arXiv subjects

Shaul Aloni

Publications and source records attributed to Shaul Aloni.

At least 19 recordsLinked to original sources

arXiv2024

Observation of Interface Piezoelectricity in Superconducting Devices on Silicon

The evolution of superconducting quantum processors is driven by the need to reduce errors and scale for fault-tolerant computation. Reducing physical qubit error rates requires further advances in the microscopic modeling and control of decoherence mechanisms in superconducting qubits. Piezoelectric interactions contribute to decoherence by mediating energy exchange between microwave photons and acoustic phonons. Centrosymmetric materials like silicon and sapphire do not display piezoelectricity and are the preferred substrates for superconducting qubits. However, the broken centrosymmetry at material interfaces may lead to piezoelectric losses in qubits. While this loss mechanism was predicted two decades ago, interface piezoelectricity has not been experimentally observed in superconducting devices. Here, we report the observation of interface piezoelectricity at an aluminum-silicon junction and show that it constitutes an important loss channel for superconducting devices. We fabricate aluminum interdigital surface acoustic wave transducers on silicon and demonstrate piezoelectric transduction from room temperature to millikelvin temperatures. We find an effective electromechanical coupling factor of $K^2\approx 2 \times 10^{-5}\%$ comparable to weakly piezoelectric substrates. We model the impact of the measured interface piezoelectric response on superconducting qubits and find that the piezoelectric surface loss channel limits qubit quality factors to $Q\sim10^4-10^8$ for designs with different surface participation ratios and electromechanical mode matching. These results identify electromechanical surface losses as a significant dissipation channel for superconducting qubits, and show the need for heterostructure and phononic engineering to minimize errors in next-generation superconducting qubits.

quant-ph↗

arXiv2024

Optical and spin properties of nitrogen vacancy centers formed along the tracks of high energy heavy ions

Exposure of matter to high energy, heavy ions induces defects along the trajectories of the ions through electronic and nuclear energy loss processes. Defects, including color centers, can recombine or form along latent damage tracks in many materials, such as insulators and semiconductors. Latent tracks in diamond were only recently observed. Here, we report on color center formation in diamond along the latent tracks of 1 GeV gold and uranium ions. Using depth-resolved photoluminescence, we observe direct formation of single vacancy related color centers (GR1-centers) along the ion tracks. Mobile vacancies can form NV-centers with native nitrogen atoms during thermal annealing. Molecular dynamics simulations show that isolated vacancies and vacancy clusters form through electronic stopping processes, leading to color center formation along ion trajectories from the sample surface to a depth of about 25 microns. We further report on the creation of individually isolated quasi-1D chains of NV-centers by using 1 GeV Au ions with a dilute fluence. The individual 1D NV-chains appear as isolated bright luminescence strings and present competitive electron spin properties compared to a background of NV-centers. Such spin textures can be explored as building blocks for applications in quantum information processing and quantum sensing.

quant-ph↗

arXiv2023

Elucidating the Mechanism of Large Phosphate Molecule Intercalation Through Graphene Heterointerfaces

Intercalation is a process of inserting chemical species into the heterointerfaces of two-dimensional (2D) layered materials. While much research has focused on intercalating metals and small gas molecules into graphene, the intercalation of larger molecules through the basal plane of graphene remains highly unexplored. In this work, we present a new mechanism for intercalating large molecules through monolayer graphene to form confined oxide materials at the graphene-substrate heterointerface. We investigate the intercalation of phosphorus pentoxide (P2O5) molecules directly from the vapor phase and confirm the formation of confined P2O5 at the graphene heterointerface using various techniques. Density functional theory (DFT) corroborate the experimental results and reveal the intercalation mechanism, whereby P2O5 dissociates into small fragments catalyzed by defects in the graphene that then permeates through lattice defects and reacts at the heterointerface to form P2O5. This process can also be used to form new confined metal phosphates (e.g., 2D InPO4). While the focus of this study is on P2O5 intercalation, the possibility of intercalation from pre-dissociated molecules catalyzed by defects in graphene may exist for other types of molecules as well. This study is a significant milestone in advancing our understanding of intercalation routes of large molecules via the basal plane of graphene, as well as heterointerface chemical reactions leading to the formation of distinctive confined complex oxide compounds.

cond-mat.mtrl-sci↗

arXiv2022

Carrier and Phonon Dynamics in Multilayer WSe2 captured by Extreme Ultraviolet Transient Absorption Spectroscopy

Carrier and phonon dynamics in a multilayer WSe2 film are captured by extreme ultraviolet (XUV) transient absorption (TA) spectroscopy at the W N6,7, W O2,3, and Se M4,5 edges (30-60 eV). After the broadband optical pump pulse, the XUV probe directly reports on occupations of optically excited holes and phonon-induced band renormalizations. By comparing with density functional theory calculations, XUV transient absorption due to holes are identified below the W O3 edge whereas signals at the Se M4,5 edges are dominated by phonon dynamics. Therein, 0.4 ps hole relaxation time, 1.5 ps carrier recombination time, and 1.7 ps phonon heating time are extracted. The acquisition of hole and phonon-induced signals in a single experiment can facilitate the investigation of the correlations between electron and phonon dynamics. Furthermore, the simultaneous observation of signals from different elements can be further extended to explore photochemical processes in multilayers and alloys, thereby providing key information for their applications in electronics, photocatalysts, and spintronics.

cond-mat.mtrl-sci↗

arXiv2022

Vapor-liquid-solid growth of highly-mismatched semiconductor nanowires with high-fidelity van der Waals layer stacking

Nanobelts, nanoribbons and other quasi-one-dimensional nanostructures formed from layered, so-called, van der Waals semiconductors have garnered much attention due to their high-performance, tunable optoelectronic properties. For layered alloys made from the gallium monochalcogenides GaS, GaSe, and GaTe, near-continuous tuning of the energy bandgap across the full composition range has been achieved in GaSe1-xSx and GaSe1-xTex alloys. Gold-catalyzed vapor-liquid-solid (VLS) growth of these alloys yields predominantly nanobelts, nanoribbons and other nanostructures for which the fast crystal growth front consists of layer edges in contact with the catalyst. We demonstrate that in the S-rich, GaS1-xTex system, unlike GaSe1-xSx and GaSe1-xTex, the Au-catalyzed VLS process yields van der Waals nanowires for which the fast growth direction is normal to the layers. The high mismatch between S and Te leads to extraordinary bowing of the GaS1-xTex alloy's energy bandgap, decreasing by at least 0.6 eV for x as small as 0.03. Calculations using density functional theory confirm the significant decrease in bandgap in S-rich GaS1-xTex. The nanowires can exceed fifty micrometers in length, consisting of tens of thousands of van der Waals-bonded layers with triangular or hexagonal cross-sections of uniform dimensions along the length of the nanowire. We propose that the low solubility of Te in GaS results in an enhancement in Te coverage around the Au catalyst-nanowire interface, confining the catalyst to the chalcogen-terminated basal plane (rather than the edges) and thereby enabling layer-by-layer, c-axis growth.

cond-mat.mtrl-sci↗

arXiv2022

Hard ferromagnetism down to the thinnest limit of iron-intercalated tantalum disulfide

Two-dimensional (2D) magnetic crystals hold promise for miniaturized and ultralow power electronic devices that exploit spin manipulation. In these materials, large, controllable magnetocrystalline anisotropy is a prerequisite for the stabilization and manipulation of long-range magnetic order. In known 2D magnetic crystals, relatively weak magnetocrystalline anisotropy results in typically soft ferromagnetism. Here, we demonstrate that ferromagnetic order persists down to the thinnest limit of Fe$_x$TaS$_2$ (Fe-intercalated bilayer 2H-TaS$_2$) with giant coercivities up to 3 tesla. We prepare Fe-intercalated TaS$_2$ by chemical intercalation of van der Waals layered 2H-TaS$_2$ crystals and perform variable-temperature quantum transport, transmission electron microscopy, and confocal Raman spectroscopy measurements to shed new light on the coupled effects of dimensionality, degree of intercalation, and intercalant order/disorder on the hard ferromagnetic behavior of Fe$_x$TaS$_2$. More generally, we show that chemical intercalation gives access to a rich synthetic parameter space for low-dimensional magnets, in which magnetic properties can be tailored by the choice of the host material and intercalant identity/amount, in addition to the manifold distinctive degrees of freedom available in atomically thin, van der Waals crystals.

cond-mat.mtrl-sci↗

arXiv2021

Tuning color centers at a twisted interface

Color center is a promising platform for quantum technologies, but their application is hindered by the typically random defect distribution and complex mesoscopic environment. Employing cathodoluminescence, we demonstrate that an ultraviolet-emitting single photon emitter can be readily activated and controlled on-demand at the twisted interface of two hexagonal boron nitride flakes. The brightness of the color center can be enhanced by two orders of magnitude by altering the twist angle. Additionally, a brightness modulation of nearly 100% of this color center is achieved by an external voltage. Our ab-initio GW calculations suggest that the emission is correlated to nitrogen vacancies and that a twist-induced moir\'e potential facilitates electron-hole recombination. This mechanism is further exploited to draw nanoscale color center patterns using electron beams.

cond-mat.mtrl-sci↗

arXiv2021

Coupled Valence Carrier and Core-Exciton Dynamics in WS$_{2}$ Probed by Few-Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy

Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2020

Localization and reduction of superconducting quantum coherent circuit losses

Quantum sensing and computation can be realized with superconducting microwave circuits. Qubits are engineered quantum systems of capacitors and inductors with non-linear Josephson junctions. They operate in the single-excitation quantum regime, photons of $27 μ$eV at 6.5 GHz. Quantum coherence is fundamentally limited by materials defects, in particular atomic-scale parasitic two-level systems (TLS) in amorphous dielectrics at circuit interfaces.[1] The electric fields driving oscillating charges in quantum circuits resonantly couple to TLS, producing phase noise and dissipation. We use coplanar niobium-on-silicon superconducting resonators to probe decoherence in quantum circuits. By selectively modifying interface dielectrics, we show that most TLS losses come from the silicon surface oxide, and most non-TLS losses are distributed throughout the niobium surface oxide. Through post-fabrication interface modification we reduced TLS losses by 85% and non-TLS losses by 72%, obtaining record single-photon resonator quality factors above 5 million and approaching a regime where non-TLS losses are dominant. [1]Müller, C., Cole, J. H. & Lisenfeld, J. Towards understanding two-level-systems in amorphous solids: insights from quantum circuits. Rep. Prog. Phys. 82, 124501 (2019)

quant-ph↗

arXiv2020

Electron Beam-Induced Nanopores in Bernal-Stacked Hexagonal Boron Nitride

Controlling the size and shape of nanopores in two-dimensional materials is a key challenge in applications such as DNA sequencing, sieving, and quantum emission in artificial atoms. We here investigate experimentally and theoretically triangular vacancies in (unconventional) Bernal-stacked AB-h-BN formed using a high-energy electron beam. Due to the geometric configuration of AB-h-BN, triangular pores in different layers are aligned, and their sizes are controlled by the duration of the electron irradiation. Interlayer covalent bonding at the vacancy edge is not favored, as opposed to what occurs in the more common AA'-stacked BN. A variety of monolayer, concentric and bilayer pores in bilayer AB-h-BN are observed in high-resolution transmission electron microscopy and characterized using ab initio simulations. Bilayer pores in AB-h-BN are commonly formed, and grow without breaking the bilayer character. Nanopores in AB-h-BN exhibit a wide range of electronic properties, ranging from half-metallic to non-magnetic and magnetic semiconducting. Therefore, because of the controllability of the pore size, the electronic structure is also highly controllable in these systems, and can potentially be tuned for particular applications.

cond-mat.mtrl-sci↗

arXiv2020

How Substitutional Point Defects in Two-Dimensional WS$_2$ Induce Charge Localization, Spin-Orbit Splitting, and Strain

Control of impurity concentrations in semiconducting materials is essential to device technology. Because of their intrinsic confinement, the properties of two-dimensional semiconductors such as transition metal dichalcogenides (TMDs) are more sensitive to defects than traditional bulk materials. The technological adoption of TMDs is dependent on the mitigation of deleterious defects and guided incorporation of functional foreign atoms. The first step towards impurity control is the identification of defects and assessment of their electronic properties. Here, we present a comprehensive study of point defects in monolayer tungsten disulfide (WS$_2$) grown by chemical vapor deposition (CVD) using scanning tunneling microscopy/spectroscopy, CO-tip noncontact atomic force microscopy, Kelvin probe force spectroscopy, density functional theory, and tight-binding calculations. We observe four different substitutional defects: chromium (Cr$_{\text{W}}$) and molybdenum (Mo$_{\text{W}}$) at a tungsten site, oxygen at sulfur sites in both bottom and top layers (O$_{\text{S}}$ top/bottom), as well as two negatively charged defects (CDs). Their electronic fingerprints unambiguously corroborate the defect assignment and reveal the presence or absence of in-gap defect states. The important role of charge localization, spin-orbit coupling, and strain for the formation of deep defect states observed at substitutional defects in WS$_2$ as reported here will guide future efforts of targeted defect engineering and doping of TMDs.

cond-mat.mes-hall↗

arXiv2020

Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides with experiment and theory

Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support from Transmission Electron Microscopy (TEM) and Scanning Tunneling Microscopy (STM) images. However, TEM imaging measurements do not provide direct access to the electronic structure of individual defects; and while Scanning Tunneling Spectroscopy (STS) is a direct probe of local electronic structure, the interpretation of the chemical nature of atomically-resolved STM images of point defects in 2D-TMDs can be ambiguous. As a result, the assignment of point defects as vacancies or substitutional atoms of different kinds in 2D-TMDs, and their influence on their electronic properties, has been inconsistent and lacks consensus. Here, we combine low-temperature non-contact atomic force microscopy (nc-AFM), STS, and state-of-the-art ab initio density functional theory (DFT) and GW calculations to determine both the structure and electronic properties of the most abundant individual chalcogen-site defects common to 2D-TMDs. Surprisingly, we observe no IGS for any of the chalcogen defects probed. Our results and analysis strongly suggest that the common chalcogen defects in our 2D-TMDs, prepared and measured in standard environments, are substitutional oxygen rather than vacancies.

cond-mat.mtrl-sci↗

arXiv2020

Characterizing Transition-Metal Dichalcogenide Thin-Films using Hyperspectral Imaging and Machine Learning

Atomically thin polycrystalline transition-metal dichalcogenides (TMDs) are relevant to both fundamental science investigation and applications. TMD thin-films present uniquely difficult challenges to effective nanoscale crystalline characterization. Here we present a method to quickly characterize the nanocrystalline grain structure and texture of monolayer WS2 films using scanning nanobeam electron diffraction coupled with multivariate statistical analysis of the resulting data. Our analysis pipeline is highly generalizable and is a useful alternative to the time consuming, complex, and system-dependent methodology traditionally used to analyze spatially resolved electron diffraction measurements.

cond-mat.mes-hall↗

arXiv2019

Tunable Electronic Structure in Gallium Chalcogenide van der Waals Compounds

Transition metal monochalcogenides comprise a class of two-dimensional materials with electronic band gaps that are highly sensitive to material thickness and chemical composition. Here, we explore the tunability of the electronic excitation spectrum in GaSe using angle-resolved photoemission spectroscopy. The electronic structure of the material is modified by $\textit{in-situ}$ potassium deposition as well as by forming GaS$_{x}$Se$_{1-x}$ alloy compounds. We find that potassium decouples the top-most tetra-layer of the GaSe unit cell, leading to a substantial change of the dispersion around the valence band maximum (VBM). The observed band dispersion of a single tetralayer is consistent with a transition from the direct gap character of the bulk to the indirect gap character expected for monolayer GaSe. Upon alloying with sulfur, we observe a phase transition from AB to $\text{AA}^{\prime}$ stacking. Alloying also results in a rigid energy shift of the VBM towards higher binding energies which correlates with a blue shift in the luminescence. The increase of the band gap upon sulfur alloying does not appear to change the dispersion or character of the VBM appreciably, implying that it is possible to engineer the gap of these materials while maintaining their salient electronic properties.

cond-mat.mes-hall↗

arXiv2019

Blue-Light-Emitting Color Centers in High-Quality Hexagonal Boron Nitride

Light emitters in wide band gap semiconductors are of great fundamental interest and have potential as optically addressable qubits. Here we describe the discovery of a new color center in high-quality hexagonal boron nitride (h-BN) with a sharp emission line at 435 nm. The emitters are activated and deactivated by electron beam irradiation and have spectral and temporal characteristics consistent with atomic color centers weakly coupled to lattice vibrations. The emitters are conspicuously absent from commercially available h-BN and are only present in ultra-high-quality h-BN grown using a high-pressure, high-temperature Ba-B-N flux/solvent, suggesting that these emitters originate from impurities or related defects specific to this unique synthetic route. Our results imply that the light emission is activated and deactivated by electron beam manipulation of the charge state of an impurity-defect complex.

cond-mat.mes-hall↗

arXiv2019

Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2

Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping in semiconductors. Specifically, deep in-gap defect states of chalcogen vacancies have been associated with intriguing phenomena in monolayer transition metal dichalcogenides (TMDs). Here, we report the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy (nc-AFM) and scanning tunneling microscopy (STM). Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states of the vacancy provide a unique fingerprint of this defect. Direct imaging of the defect orbitals by STM and state-of-the-art GW calculations reveal that the large splitting of 252 meV between these defect states is induced by spin-orbit coupling. The controllable incorporation and potential decoration of chalcogen vacancies provide a new route to tailor the optical, catalytic and magnetic properties of TMDs.

cond-mat.mtrl-sci↗

arXiv2018

Alternative Stacking Sequences in Hexagonal Boron Nitride

The relative orientation of successive sheets, i.e. the stacking sequence, in layered two-dimensional materials is central to the electronic, thermal, and mechanical properties of the material. Often different stacking sequences have comparable cohesive energy, leading to alternative stable crystal structures. Here we theoretically and experimentally explore different stacking sequences in the van der Waals bonded material hexagonal boron nitride (h-BN). We examine the total energy, electronic bandgap, and dielectric response tensor for five distinct high symmetry stacking sequences for both bulk and bilayer forms of h-BN. Two sequences, the generally assumed AA' sequence and the relatively unknown (for h-BN) AB (Bernal) sequence, are predicted to have comparably low energy. We present a scalable modified chemical vapor deposition method that produces large flakes of virtually pure AB stacked h-BN; this new material complements the generally available AA' stacked h-BN.

cond-mat.mtrl-sci↗

arXiv2018

Cathodoluminescence-based nanoscopic thermometry in a lanthanide-doped phosphor

Crucial to analyze phenomena as varied as plasmonic hot spots and the spread of cancer in living tissue, nanoscale thermometry is challenging: probes are usually larger than the sample under study, and contact techniques may alter the sample temperature itself. Many photostable nanomaterials whose luminescence is temperature-dependent, such as lanthanide-doped phosphors, have been shown to be good non-contact thermometric sensors when optically excited. Using such nanomaterials, in this work we accomplished the key milestone of enabling far-field thermometry with a spatial resolution that is not diffraction-limited at readout. We explore thermal effects on the cathodoluminescence of lanthanide-doped NaYF$_4$ nanoparticles. Whereas cathodoluminescence from such lanthanide-doped nanomaterials has been previously observed, here we use quantitative features of such emission for the first time towards an application beyond localization. We demonstrate a thermometry scheme that is based on cathodoluminescence lifetime changes as a function of temperature that achieves $\sim$ 30 mK sensitivity in sub-$μ$m nanoparticle patches. The scheme is robust against spurious effects related to electron beam radiation damage and optical alignment fluctuations. We foresee the potential of single nanoparticles, of sheets of nanoparticles, and also of thin films of lanthanide-doped NaYF$_4$ to yield temperature information via cathodoluminescence changes when in the vicinity of a sample of interest; the phosphor may even protect the sample from direct contact to damaging electron beam radiation. Cathodoluminescence-based thermometry is thus a valuable novel tool towards temperature monitoring at the nanoscale, with broad applications including heat dissipation in miniaturized electronics and biological diagnostics.

cond-mat.mes-hall↗