Nanoscale Imaging and Control of Volatile and Non-Volatile Resistive Switching in VO2.

Control of the metal-insulator phase transition is vital for emerging neuromorphic and memristive technologies. The ability to alter the electrically driven transition between volatile and non-volatile states is particularly important for quantum-materials-based emulation of neurons and synapses. The major challenge of this implementation is to understand and control the nanoscale mechanisms behind these two fundamental switching modalities. Here, in situ X-ray nanoimaging is used to follow the evolution of the nanostructure and disorder in the archetypal Mott insulator VO2 during an electrically driven transition. Our findings demonstrate selective and reversible stabilization of either the insulating or metallic phases achieved by manipulating the defect concentration. This mechanism enables us to alter the local switching response between volatile and persistent regimes and demonstrates a new possibility for nanoscale control of the resistive switching in Mott materials.

Extracting contrast in an X-ray speckle visibility spectroscopy experiment under imperfect conditions.

Pump-probe experiments at synchrotrons and free-electron lasers to study ultrafast dynamics in materials far from equilibrium have been well established, but techniques to investigate equilibrium dynamics on the nano- and pico-second timescales remain underdeveloped and experimentally challenging. A promising approach relies on a double-probe X-ray speckle visibility spectroscopy setup at split-and-delay beamlines of X-ray free-electron lasers. However, the logistics in consistently producing two collinear, perfectly overlapping pulses necessary to conduct a faithful experiment is difficult to achieve. In this paper, a method is introduced to extract contrast in the case where an angular misalignment and imperfect overlap exists between the two pulses. Numerical simulations of a dynamical system show that contrast can still be extracted for significant angular misalignments accompanied by partial overlap between the two pulses.

Perovskite neural trees.

Trees are used by animals, humans and machines to classify information and make decisions. Natural tree structures displayed by synapses of the brain involves potentiation and depression capable of branching and is essential for survival and learning. Demonstration of such features in synthetic matter is challenging due to the need to host a complex energy landscape capable of learning, memory and electrical interrogation. We report experimental realization of tree-like conductance states at room temperature in strongly correlated perovskite nickelates by modulating proton distribution under high speed electric pulses. This demonstration represents physical realization of ultrametric trees, a concept from number theory applied to the study of spin glasses in physics that inspired early neural network theory dating almost forty years ago. We apply the tree-like memory features in spiking neural networks to demonstrate high fidelity object recognition, and in future can open new directions for neuromorphic computing and artificial intelligence.

Orbital Domain Dynamics in Magnetite below the Verwey Transition.

The metal-insulator phase transition in magnetite, known as the Verwey transition, is characterized by a charge-orbital ordering and a lattice transformation from a cubic to monoclinic structure. We use x-ray photon correlation spectroscopy to investigate the dynamics of this charge-orbitally ordered insulating phase undergoing the insulator-to-metal transition. By tuning to the Fe L_{3} edge at the (001/2) superlattice peak, we probe the evolution of the Fe t_{2g} orbitally ordered domains present in the low temperature insulating phase and forbidden in the high temperature metallic phase. We observe two distinct regimes below the Verwey transition. In the first regime, magnetite follows an Arrhenius behavior and the characteristic timescale for orbital fluctuations decreases as the temperature increases. In the second regime, magnetite phase separates into metallic and insulating domains, and the kinetics of the phase transition is dictated by metallic-insulating interfacial boundary conditions.

Nonequilibrium Phase Precursors during a Photoexcited Insulator-to-Metal Transition in V_{2}O_{3}.

Here, we photoinduce and directly observe with x-ray scattering an ultrafast enhancement of the structural long-range order in the archetypal Mott system V_{2}O_{3}. Despite the ultrafast increase in crystal symmetry, the change of unit cell volume occurs an order of magnitude slower and coincides with the insulator-to-metal transition. The decoupling between the two structural responses in the time domain highlights the existence of a transient photoinduced precursor phase, which is distinct from the two structural phases present in equilibrium. X-ray nanoscopy reveals that acoustic phonons trapped in nanoscale twin domains govern the dynamics of the ultrafast transition into the precursor phase, while nucleation and growth of metallic domains dictate the duration of the slower transition into the metallic phase. The enhancement of the long-range order before completion of the electronic transition demonstrates the critical role the nonequilibrium structural phases play during electronic phase transitions in correlated electrons systems.