Here we study intense femtosecond optical pulse irradiation effects by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. We show that the structural coherence of the low- T broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the low- T disordered weakly conducting state. The electronic order shows a transient gap filling at a significantly lower fluence threshold. The data suggest that the photoinduced-transition dynamics to the high- T metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete ultrafast structural transition even when the absorbed energy significantly exceeds the equilibrium enthalpy difference to the high- T metallic phase.

Light-matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe., Competing Interests: The authors have no conflicts to disclose., (© 2024 Author(s).)

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-TaS 2 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., (© 2023. The Author(s).)

Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s-2p core-valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p-3d resonance (L 2 -edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 ± 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap.

Current trends in data processing have given impetus for an intense search of new concepts of memory devices with emphasis on efficiency, speed, and scalability. A promising new approach to memory storage is based on resistance switching between charge-ordered domain states in the layered dichalcogenide 1T-TaS 2 . Here we investigate the energy efficiency scaling of such charge configuration memory (CCM) devices as a function of device size and data write time τ W as well as other parameters that have bearing on efficient device operation. We find that switching energy efficiency scales approximately linearly with both quantities over multiple decades, departing from linearity only when τ W approaches the ∼0.5 ps intrinsic switching limit. Compared to current state of the art memory devices, CCM devices are found to be much faster and significantly more energy efficient, demonstrated here with two-terminal switching using 2.2 fJ, 16 ps electrical pulses.

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.

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-TaS 2 . We map out its temporal phase diagram using the photon density and temperature as control parameters on timescales ranging from 10 -12 to 10 3 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.

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.

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 TaS 2 created in situ on the surface of an orthorhombic 1T-TaS 2 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., Competing Interests: The authors declare no competing financial interest.

Recent demonstrations of controlled switching between different ordered macroscopic states by impulsive electromagnetic perturbations in complex materials have opened some fundamental questions on the mechanisms responsible for such remarkable behavior. Here we experimentally address the question of whether two-dimensional (2D) Mott physics can be responsible for unusual switching between states of different electronic order in the layered dichalcogenide 1T-TaS 2 , or it is a result of subtle inter-layer "orbitronic" re-ordering of its stacking structure. We report on in-plane (IP) and out-of-plane (OP) resistance switching by current-pulse injection at low temperatures. Elucidating the controversial theoretical predictions, we also report on measurements of the anisotropy of the electrical resistivity below room temperature. From the T-dependence of ρ ⊥ and ρ || , we surmise that the resistivity is more consistent with collective motion than single particle diffusive or band-like transport. The relaxation dynamics of the metastable state for both IP and OP electron transport are seemingly governed by the same mesoscopic quantum re-ordering process. We conclude that 1T-TaS 2 shows resistance switching arising from an interplay of both IP and OP correlations.

Controllable switching between metastable macroscopic quantum states under nonequilibrium conditions induced either by light or with an external electric field is rapidly becoming of great fundamental interest. We investigate the relaxation properties of a "hidden" (H) charge density wave (CDW) state in thin single crystals of the layered dichalcogenide 1T-TaS2, which can be reached by either a single 35-fs optical laser pulse or an ~30-ps electrical pulse. From measurements of the temperature dependence of the resistivity under different excitation conditions, we find that the metallic H state relaxes to the insulating Mott ground state through a sequence of intermediate metastable states via discrete jumps over a "Devil's staircase." In between the discrete steps, an underlying glassy relaxation process is observed, which arises because of reciprocal-space commensurability frustration between the CDW and the underlying lattice. We show that the metastable state relaxation rate may be externally stabilized by substrate strain, thus opening the way to the design of nonvolatile ultrafast high-temperature memory devices based on switching between CDW states with large intrinsic differences in electrical resistance.

Construction and characterization of a multichannel photodiode detector based on commercially available components with high signal to noise of ∼10(6) and a rapid frame rate, suitable for time resolved femtosecond spectroscopy with high repetition femtosecond sources, is presented.

Hidden states of matter may be created if a system out of equilibrium follows a trajectory to a state that is inaccessible or does not exist under normal equilibrium conditions. We found such a hidden (H) electronic state in a layered dichalcogenide crystal of 1T-TaS2 (the trigonal phase of tantalum disulfide) reached as a result of a quench caused by a single 35-femtosecond laser pulse. In comparison to other states of the system, the H state exhibits a large drop of electrical resistance, strongly modified single-particle and collective-mode spectra, and a marked change of optical reflectivity. The H state is stable until a laser pulse, electrical current, or thermal erase procedure is applied, causing it to revert to the thermodynamic ground state.