arXiv subjects

Ivan K. Schuller

Publications and source records attributed to Ivan K. Schuller.

At least 37 records · Page 2Linked to original sources

arXiv2023

Local strain inhomogeneities during the electrical triggering of a metal-insulator transition revealed by the x-ray microscopy

Electrical triggering of a metal-insulator transition (MIT) often results in the formation of characteristic spatial patterns such as a metallic filament percolating through an insulating matrix or an insulating barrier splitting a conducting matrix. When the MIT triggering is driven by electrothermal effects, the temperature of the filament or barrier can be substantially higher than the rest of material. Using x-ray microdiffraction and dark-field x-ray microscopy, we show that electrothermal MIT triggering leads to the development of an inhomogeneous strain profile across the switching device, even when the material does not undergo a 1st order structural phase transition coinciding with the MIT. Diffraction measurements further reveal evidence of lattice distortions and twinning occurring within the MIT switching device, highlighting a qualitative distinction between the electrothermal process and equilibrium thermal lattice expansion in nonlinear electrical systems. Electrically induced strain development, lattice distortions, and twinning could have important contributions in the MIT triggering process and could drive the material into non-equilibrium states, providing an unconventional pathway to explore the phase space of strongly correlated electronic systems.

cond-mat.mtrl-sci↗

arXiv2023

Reconfigurable cascaded thermal neuristors for neuromorphic computing

While the complementary metal-oxide semiconductor (CMOS) technology is the mainstream for the hardware implementation of neural networks, we explore an alternative route based on a new class of spiking oscillators we call thermal neuristors, which operate and interact solely via thermal processes. Utilizing the insulator-to-metal transition in vanadium dioxide, we demonstrate a wide variety of reconfigurable electrical dynamics mirroring biological neurons. Notably, inhibitory functionality is achieved just in a single oxide device, and cascaded information flow is realized exclusively through thermal interactions. To elucidate the underlying mechanisms of the neuristors, a detailed theoretical model is developed, which accurately reflects the experimental results. This study establishes the foundation for scalable and energy-efficient thermal neural networks, fostering progress in brain-inspired computing.

cs.ET↗

arXiv2023

High-Resolution Full-field Structural Microscopy of the Voltage Induced Filament Formation in Neuromorphic Devices

Neuromorphic functionalities in memristive devices are commonly associated with the ability to electrically create local conductive pathways by resistive switching. The archetypal correlated material, VO2, has been intensively studied for its complex electronic and structural phase transition as well as its filament formation under applied voltages. Local structural studies of the filament behavior are often limited due to time-consuming rastering which makes impractical many experiments aimed at investigating large spatial areas or temporal dynamics associated with the electrical triggering of the phase transition. Utilizing Dark Field X-ray Microscopy (DFXM), a novel full-field x-ray imaging technique, we study this complex filament formation process in-operando in VO2 devices from a structural perspective. We show that prior to filament formation, there is a significant gain of the metallic rutile phase beneath the metal electrodes that define the device. We observed that the filament formation follows a preferential path determined by the nucleation sites within the device. These nucleation sites are predisposed to the phase transition and can persistently maintain the high-temperature rutile phase even after returning to room temperature, which can enable a novel training/learning mechanism. Filament formation also appears to follow a preferential path determined by a nucleation site within the device which is predisposed to the rutile transition even after returning to room temperature. Finally, we found that small isolated low-temperature phase clusters can be present inside the high-temperature filaments indicating that the filament structure is not uniform. Our results provide a unique perspective on the electrically induced filament formation in metal-insulator transition materials, which further the basic understanding of this resistive switching.

physics.app-ph↗

arXiv2023

Magnetoresistance anomaly during the electrical triggering of a metal-insulator transition

Phase separation naturally occurs in a variety of magnetic materials and it often has a major impact on both electric and magnetotransport properties. In resistive switching systems, phase separation can be created on demand by inducing local switching, which provides an opportunity to tune the electronic and magnetic state of the device by applying voltage. Here we explore the magnetotransport properties in the ferromagnetic oxide (La,Sr)MnO3 (LSMO) during the electrical triggering of an intrinsic metal-insulator transition (MIT) that produces volatile resistive switching. This switching occurs in a characteristic spatial pattern, i.e., the formation of an insulating barrier perpendicular to the current flow, enabling an electrically actuated ferromagnetic-paramagnetic-ferromagnetic phase separation. At the threshold voltage of the MIT triggering, both anisotropic and colossal magnetoresistances exhibit anomalies including a large increase in magnitude and a sign flip. Computational analysis revealed that these anomalies originate from the coupling between the switching-induced phase separation state and the intrinsic magnetoresistance of LSMO. This work demonstrates that driving the MIT material into an out-of-equilibrium resistive switching state provides the means to electrically control of the magnetotransport phenomena.

cond-mat.mtrl-sci↗

arXiv2023

Light induced decoupling of electronic and magnetic properties in manganites

The strongly correlated material La0.7Sr0.3MnO3 (LSMO) exhibits metal-to-insulator and magnetic transition near room temperature. Although the physical properties of LSMO can be manipulated by strain, chemical doping, temperature, or magnetic field, they often require large external stimuli. To include additional flexibility and tunability, we developed a hybrid optoelectronic heterostructure that uses photocarrier injection from cadmium sulfide (CdS) to an LSMO layer to change its electrical conductivity. LSMO exhibits no significant optical response, however, the CdS/LSMO heterostructures show an enhanced conductivity, with ~ 37 % resistance drop, at the transition temperature under light stimuli. This enhanced conductivity in response to light is comparable to the effect of a 9 T magnetic field in pure LSMO. Surprisingly, the optical and magnetic responses of CdS/LSMO heterostructures are decoupled and exhibit different effects when both stimuli are applied. This unexpected behavior shows that heterostructuring strongly correlated oxides may require a new understanding of the coupling of physical properties across the transitions and provide the means to implement new functionalities.

cond-mat.mtrl-sci↗

arXiv2023

Unusual magnetic hysteresis and transition between vortex to double pole states arising from interlayer coupling in diamond shaped nanostructures

Controlling the magnetic ground states at the nanoscale is a long-standing basic research problem and an important issue in magnetic storage technologies. Here, we designed a nanostructured material that exhibits very unusual hysteresis loops due to a transition between vortex and double pole states. Arrays of 700 nm diamond-shape nanodots consisting of Py(30 nm)/Ru(tRu)/Py(30 nm) (Py, permalloy (Ni80Fe20)) trilayers were fabricated by interference lithography and e-beam evaporation. We show that varying the Ru interlayer spacer thickness (tRu) governs the interaction between the Py layers. We found this interaction mainly mediated by two mechanisms: magnetostatic interaction that favors antiparallel (antiferromagnetic, AFM) alignment of the Py layers and exchange interaction that oscillates between ferromagnetic (FM) and AFM couplings. For a certain range of Ru thicknesses, FM coupling dominates and forms magnetic vortices in the upper and lower Py layers. For Ru thicknesses at which AFM coupling dominates, the magnetic state in remanence is a double pole structure. Our results showed that the interlayer exchange coupling interaction remains finite even at 4 nm Ru thickness. The magnetic states in remanence, observed by Magnetic Force Microscopy (MFM), are in good agreement with corresponding hysteresis loops obtained by Magneto-Optic Kerr Effect (MOKE) and micromagnetic simulations.

cond-mat.mes-hall↗

arXiv2023

Correlative mapping of local hysteresis properties in VO$_2$

We have developed a new optical microscopy technique able to track micron-sized surface clusters as temperature is varied. Potential candidates for study include phase separated metal-insulator materials, ferroelectrics, and porous structures. Several key techniques (including autofocus, step motor/cross correlation alignments, single-pixel thresholding, pair connectivity correlation length and image convolution) were implemented in order to obtain a time series of thresholded images. Here, we apply this new method to probe the archetypal phase separated insulator-metal transition in VO$_2$. A precise time and temperature series of the insulator-metal transition was achieved, allowing us to construct for the first time in this material spatial maps of the transition temperature T$_c$. These maps reveal multiple interesting features such as fractal electronic patterns on micron scales, regions of the sample with an extremely large or nearly absent local hysteresis, a positive correlation between the T$_c$ value and the hysteresis width $Δ$T$_c$, and high cycle-to-cycle reproducibility of the transition. These maps also allow for the identification of individual pixels with unique transition characteristics. This unprecedented knowledge of the local properties of each spot along with the behavior of the entire network paves the way to novel electronics applications enabled by, {\em e.g.}, addressing specific regions with desired memory and/or switching characteristics, as well as detailed explorations of open questions in the theory of hysteresis.

cond-mat.str-el↗

arXiv2022

Spin Seebeck effect at low temperatures in the nominally paramagnetic insulating state of vanadium dioxide

The low temperature monoclinic, insulating phase of vanadium dioxide is ordinarily considered nonmagnetic, with dimerized vanadium atoms forming spin singlets, though paramagnetic response is seen at low temperatures. We find a nonlocal spin Seebeck signal in VO2 films that appears below 30 K and which increases with decreasing temperature. The spin Seebeck response has a non-hysteretic dependence on in-plane external magnetic field. This paramagnetic spin Seebeck response is discussed in terms of prior findings on paramagnetic spin Seebeck effects and expected magnetic excitations of the monoclinic ground state.

cond-mat.str-el↗

arXiv2022

Imaging the itinerant-to-localized transmutation of electrons across the metal-to-insulator transition in V$_2$O$_3$

In solids, strong repulsion between electrons can inhibit their movement and result in a "Mott" metal-to-insulator transition (MIT), a fundamental phenomenon whose understanding has remained a challenge for over 50 years. A key issue is how the wave-like itinerant electrons change into a localized-like state due to increased interactions. However, observing the MIT in terms of the energy- and momentum-resolved electronic structure of the system, the only direct way to probe both itinerant and localized states, has been elusive. Here we show, using angle-resolved photoemission spectroscopy (ARPES), that in V$_2$O$_3$ the temperature-induced MIT is characterized by the progressive disappearance of its itinerant conduction band, without any change in its energy-momentum dispersion, and the simultaneous shift to larger binding energies of a quasi-localized state initially located near the Fermi level.

cond-mat.str-el↗

arXiv2022

Quantum materials for energy-efficient neuromorphic computing

Neuromorphic computing approaches become increasingly important as we address future needs for efficiently processing massive amounts of data. The unique attributes of quantum materials can help address these needs by enabling new energy-efficient device concepts that implement neuromorphic ideas at the hardware level. In particular, strong correlations give rise to highly non-linear responses, such as conductive phase transitions that can be harnessed for short and long-term plasticity. Similarly, magnetization dynamics are strongly non-linear and can be utilized for data classification. This paper discusses select examples of these approaches, and provides a perspective for the current opportunities and challenges for assembling quantum-material-based devices for neuromorphic functionalities into larger emergent complex network systems.

cs.ET↗

arXiv2022

Direct visualization of percolating metal-insulator transition in V2O3 using scanning microwave impedance microscopy

Using the extensively studied V2O3 as a prototype system, we investigate the role of percolation in metal-insulator transition (MIT). We apply scanning microwave impedance microscopy to directly determine the metallic phase fraction p and relate it to the macroscopic conductance G, which shows a sudden jump when p reaches the percolation threshold. Interestingly, the conductance G exhibits a hysteretic behavior against p, suggesting two different percolating processes upon cooling and warming. Based on our image analysis and model simulation, we ascribe such hysteretic behavior to different domain nucleation and growth processes between cooling and warming, which is likely caused by the decoupled structural and electronic transitions in V2O3 during MIT. Our work provides a microscopic view of how the interplay of structural and electronic degrees of freedom affects MIT in strongly correlated systems.

cond-mat.str-el↗

arXiv2022

Probing FeSi, a d-electron topological Kondo insulator candidate, with magnetic field, pressure, and microwaves

Recently, evidence for a conducting surface state below 19 K was reported for the correlated d-electron small gap semiconductor FeSi. In the work reported herein, the conducting surface state and the bulk phase of FeSi were probed via electrical resistivity measurements as a function of temperature T, magnetic field B to 60 T and pressure P to 7.6 GPa, and by means of a magnetic field modulated microwave spectroscopy (MFMMS) technique. The properties of FeSi were also compared to those of the Kondo insulator SmB6 to address the question of whether FeSi is a d-electron analogue of an f-electron Kondo insulator and, in addition, a topological Kondo insulator. The overall behavior of the magnetoresistance MR of FeSi at temperatures above and below the onset temperature (T_S) 19 K of the conducting surface state is similar to that of SmB6. The two energy gaps, inferred from the resistivity data in the semiconducting regime, increase with pressure up to about 7 GPa, followed by a drop which coincides with a sharp suppression of T_S. This behavior is similar to that reported for SmB6, except that the two energy gaps in SmB6 decrease with pressure before dropping abruptly at T_S. The MFMMS measurements showed a sharp feature at T_S (19 K) for FeSi, but no such feature was observed at T_S 4.5 K for SmB6. The absence of a feature at T_S for SmB6 may be due to experimental issues and will be the subject of a future investigation.

cond-mat.str-el↗

arXiv2022

Tuning spin-orbit torques across the phase transition in VO$_2$/NiFe heterostructure

The emergence of spin-orbit torques as a promising approach to energy-efficient magnetic switching has generated large interest in material systems with easily and fully tunable spin-orbit torques. Here, current-induced spin-orbit torques in VO$_2$/NiFe heterostructures were investigated using spin-torque ferromagnetic resonance, where the VO$_2$ layer undergoes a prominent insulator-metal transition. A roughly two-fold increase in the Gilbert damping parameter, $α$, with temperature was attributed to the change in the VO$_2$/NiFe interface spin absorption across the VO$_2$ phase transition. More remarkably, a large modulation ($\pm$100%) and a sign change of the current-induced spin-orbit torque across the VO$_2$ phase transition suggest two competing spin-orbit torque generating mechanisms. The bulk spin Hall effect in metallic VO$_2$, corroborated by our first-principles calculation of spin Hall conductivity, $σ_{SH} \approx 10^4 \frac{\hbar}{e} Ω^{-1} m^{-1}$, is verified as the main source of the spin-orbit torque in the metallic phase. The self-induced/anomalous torque in NiFe, of the opposite sign and a similar magnitude to the bulk spin Hall effect in metallic VO$_2$, could be the other competing mechanism that dominates as temperature decreases. For applications, the strong tunability of the torque strength and direction opens a new route to tailor spin-orbit torques of materials which undergo phase transitions for new device functionalities.

cond-mat.mtrl-sci↗

arXiv2021

Stress-tailoring magnetic anisotropy of V$_2$O$_3$/Ni bilayers

We report on a temperature-driven reversible change of the in-plane magnetic anisotropy of V$_2$O$_3$/Ni bilayers. This is caused by the rhombohedral to monoclinic structural phase transition of V$_2$O$_3$ at $T_C$ = 160 K. The in-plane magnetic anisotropy is uniaxial above $T_C$, but as the bilayer is cooled through the structural phase transition, a secondary magnetic easy axis emerges. Ferromagnetic resonance measurements show that this change in magnetic anisotropy is reversible with temperature. We identify two structural properties of the V$_2$O$_3$/Ni bilayers affecting the in-plane magnetic anisotropy: (1) a growth-induced uniaxial magnetic anisotropy associated with step-like terraces in the bilayer microstructure and (2) a low-temperature strain-induced biaxial anisotropy associated with the V$_2$O$_3$ structural phase transition. Magnetoresistance measurements corroborate the change in magnetic anisotropy across the structural transition and suggest that the negative magnetostriction of Ni leads to the emergence of a strain-induced easy-axis. This shows that a temperature-dependent structural transition in V$_2$O$_3$ may be used to tune the magnetic anisotropy in an adjacent ferromagnetic thin film.

cond-mat.mtrl-sci↗

arXiv2021

Optical imaging of strain-mediated phase coexistence during electrothermal switching in a Mott insulator

Resistive-switching -- the current-/voltage-induced electrical resistance change -- is at the core of memristive devices, which play an essential role in the emerging field of neuromorphic computing. This study is about resistive switching in a Mott-insulator, which undergoes a thermally driven metal-to-insulator transition. Two distinct switching mechanisms were reported for such a system: electric-field-driven resistive switching and electrothermal resistive switching. The latter results from an instability caused by Joule heating. Here, we present the visualization of the reversible resistive switching in a planar V$_2$O$_3$ thin-film device using high-resolution wide-field microscopy in combination with electric transport measurements. We investigate the interaction of the electrothermal instability with the strain-induced spontaneous phase-separation in the V$_2$O$_3$ thin film at the Mott-transition. The photomicrographs show the formation of a narrow metallic filament with a minimum width $\lesssim$ 500\,nm. Although the filament formation and the overall shape of the current-voltage characteristics (IVCs) are typical of an electrothermal breakdown, we also observe atypical effects like oblique filaments, filament splitting, and hysteretic IVCs with sawtooth-like jumps at high currents in the low-resistance regime. We were able to reproduce the experimental results in a numerical model based on a two-dimensional resistor network. This model demonstrates that resistive switching, in this case, is indeed electrothermal and that the intrinsic heterogeneity is responsible for the atypical effects. This heterogeneity is strongly influenced by strain, thereby establishing a link between switching dynamics and structural properties.

cond-mat.mtrl-sci↗

arXiv2020

Direct observation of the electrically triggered Insulator-Metal transition in V3O5 far below the transition temperature

Resistive switching is one of the key phenomena for applications such as nonvolatile memories or neuromorphic computing. V3O5, a compound of the vanadium oxide Magnéli series, is one of the rare materials to exhibit an insulator-metal transition (IMT) above room temperature (Tc ~ 415 K). Here we demonstrate both static dc resistive switching (RS) and fast oscillatory spiking regimes in V3O5 devices at room temperature (120 K below the phase transition temperature) by applying an electric field. We use operando optical imaging to track a reflectivity change during the RS and find that a percolating high temperature metallic phase filament is formed. This demonstrates that the electrically induced RS triggers the phase transition. Furthermore, we optically capture the spiking oscillations that we link to the negative differential resistance regime and find the filament forms and dissolves via a periodic spatio-temporal instability that we describe by numerical simulations.

cond-mat.mtrl-sci↗

arXiv2020

A hybrid optoelectronic Mott insulator

The coupling of electronic degrees of freedom in materials to create hybridized functionalities is a holy grail of modern condensed matter physics that may produce novel mechanisms of control. Correlated electron systems often exhibit coupled degrees of freedom with a high degree of tunability which sometimes lead to hybridized functionalities based on external stimuli. However, the mechanisms of tunability and the sensitivity to external stimuli are determined by intrinsic material properties which are not always controllable. A Mott metal-insulator transition, which is technologically attractive due to the large changes in resistance, can be tuned by doping, strain, electric fields, and orbital occupancy but cannot be, in and of itself, controlled externally with light. Here we present a new approach to produce hybridized functionalities using a properly engineered photoconductor/strongly-correlated hybrid heterostructure, showing control of the Metal-to-Insulator transition (MIT) using optical means. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the close proximity between the two materials, the heterostructure exhibits large volatile and nonvolatile, photoinduced resistivity changes and substantial photoinduced shifts in the MIT transition temperatures. This approach can potentially be extended to other judiciously chosen combinations of strongly correlated materials with systems which exhibit optically, electrically or magnetically controllable behavior.

physics.app-ph↗

arXiv2020

Resistive switching in reverse: voltage driven formation of a transverse insulating barrier

Application of an electric stimulus to a material with a metal-insulator transition can trigger a large resistance change. Resistive switching from an insulating into a metallic phase, which typically occurs by the formation of conducting filaments parallel to the current flow, has been an active research topic. Here we present the discovery of an opposite, metal-to-insulator switching that proceeds via nucleation and growth of an insulating barrier perpendicular to the driving current. The barrier formation leads to an unusual N-type negative differential resistance in the current-voltage characteristics. Electrically inducing a transverse barrier enables a novel approach to voltage-controlled magnetism. By triggering a metal-to-insulator resistive switching in a magnetic material, local on/off control of ferromagnetism can be achieved by a global voltage bias applied to the whole device.

cond-mat.mtrl-sci↗