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Michael Sing

Publications and source records attributed to Michael Sing.

17 recordsLinked to original sources

Gate-controlled analog memcapacitance in LaAlO3/SrTiO3 interface-based devices

Current memcapacitor implementations typically demand complex fabrication processes or depend on organic materials exhibiting poor environmental stability and reproducibility. Here, we demonstrate memcapacitor structures utilizing a quasi 2-dimensional electron gas, formed at the crystalline LaAlO3/SrTiO3 heterointerface, as electrodes and SiO2/SrTiO3 as dielectric layer. The observed memcapacitance originates from the charge localization in a lateral floating gate, while an applied gate voltage enables reversible tuning of the device capacitance. Furthermore, preprogrammed or erased gate biases enable controllable shifts of the capacitance hysteresis window toward positive or negative bias, leading to an enlarged capacitance gap at zero bias. A memcapacitor model developed for this system reproduces the main features of the experimental capacitance hysteresis, capturing the effects of charge fluctuations and dielectric frequency modulation within the oxide layer. The demonstrated low-voltage operation and gate tunability of oxide interface-based memcapacitors highlight their potential for power-efficient, capacitor-based neuromorphic and synaptic electronic architectures.

physics.app-ph

Oxide Interface-Based Polymorphic Electronic Devices for Neuromorphic Computing

Aside from recent advances in artificial intelligence (AI) models, specialized AI hardware is crucial to address large volumes of unstructured and dynamic data. Hardware-based AI, built on conventional complementary metal-oxidesemiconductor (CMOS)-technology, faces several critical challenges including scaling limitation of devices [1, 2], separation of computation and memory units [3] and most importantly, overall system energy efficiency [4]. While numerous materials with emergent functionalities have been proposed to overcome these limitations, scalability, reproducibility, and compatibility remain critical obstacles [5, 6]. Here, we demonstrate oxide-interface based polymorphic electronic devices with programmable transistor, memristor, and memcapacitor functionalities by manipulating the quasi-two-dimensional electron gas in LaAlO3/SrTiO3 heterostructures [7, 8] using lateral gates. A circuit utilizing two polymorphic functionalities of transistor and memcapacitor exhibits nonlinearity and short-term memory, enabling implementation in physical reservoir computing. An integrated circuit incorporating transistor and memristor functionalities is utilized for the transition from short- to long-term synaptic plasticity and for logic operations, along with in-situ logic output storage. The same circuit with advanced reconfigurable synaptic logic operations presents high-level multi-input decision-making tasks, such as patient-monitoring in healthcare applications. Our findings pave the way for oxide-based monolithic integrated circuits in a scalable, silicon compatible, energy efficient single platform, advancing both the polymorphic and neuromorphic computings.

cond-mat.dis-nn

Inducing ferromagnetism by structural engineering in a strongly spin-orbit coupled oxide

Magnetic materials with strong spin-orbit coupling (SOC) are essential for the advancement of spin-orbitronic devices, as they enable efficient spin-charge conversion, complex magnetic structures, spin-valley physics, topological phases and other exotic phenomena. 5d transition-metal oxides such as SrIrO3 feature large SOC, but usually show paramagnetic behavior due to broad bands and a low density of states at the Fermi level, accompanied by a relatively low Coulomb repulsion. Here, we unveil ferromagnetism in 5d SrIrO3 thin films grown on SrTiO3 (111). Through substrate-induced structural engineering, a zigzag stacking of three-unit-cell thick layers along the [111] direction is achieved, stabilizing a ferromagnetic state at the interfaces. Magnetotransport measurements reveal an anomalous Hall effect below ~30 K and hysteresis in the Hall conductivity below 7 K, indicating ferromagnetic ordering. X-ray magnetic circular dichroism further supports these results. Theoretical analysis suggests that the structural engineering of the IrO6 octahedral network enhances the density of states at the Fermi level and thus stabilizes Stoner ferromagnetism. This work highlights the potential of structurally engineered 5d oxides for spin-orbitronic devices, where efficient control of SOC-induced magnetic phases by electric currents can lead to lower energy consumption and improved performance in next-generation device technologies.

cond-mat.mtrl-sci

Hybrid Photoelectron Momentum Microscope at the Soft X-ray Beamline I09 of the Diamond Light Source

Soft X-ray momentum microscopy of crystalline solids is a highly efficient approach to map the photoelectron distribution in four-dimensional (E,k) parameter space over the entire Brillouin zone. The fixed sample geometry eliminates any modulation of the matrix element otherwise caused by changing the angle of incidence. We present a new endstation at the soft X-ray branch of beamline I09 at the Diamond Light Source, UK. The key component is a large single hemispherical spectrometer combined with a time-of-flight analyzer behind the exit slit. The photon energy ranges from hv = 105 eV to 2 keV, with circular polarization available for hv > 150 eV, allowing for circular dichroism measurements in angle-resolved photoemission (CD-ARPES). A focused and monochromatized He lamp is used for offline measurements. Under k-imaging conditions, energy and momentum resolution are 10.2 meV (FWHM) and 0.010 angstroms^-1 (base resolution 4.2 meV with smallest slits and a pass energy of 8 eV). The large angular filling of the entrance lens and hemisphere (225 mm path radius) allows k-field-of-view diameters > 6 angstroms^-1. Energy filtered X-PEEM mode using synchrotron radiation revealed a resolution of 300 nm. As examples we show 2D band mapping of bilayer graphene, 3D mapping of the Fermi surface of Cu, CD-ARPES for intercalated indenene layers and the sp valence bands of Cu and Au, and full-field photoelectron diffraction patterns of Ge.

cond-mat.mtrl-sci

Epitaxial RuO$_2$ and IrO$_2$ films by pulsed laser deposition on TiO$_2$(110)

We present a systematic growth study of epitaxial RuO$_2$(110) and IrO$_2$(110) on TiO$_2$(110) substrates by pulsed laser deposition. We describe the main challenges encountered in the growth process, such as a deteriorating material flux due to laser induced target metallization or the delicate balance of under- vs over-oxidation of the 'stubborn' Ru and Ir metals. We identify growth temperatures and oxygen partial pressures of 700 K, $1\times 10^{-3}$ mbar for RuO$_2$ and 770 K, $5\times 10^{-4}$ mbar for IrO$_2$ to optimally balance between metal oxidation and particle mobility during nucleation. In contrast to IrO$_2$, RuO$_2$ exhibits layer-by-layer growth up to 5 unit cells if grown at high deposition rates. At low deposition rates, the large lattice mismatch between film and substrate fosters initial 3D island growth and cluster formation. In analogy to reports for RuO$_2$ based on physical vapor deposition, we find these islands to eventually merge and growth to continue in a step flow mode, resulting in highly crystalline, flat, stoichiometric films of RuO$_2$(110) (up to 30 nm thickness) and IrO$_2$(110) (up to 13 nm thickness) with well defined line defects.

cond-mat.mtrl-sci

Nature of the metallic and in-gap states in Ni-doped SrTiO$_3$

Epitaxial thin films of SrTiO$_3$(100) doped with 6% and 12% Ni are studied with resonant angle-resolved photoelectron spectroscopy (ARPES) at the Ti and Ni L2,3-edges. We find that the Ni doping shifts the valence band (VB) of pristine SrTiO$_3$ towards the Fermi level (p-doping) and reduces its band gap. This is accompanied by an upward energy shift of the Ti t2g-derived mobile electron system (MES). Thereby, the in-plane dxy-derived bands reduce the embedded electron density, as evidenced by progressive reduction of their Fermi momentum with the Ni concentration, and the out-of-plane dxz/yz-derived bands depopulate, making the MES purely two-dimensional. Furthermore, the Ti and Ni L2,3-edge resonant photoemission is used to identify the Ni 3d impurity state in the vicinity of the valence-band maximum, and decipher the full spectrum of the VO-induced in-gap states originating from the Ni atoms, Ti atoms, and from their hybridized orbitals. Our experimental information about the dependence of the valence bands, MES and in-gap states in Ni-doped SrTiO$_3$ may help development of this material towards its device applications associated with the reduced optical band gap.

cond-mat.mtrl-sci

Linear colossal magnetoresistance driven by magnetic textures in LaTiO3 thin films on SrTiO3

Linear magnetoresistance (LMR) is of particular interest for memory, electronics, and sensing applications, especially when it does not saturate over a wide range of magnetic fields. One of its principal origins is local mobility or density inhomogeneities, often structural, which in the Parish-Littlewood theory leads to an unsaturating LMR proportional to mobility. Structural disorder, however, also tends to limit the mobility and hence the overall LMR amplitude. An alternative route to achieve large LMR is via non-structural inhomogeneities which do not affect the zero field mobility, like magnetic domains. Here, linear positive magnetoresistance caused by magnetic texture is reported in \ch{LaTiO3}/\ch{SrTiO3} heterostructures. The LMR amplitude reaches up to 6500\% at 9T. This colossal value is understood by the unusual combination of a very high thin film mobility, up to 40 000 cm$^2$/V.s, and a very large coverage of low-mobility regions. These regions correlate with a striped magnetic structure, compatible with a spiral magnetic texture in the \ch{LaTiO3} film, revealed by low temperature Lorentz transmission electron microscopy. These results provide a novel route for the engineering of large-LMR devices.

cond-mat.mes-hall

Toward Functionalized Ultrathin Oxide Films: the Impact of Surface Apical Oxygen

Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO$_3$ as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which persist even in an ultrahigh vacuum environment, are shown to severely affect the intrinsic electronic structure of a transition metal oxide film. Their presence leads to the formation of an electronically dead surface layer but also alters the band filling and the electron correlations in the thin films. These findings highlight that it is important to take into account surface apical oxygen or -- mutatis mutandis -- the specific oxygen configuration imposed by a capping layer to predict the behavior of ultrathin films of transition metal oxides near the single unit-cell limit.

cond-mat.mtrl-sci

Hard x-ray angle-resolved photoemission from a buried high-mobility electron system

Novel two-dimensional electron systems at the interfaces and surfaces of transition-metal oxides recently have attracted much attention as they display tunable, intriguing properties that can be exploited in future electronic devices. Here we show that a high-mobility quasi-two-dimensional electron system with strong spin-orbit coupling can be induced at the surface of a KTaO$_3$ (001) crystal by pulsed laser deposition of a disordered LaAlO$_3$ film. The momentum-resolved electronic structure of the buried electron system is mapped out by hard x-ray angle-resolved photoelectron spectroscopy. From a comparison to calculations it is found that the band structure deviates from that of electron-doped bulk KTaO$_3$ due to the confinement to the interface. Nevertheless, the Fermi surface appears to be clearly three-dimensional. From the $k$ broadening of the Fermi surface and core-level depth profiling we estimate the extension of the electron system to be at least 1 nm but not much larger than 2 nm, respectively.

cond-mat.str-el

Controlling the electronic interface properties of AlO$_x$/SrTiO$_3$ heterostructures

Depositing disordered Al on top of SrTiO$_3$ is a cheap and easy way to create a two-dimensional electron system in the SrTiO$_3$ surface layers. To facilitate future device applications we passivate the heterostructure by a disordered LaAlO$_3$ capping layer to study the electronic properties by complementary x-ray photoemission spectroscopy and transport measurements on the very same samples. We also tune the electronic interface properties by adjusting the oxygen pressure during film growth.

cond-mat.mtrl-sci

Effects of finite-range interactions on the one-electron spectral properties of TTF-TCNQ

The electronic dispersions of the quasi-one-dimensional organic conductor TTF-TCNQ are studied by angle-resolved photoelectron spectroscopy (ARPES) with higher angular resolution and accordingly smaller step width than in previous studies. Our experimental results suggest that a refinement of the single-band 1D Hubbard model that includes finite-range interactions is needed to explain these photoemission data. To account for the effects of these finite-range interactions we employ a mobile quantum impurity scheme that describes the scattering of fractionalized particles at energies above the standard Tomonaga-Luttinger liquid limit. Our theoretical predictions agree quantitatively with the location in the $(k,\omega)$ plane of the experimentally observed ARPES structures at these higher energies. The nonperturbative microscopic mechanisms that control the spectral properties are found to simplify in terms of the exotic scattering of the charge fractionalized particles. We find that the scattering occurs in the unitary limit of (minus) infinite scattering length, which limit occurs within neutron-neutron interactions in shells of neutron stars and in the scattering of ultracold atoms but not in perturbative electronic condensed-matter systems. Our results provide important physical information on the exotic processes involved in the finite-range electron interactions that control the high-energy spectral properties of TTF-TCNQ. Our results also apply to a wider class of 1D and quasi-1D materials and systems that are of theoretical and potential technological interest.

cond-mat.str-el

Tailoring Materials for Mottronics: Excess Oxygen Doping of a Prototypical Mott Insulator

The Mott transistor is a paradigm for a new class of electronic devices---often referred to by the term Mottronics---, which are based on charge correlations between the electrons. Since correlation-induced insulating phases of most oxide compounds are usually very robust, new methods have to be developed to push such materials right to the boundary to the metallic phase in order to enable the metal-insulator transition to be switched by electric gating. Here we demonstrate that thin films of the prototypical Mott insulator LaTiO$_3$ grown by pulsed laser deposition under oxygen atmosphere are readily tuned by excess oxygen doping across the line of the band-filling controlled Mott transition in the electronic phase diagram. The detected insulator to metal transition is characterized by a strong change in resistivity of several orders of magnitude. The use of suitable substrates and capping layers to inhibit oxygen diffusion facilitates full control of the oxygen content and renders the films stable against exposure to ambient conditions, making LaTiO$_{3+x}$ a promising functional material for Mottronics devices.

cond-mat.mtrl-sci

Gate-tunable, normally-on to normally-off memristance transition in patterned LaAlO3/SrTiO3 interfaces

We report gate-tunable memristive switching in patterned LaAlO3/SrTiO3 interfaces at cryogenic temperatures. The application of voltages in the order of a few volts to the back gate of the device allows controlling and switching-on and -off the inherent memory functionality (memristance). For large and small gate voltages a simple non-linear resistance characteristic is observed while a pinched hysteresis loop and memristive switching occurs in an intermediate voltage range. The memristance is further controlled by the density of oxygen vacancies, which is tuned by annealing the sample at 300 {\deg}C in nitrogen atmosphere. Depending on the annealing time the memristance at zero gate voltage can be switched on and off leading to normally-on and normally-off memristors. The presented device offers reversible and irreversible control of memristive characteristics by gate voltages and annealing, respectively, which may allow to compensate fabrication variabilities of memristors that complicate the realization of large memristor-based neural networks.

cond-mat.mes-hall

Absence of metallicity in K-doped picene: Importance of electronic correlations

Potassium-doped picene (K$_x$picene) has recently been reported to be a superconductor at $x=3$ with critical temperatures up to 18 K. Here we study the electronic structure of K-doped picene films by photoelectron spectroscopy and {\it ab initio} density functional theory combined with dynamical mean-field theory (DFT+DMFT). Experimentally we observe that, except for spurious spectral weight due to the lack of a homogeneous chemical potential at low K-concentrations ($x \approx 1$), the spectra always display a finite energy gap. This result is supported by our DFT+DMFT calculations which provide clear evidence that K$_x$picene is a Mott insulator for integer doping concentrations $x=1$, 2, and 3. We discuss various scenarios to understand the discrepancies with previous reports of superconductivity and metallic behavior.

cond-mat.str-el

Unoccupied electronic structure of TiOCl studied by x-ray absorption near-edge spectroscopy

We study the unoccupied electronic structure of the spin-1/2 quantum magnet TiOCl by x-ray absorption near-edge spectroscopy (XANES) at the Ti L and O K edges. Data is acquired both in total electron and fluorescence yield mode (TEY and FY, respectively). While only the latter allows to access the unconventional low-temperature spin-Peierls (SP) phase of TiOCl the signal is found to suffer from significant self-absorption in this case. Nevertheless, we conclude from FY data that effects of the SP distortion on the electronic structure are absent within experimental accuracy. The similarity of room-temperature FY and TEY data, the latter not being obscured by self-absorption, allows us to use TEY spectra for comparison with simulations. These are performed by cluster calculations in D$_{4h}$ and D$_{2h}$ symmetries using two different codes. We extract values of the crystal-field splitting (CFS) and parametrize our results in often found notations by Slater, Racah and Butler. In all cases, good agreement with published values from other studies is found.

cond-mat.str-el

Two-Spinon and Orbital Excitations of the Spin-Peierls System TiOCl

We combine high-resolution resonant inelastic x-ray scattering with cluster calculations utilizing a recently derived effective magnetic scattering operator to analyze the polarization, excitation energy, and momentum dependent excitation spectrum of the low-dimensional quantum magnet TiOCl in the range expected for orbital and magnetic excitations (0 - 2.5 eV). Ti 3d orbital excitations yield complete information on the temperature-dependent crystal-field splitting. In the spin-Peierls phase we observe a dispersive two-spinon excitation and estimate the inter- and intra-dimer magnetic exchange coupling from a comparison to cluster calculations.

cond-mat.str-el

Resonant Inelastic X-Ray Scattering (RIXS) in SrCuO$_{2}$

The resonant inelastic x-ray scattering (RIXS) was measured in an insulating SrCuO$_{2}$ with changing the incident photon energy ($hν$) near the Cu $1s$ absorption edge (K-edge). Complex structures and their dependences on the momentum transfer($Δk$) and $hν$ were observed. The $hν$ dependence of the RIXS spectra measured for a constant $Δk$=2.4$π$ has shown a remarkable enhancement near the absorption maximum and a shift of the spectral weight toward larger loss-energy with increasing $hν$. Also, the energy of the inelastic loss peak in the RIXS spectra for the fixed excitation at 8.993 keV, 10 eV below the absorption maximum, has shown a clear dependence on $Δk$. These results are in a qualitative agreement with a theoretical prediction. Full utilization of the potential of the high brilliance X ray light source at BL19LXU of SPring-8 with 27 m long insertion device will open up a breakthrough in RIXS for heavy transition metal compounds in accordance with the improvement in focussing and analyzing elements.

cond-mat.str-el