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Register a new userDynamics of the photoinduced insulator-to-metal transition in a nickelate film
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The control of materials properties with light is a promising approach towards the realization of faster and smaller electronic devices. With phases that can be controlled via strain, pressure, chemical composition or dimensionality, nickelates are good candidates for the development of a new generation of high performance and low consumption devices. Here we analyze the photoinduced dynamics in a single crystalline NdNiO$_3$ film upon excitation across the electronic gap. Using time-resolved reflectivity and resonant x-ray diffraction, we show that the pump pulse induces an insulator-to-metal transition, accompanied by the melting of the charge order. Finally we compare our results to similar studies in manganites and show that the same model can be used to describe the dynamics in nickelates, hinting towards a unified description of these photoinduced phase transitions.
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Heavily oxygen deficient NdNiO$_3$ (NNO) films, which are insulating due to electron localization, contain pristine regions that undergo a hidden metal-insulator transition. Increasing oxygen content increases the connectivity of the metallic regions and the metal-insulator transition is first revealed, upon reaching the percolation threshold, by the presence of hysteresis. Only upon further oxygenation is the global metallic state (with a change in the resistivity slope) eventually achieved. It is shown that sufficient oxygenation leads to linear temperature dependence of resistivity in the metallic state, with a scattering rate directly proportional to temperature. Despite the known difficulties to establish the proportionality constant, the experiments are consistent with a relationship 1/$tau$= $alpha k_B T/hbar$, with $alpha$ not far from unity. These results could provide experimental support for recent theoretical predictions of disorder in a two-fluid model as a possible origin of Planckian dissipation.
We studied the electronic and magnetic dynamics of ferromagnetic insulating BaFeO3 thin films by using pump-probe time-resolved resonant x-ray reflectivity at the Fe 2p edge. By changing the excitation density, we found two distinctly different types of demagnetization with a clear threshold behavior. We assigned the demagnetization change from slow (~ 150 ps) to fast (< 70 ps) to a transition into a metallic state induced by laser excitation. These results provide a novel approach for locally tuning magnetic dynamics. In analogy to heat assisted magnetic recording, metallization can locally tune the susceptibility for magnetic manipulation, allowing to spatially encode magnetic information.
Transition metal oxides possess complex free energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained $mathrm{La_{0.67}Ca_{0.33}MnO_3}$, optical excitation with a sub-100 fs pulse above $2 mathrm{mJ/cm^2}$ leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multi-step process. We conclude that the phase transition is driven by partial charge order melting, followed by growth of the persistent metallic phase on longer timescales. A time-dependent Ginzburg-Landau model can describe the fast dynamics of the reflectivity, followed by longer timescale in-growth of the metallic phase.
The insulator-to-metal transition (IMT) of the simple binary compound of vanadium dioxide VO$_2$ at $sim 340$ K has been puzzling since its discovery more than five decades ago. A wide variety of photon and electron probes have been applied in search of a satisfactory microscopic mechanistic explanation. However, many of the conclusions drawn have implicitly assumed a {em homogeneous} material response. Here, we reveal inherently {em inhomogeneous} behavior in the study of the dynamics of individual VO$_2$ micro-crystals using a combination of femtosecond pump-probe microscopy with nano-IR imaging. The time scales of the photoinduced bandgap reorganization in the ultrafast IMT vary from $simeq 40 pm 8$ fs, i.e., shorter than a suggested phonon bottleneck, to $sim 200pm20$ fs, with an average value of $80 pm 25$ fs, similar to results from previous studies on polycrystalline thin films. The variation is uncorrelated with crystal size, orientation, transition temperature, and initial insulating phase. This together with details of the nano-domain behavior during the thermally-induced IMT suggests a significant sensitivity to local variations in, e.g., doping, defects, and strain of the microcrystals. The combination of results points to an electronic mechanism dominating the photoinduced IMT in VO$_2$, but also highlights the difficulty of deducing mechanistic information where the intrinsic response in correlated matter may not yet have been reached.
Phase transitions driven by ultrashort laser pulses have attracted interest both for understanding the fundamental physics of phase transitions and for potential new data storage or device applications. In many cases these transitions involve transient states that are different from those seen in equilibrium. To understand the microscopic properties of these states, it is useful to develop elementally selective probing techniques that operate in the time domain. Here we show fs-time-resolved measurements of V Ledge Resonant Inelastic X-Ray Scattering (RIXS) from the insulating phase of the Mott- Hubbard material V2O3 after ultrafast laser excitation. The probed orbital excitations within the d-shell of the V ion show a sub-ps time response, which evolve at later times to a state that appears electronically indistinguishable from the high-temperature metallic state. Our results demonstrate the potential for RIXS spectroscopy to study the ultrafast orbital dynamics in strongly correlated materials.
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