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Khalil Harrabi

Publications and source records attributed to Khalil Harrabi.

11 recordsLinked to original sources

Distribution of Relaxation Times analysis of evolution of Oxygen Reduction Pathways for ionic conductor infiltration on MIEC cathode

Solid oxide fuel cells (SOFCs) are promising electrochemical energy conversion devices; however, the sluggish cathodic oxygen reduction reaction (ORR) remains a major limitation for intermediate-temperature operation. ORR subprocesses can be modified by infiltrating ionic Sm0.2Ce0.8O2-delta (SDC) on mixed ionic electronic SrFe0.9Ti0.1O3-delta (STF). However, the processes are indistinguishable in most cases and poorly understood using conventional equivalent circuits. Distribution of Relaxation Times (DRT) analysis distinguishes these processes to identify the dynamics with temperature and surface reconstruction. Such analysis is being reported, revealing the connection between increase of active sites, temperature, and polarization resistance (RP). SDC infiltration preferentially accelerates oxygen surface exchange and activation processes over the relatively high frequency charge transfer process related to cathode surface at elevated temperatures for the infiltrated cells. RP was reduced substantially with the systematic redistribution of each process to as low as 0.04 ohm.cm2 at 800 degC. This work underlines the deconvolution of the processes using DRT as a tool, and SDC infiltrated STF as a model cathode system to provide a mechanistic insight of understanding ORR kinetics and design a rationale for developing high-performance SOFC air electrodes

cond-mat.mtrl-sci

Pattern recognition with superconducting wirelet neurons

Neuromorphic computing aims to reproduce the energy efficiency and adaptability of biological intelligence in hardware. Superconducting devices are an attractive platform due to their ultra-low dissipation and fast switching dynamics. Here we employ a resistively shunted superconducting wirelet as a minimal artificial neuron for temporal neuromorphic computation. This simple architecture enables straightforward fabrication, electronic control, and high scalability. Through experiments and advanced simulations, we show that it exhibits spiking voltage dynamics driven by the interplay of resistive switching and relaxation, with threshold, firing frequency, and refractory time tunable through applied current, temperature, and shunt resistance. We demonstrate neural network operation by synaptically training temporal voltage signals generated by individual neurons. In this approach, trainable temporal weights act directly on the time-dependent wirelet-neuron responses rather than on static neuron outputs alone, allowing the computation to exploit the full temporal structure of the superconducting spikes. As an illustrative example, we apply this framework to handwritten digit recognition and show accurate classification using only three superconducting wirelet neurons. We further discuss on-chip training based on related gated wirelets as tunable synaptic elements, establishing shunted superconducting wirelets as scalable, energy-efficient building blocks for cryogenic artificial intelligence hardware that can be integrated with other emerging superconducting technologies.

cond-mat.supr-con

Shunt-controlled resistive state of superconducting wires

The use of resistive shunts in superconducting electronics is vast and versatile, to dampen oscillations in junctions, stabilize switching behavior, aid current sensing, divert current during quenches, and protect both the superconductor and the circuit from damage. In single-photon detection by superconducting nanowires, the shunt is crucial for the timely relaxation of the sensor between the events to detect. Here we step out from the superconducting state and discuss the effect of the shunt resistor on the resistive state of a superconducting wire, at elevated currents still below the critical current for the transition to the normal state. We reveal how the shunt resistance controls the system dynamics and the onset of different resistive phases that include hot-spot and phase-slippage events. The accompanying dynamic current redistribution in the circuit also affects the local heating properties and additionally contributes to the control of the resistive state, particularly important at the elevated operation temperatures.

cond-mat.supr-con

Increased Covalence and V-center mediated Dark Fenton-Like Reactions in V-doped TiO2: Mechanisms of Enhanced Charge-Transfer

Tuning the valence state and electronic structure of catalytically active sites is crucial for improving Fenton and Fenton-like reactions, which rely on the efficient activation of the H2O2 molecule. Pure TiO2, however, has inadequate activity towards the H2O2 activation and is often constrained by the intrinsic electronic limitations of pristine TiO2. Herein, a rational approach has been demonstrated to improve the Fenton-like catalytic performance of TiO2 through multivalent vanadium (V) doping. A comprehensive characterization using X-Ray Diffraction (XRD), Raman spectroscopy, UV-Vis spectroscopy, X-Ray photoelectron spectroscopy (XPS), Electron paramagnetic resonance (EPR), and Density functional theory (DFT) reveals that V incorporation substantially alters the electronic structure of TiO2. The DFT results, supported by experimental data, indicate that V doping enhances Ti-O covalence and introduces mid-gap states, resulting in a reduced band gap and improved charge transfer. XPS confirms the coexistence of multiple oxidation states of V, which serve as active centres for activating H2O2 and generating OH radicals. As a result, V-doped TiO2 exhibits significantly enhanced dark-catalytic activity in degrading the organic dye Rhodamine B (RhB). Overall, this study provides fundamental insights into multivalent-cation-induced valence state and electronic structure modulation in TiO2, offering a promising strategy for designing high-performance catalysts via defect engineering for sustainable environmental remediation.

cond-mat.mtrl-sci

Hexagonal polymorphism induced structural disorder and dielectric anomalies of Ca/Mn modified BaTiO3

This work involves the local structural investigation of the samples using Extended X-ray Absorption Spectra (EXAFS) analysis to investigate structural changes due to the Ca and Mn-modified BaTiO3. TEM investigation of the crystal structure reveals the coexistence of the tetragonal and hexagonal phases of BaTiO3. Band gap modification and Urbach tail variation in UV-DRS measurements reveal a reduction of band gap from UV to Visible range (3.2 eV to 2 eV). This band gap change is correlated with the valence band modification observed in PES measurements due to localised defects in the material, and supported by theoretical Density of States calculations. The electron localisation function calculation is used to analyse the changes in the localised electron density near the dopant atoms. It reveals the local expansion and contraction of the lattice surrounding the dopant atom. All these structural modifications lead to variations in the dielectric properties and diffusive nature of the phase transition. The defect-induced structural modifications, multiple phase coexistence, band gap variations and dielectric properties are explored and correlated.

cond-mat.mtrl-sci

Correlation of the role of Li-doping in control of O-vacancies and Li interstitial formations in NiO with electrochemical properties

Aliovalent doping in an oxide material introduces modifications in the valence state of the host cation and often leads to tailoring the oxygen content in the lattice. Moreover, if the dopant cation is larger than the host cation, the lattice strain and disorder may be affected. Such changes are expected to modify the electronic clouds and lead to different ligand fields, which in turn should modify the bond lengths, and therefore phonons, electronic properties, transport properties, and charge storage properties. To understand such correlations an example is being investigated in this study by doping a larger Li+ ion in a NiO lattice. The effect on structure, phonons, electronic properties, and charge storage properties are investigated and correlated in a first-of-its-kind report. The charge storage properties are observed to improve with Li+ doping until 3% substitution and thereafter decrease due to the generation of Li+ interstitial in a 6% incorporated sample. The connection of oxygen vacancies and Ni3+ formation with Li+ incorporation is the backbone of this report.

cond-mat.mtrl-sci

Room temperature ferromagnetism induced by high valence cation V$^{+5}$/V$^{+4}$ substitution in SrFeO$_{3-δ}$

The structural and magnetic effects of non-magnetic vanadium (V) doping in helimagnetic SrFeO$_{3-δ}$ (SFO) are investigated, focusing on up to 3% substitution at the Fe site. Structural analysis from X-ray diffraction (XRD) and Raman spectroscopy, supported by phonon mode calculations, reveals that pure SFO exists as a mixed tetragonal-orthorhombic phase, while V-doped samples exhibit an emerging cubic phase alongside tetragonal symmetry. Magnetic hysteresis (M-H) loops show notable ferromagnetic behavior within the antiferromagnetic matrix, persisting even at room temperature. Temperature-dependent magnetization measurements indicate a Neel temperature (TN ) shift from 70K to 55K, along with increased magnetization differences in field-cooled (FC) and zero field-cooled (ZFC) data, reflecting heightened magnetic frustration due to competing FM/AFM exchange interactions. X-ray photoelectron spectroscopy (XPS) and X-ray absorption near-edge structure (XANES) analyses reveal a rise in Fe$^{3+}$ and V$^{5+}$ states, affecting oxygen vacancy distributions and corresponding structural shifts seen in XRD and Raman results. The multivalent Fe$^{3+}$/Fe$^{4+}$ and V$^{4+}$/V$^{5+}$ states enhance double-exchange (DE) and super-exchange (SE) interactions (Fe$^{3+}$-O-Fe$^{4+}$ and Fe$^{3+}$-O-V$^{5+}$), promoting ferromagnetism. Frequency-dependent magnetization studies display a subtle susceptibility peak shift, indicating spin-glass-like behavior in V-doped samples.

cond-mat.mtrl-sci

Room temperature Multiferroicity and Magnetoelectric coupling in Ca/Mn modified BaTiO3

Materials with magnetoelectric coupling (MEC) between ferroic orders at room temperature are emerging field in modern technology and physics. BaTiO3 is a robust ferroelectric in which several doping has led to MEC. In Ca and Mn modified BaTiO3 has been study with a series of Ba(1-x)Ca(x)Ti(1-y)Mn(y)O3 (x=y= 0, 0.03, 0.06, 0.09), in this MEC was only observed in x=0.03. The structural modifications with changing substitution reveal a reduced Ti-O-Ti bond angle for this sample which is the most ferromagnetic in nature. A mixed phase of tetragonal P4mm and hexagonal P63/mmc space groups of BaTiO3 is observed in the substituted samples, with nominal contribution of the hexagonal phase for x=0.03. A valence state study using XPS and XANES reveals the presence of enhanced proportion of Mn3+ ions in the sample which support a pseudo Jahn-Teller distortion, thereby supporting the ferroelectricity for x=0.03. Direct evidences of MEC was obtained from magnetoelectric measurements. A magnetoelectric coupling coefficient, {\alpha}ME ~44 mVcm-1Oe-1 was obtained for dc magnetic field of 600 Oe and a 10Hz ac field of 40 Oe. Such MEC was not observed for higher substitution which emphasizes the sensitivity of the structural properties on substitution.

cond-mat.mtrl-sci

Spectroscopy of low-frequency noise and its temperature dependence in a superconducting qubit

We report a direct measurement of the low-frequency noise spectrum in a superconducting flux qubit. Our method uses the noise sensitivity of a free-induction Ramsey interference experiment, comprising free evolution in the presence of noise for a fixed period of time followed by single-shot qubit-state measurement. Repeating this procedure enables Fourier-transform noise spectroscopy with access to frequencies up to the achievable repetition rate, a regime relevant to dephasing in ensemble-averaged time-domain measurements such as Ramsey interferometry. Rotating the qubit's quantization axis allows us to measure two types of noise: effective flux noise and effective critical-current or charge noise. For both noise sources, we observe that the very same 1/f-type power laws measured at considerably higher frequencies (0.2-20 MHz) are consistent with the noise in the 0.01-100-Hz range measured here. We find no evidence of temperature dependence of the noises over 65-200 mK, and also no evidence of time-domain correlations between the two noises. These methods and results are pertinent to the dephasing of all superconducting qubits.

cond-mat.supr-con

Driven dynamics and rotary echo of a qubit tunably coupled to a harmonic oscillator

We have investigated the driven dynamics of a superconducting flux qubit that is tunably coupled to a microwave resonator. We find that the qubit experiences an oscillating field mediated by off-resonant driving of the resonator, leading to strong modifications of the qubit Rabi frequency. This opens an additional noise channel, and we find that low-frequency noise in the coupling parameter causes a reduction of the coherence time during driven evolution. The noise can be mitigated with the rotary-echo pulse sequence, which, for driven systems, is analogous to the Hahn-echo sequence.

cond-mat.supr-con

Dynamical decoupling and noise spectroscopy with a superconducting flux qubit

The characterization and mitigation of decoherence in natural and artificial two-level systems (qubits) is fundamental to quantum information science and its applications. Decoherence of a quantum superposition state arises from the interaction between the constituent system and the uncontrolled degrees of freedom in its environment. Within the standard Bloch-Redfield picture of two-level system dynamics, qubit decoherence is characterized by two rates: a longitudinal relaxation rate Gamma1 due to the exchange of energy with the environment, and a transverse relaxation rate Gamma2 = Gamma1/2 + Gamma_phi which contains the pure dephasing rate Gamma_phi. Irreversible energy relaxation can only be mitigated by reducing the amount of environmental noise, reducing the qubit's internal sensitivity to that noise, or through multi-qubit encoding and error correction protocols (which already presume ultra-low error rates). In contrast, dephasing is in principle reversible and can be refocused dynamically through the application of coherent control pulse methods. In this work we demonstrate how dynamical-decoupling techniques can moderate the dephasing effects of low-frequency noise on a superconducting qubit with energy-relaxation time T1 = 1/Gamma1 = 12 us. Using the CPMG sequence with up to 200 pi-pulses, we demonstrate a 50-fold improvement in the transverse relaxation time T2 over its baseline value. We observe relaxation-limited times T2(CPMG) = 23 us = 2 T1 resulting from CPMG-mediated Gaussian pure-dephasing times in apparent excess of 100 us. We leverage the filtering property of this sequence in conjunction with Rabi and energy relaxation measurements to facilitate the spectroscopy and reconstruction of the environmental noise power spectral density.

cond-mat.supr-con