arXiv subjects

Judith L. MacManus-Driscoll

Publications and source records attributed to Judith L. MacManus-Driscoll.

17 recordsLinked to original sources

arXiv2026

Computing at the Edge Enabled by Indoor Photovoltaics and Ferroelectrics

The exponential, pervasive rise of artificial intelligence (AI), hosted in large data centres, will test the limits of the underpinning infrastructure, including electricity and water supplies, which are becoming increasingly precious resources. Rather than performing all AI computations in centralized servers, for many functionalities, these can be performed locally across a network of billions of small, autonomous nodes, saving substantial energy costs associated with communication. This alternative paradigm is known as edge computing, or distributed intelligence (DI), but has been held back by the lack of availability of reliable local energy supplies matching the energy requirements of the computational infrastructure. Opportunities to address this challenge are emerging with rapid advances in high-performance indoor photovoltaics (IPVs) for local energy harvesting, as well as reductions in computational cost through neuromorphic or in-memory computing devices. In this perspective, we discuss the requirements of IPVs for DI, the extent to which emerging materials fulfil these requirements, and how current gaps could be addressed. We make the case that (anti)ferroelectric materials can surpass bottlenecks for both electrostatic energy storage and low-power in-memory neuromorphic computing. The core theme of this perspective is that co-creation between energy harvesting, storage and computing is essential for making DI a reliable and more sustainable alternative to centralized AI.

cond-mat.mtrl-sci↗

arXiv2022

Ferroelectricity and resistive switching in BaTiO$_3$ thin films with liquid electrolyte top contact for bioelectronic devices

We investigate ferroelectric- and resistive switching behavior in 18-nm-thick epitaxial BaTiO$_3$ (BTO) films in a model electrolyte-ferroelectric-semiconductor (EFS) configuration. The system is explored for its potential as a ferroelectric microelectrode in bioelectronics. The BTO films are grown by pulsed laser deposition (PLD) on semiconducting Nb-doped (0.5 wt\%) SrTiO$_{3}$ (Nb:STO) single crystal substrates. The ferroelectric properties of the bare BTO films are demonstrated by piezoresponse force microscopy (PFM) measurements. Cyclic voltammetry (CV) measurements in EFS configuration, with phosphate buffered saline (PBS) acting as the liquid electrolyte top contact, indicate characteristic ferroelectric switching peaks in the bipolar current-voltage loop. The ferroelectric nature of the observed switching peaks is confirmed by analyzing the current response of the EFS devices to unipolar voltage signals. Moreover, electrochemical impedance spectroscopy (EIS) measurements indicate bipolar resisitive switching behavior of the EFS devices, which is controlled by the remanent polarization state of the BTO layer. Our results represent a constitutive step towards the realization of neuroprosthetic implants and hybrid neurocomputational systems based on ferroelectric microelectrodes.

physics.app-ph↗

arXiv2022

Local Symmetry Breaking Drives Picosecond Spin Domain Formation in Polycrystalline Semiconducting Films

Photoinduced spin-charge interconversion in semiconductors with spin-orbit coupling could provide a route to optically addressable spintronics without the use of external magnetic fields. A central question is whether the resulting spin-associated charge currents are robust to structural disorder, which is inherent to polycrystalline semiconductors that are desirable for device applications. Using femtosecond circular polarization-resolved pump-probe microscopy on polycrystalline halide perovskite thin films, we observe the photoinduced ultrafast formation of spin-polarized positive and, unexpectedly, negative spin domains on the micron scale formed through lateral currents. Further, the polarization of these domains and lateral transport direction is switched upon switching the polarization of the pump helicity. Micron scale variations in the intensity of optical second-harmonic generation and vertical piezoresponse suggest that the spin domain formation is driven by the presence of strong local inversion symmetry breaking via inter-grain structural disorder. We propose that this leads to spatially varying Rashba-like spin textures that drive spin-momentum locked currents, leading to local spin accumulation. Our results establish ultrafast spin domain formation in polycrystalline semiconductors as a new optically addressable platform for nanoscale spin-device physics.

cond-mat.mes-hall↗

arXiv2021

Materials Informatics Reveals Unexplored Structure Space in Cuprate Superconductors

High-temperature superconducting cuprates have the potential to be transformative in a wide range of energy applications. In this work we analyse the corpus of historical data about cuprates using materials informatics and re-examine how their structures are related to their critical temperatures (Tc). The available data is highly clustered and no single database contains all the features of interest to properly examine trends. To work around these issues we employ a linear calibration approach that allows us to utilise multiple data sources -- combining fine resolution data for which the Tc is unknown with coarse resolution data where it is known. The hybrid data set constructed enables us to explore the trends in Tc with the apical and in-plane copper-oxygen distances. We show that large regions of the materials space have yet to be explored and highlight how novel experiments relying on nano-engineering of the crystal structure may enable us to explore such new regions. Based on the trends identified we propose that single layer Bi-based cuprates are good candidate systems for such experiments.

cond-mat.supr-con↗

arXiv2021

Tuneable vertical hysteresis loop shift in Ni80Fe20/SrRuO3 heterostructures

A novel vertical hysteresis loop shift is observed for a bilayer thin film of Ni80Fe20/SrRuO3 (1:2 thickness ratio) on SrTiO3 substrate, after field cooled through the Curie temperature ~125 K of SrRuO3, whereas no shift is found for zero field cooled measurement. The vertical shift is noticed below ~125 K which increases with decreasing temperature and reaches a maximum of 33% at 2 K. The vertical shift is modelled closely using micromagnetic simulations. It is shown that the amount of vertical shift depends on the competition between the relative thicknesses and the anisotropies of the two films governed by Spring Thickness law and Imperial Law, respectively. We propose a generalized model of vertical shift which is applicable for other material systems, and hence could be informative for use of vertical shift in future spintronic devices.

cond-mat.mtrl-sci↗

arXiv2021

Route to High-Performance Micro-solid Oxide Fuel Cells on Metallic Substrates

Micro-solid oxide fuel cells based on thin films have strong potential for use in portable power devices. However, devices based on silicon substrates typically involve thin-film metallic electrodes which are unstable at high temperatures. Devices based on bulk metal substrates overcome these limitations, though performance is hindered by the challenge of growing state-of-the-art epitaxial materials on metals. Here, we demonstrate for the first time the growth of epitaxial cathode materials on metal substrates (stainless steel) commercially supplied with epitaxial electrolyte layers (1.5 {um (Y2O3)0.15(ZrO2)0.85 (YSZ) + 50 nm CeO2). We create epitaxial mesoporous cathodes of (La0.60Sr0.40)0.95Co0.20Fe0.80O3 (LSCF) on the substrate by growing LSCF/MgO vertically aligned nanocomposite films by pulsed laser deposition, followed by selectively etching out the MgO. To enable valid comparison with the literature, the cathodes are also grown on single-crystal substrates, confirming state-of-the-art performance with an area specific resistance of 100ohmegacm2 at 500dC and activation energy down to 0.97 eV. The work marks an important step toward the commercialization of high-performance micro-solid oxide fuel cells for portable power applications.

physics.app-ph↗

arXiv2020

Identifying and reducing interfacial losses to enhance color-pure electroluminescence in blue-emitting perovskite nanoplatelet light-emitting diodes

Perovskite nanoplatelets (NPls) hold great promise for light-emitting applications, having achieved high photoluminescence quantum efficiencies (PLQEs) approaching unity in the blue wavelength range, where other metal-halide perovskites have typically been ineffective. However, the external quantum efficiency (EQE) of blue-emitting NPl light-emitting diodes (LEDs) have only reached 0.12%, with typical values well below 0.1%. In this work, we show that the performance of NPl LEDs is primarily hindered by a poor electronic interface between the emitter and hole-injector. Through Kelvin Probe and X-ray photoemission spectroscopy measurements, we reveal that the NPls have remarkably deep ionization potentials (>=6.5 eV), leading to large barriers for hole injection, as well as substantial non-radiative decay at the interface between the emitter and hole-injector. We find that an effective way to reduce these non-radiative losses is by using poly(triarylamine) interlayers. This results in an increase in the EQE of our blue LEDs emitting at 464 nm wavelength to 0.3%. We find that our results can be generalized to thicker sky-blue-emitting NPls, where we increase the EQE to 0.55% using the poly(triarylamine) interlayer. Our work also identifies the key challenges for further efficiency increases.

physics.optics↗

arXiv2020

Evidence of Rotational Fröhlich Coupling in Polaronic Trions

Electrons commonly couple through Fröhlich interactions with longitudinal optical phonons to form polarons. However, trions possess a finite angular momentum and should therefore couple instead to rotational optical phonons. This creates a polaronic trion whose binding energy is determined by the crystallographic orientation of the lattice. Here, we demonstrate theoretically within the Fröhlich approach and experimentally by photoluminescence emission that the bare trion binding energy (20 meV) is significantly enhanced by the phonons at the interface between the two-dimensional semiconductor MoS$_2$ and the bulk transition metal oxide SrTiO$_3$. The low-temperature {binding energy} changes from 60 meV in [001]-oriented substrates to 90 meV for [111] orientation, as a result of the counter-intuitive interplay between the rotational axis of the MoS$_2$ trion and that of the SrTiO$_3$ phonon mode.

cond-mat.mes-hall↗

arXiv2020

Printed high-mobility p-type buffer layers on perovskite photovoltaics for efficient semi-transparent devices

Perovskite solar cells (PSCs) with transparent electrodes can be integrated with existing solar panels in tandem configurations to increase the power conversion efficiency. A critical layer in semi-transparent PSCs is the inorganic buffer layer, which protects the PSC against damage when the transparent electrode is sputtered on top. The development of n-i-p structured semi-transparent PSCs has been hampered by the lack of suitable p-type buffer layers. In this work we develop a p-type CuOx buffer layer, which can be grown uniformly over the perovskite device without damaging the perovskite or organic charge transport layers, can be grown using industrially scalable techniques and has high hole mobility (4.3 +/- 2 cm2 V-1 s-1), high transmittance (>95%), and a suitable ionisation potential for hole extraction (5.3 +/- 0.2 eV). Semi-transparent PSCs with efficiencies up to 16.7% are achieved using the CuOx buffer layer. Our work demonstrates a new approach to integrate PSCs into tandem configurations, as well as enable the development of other devices that need high quality p-type layers.

physics.app-ph↗

arXiv2020

Influence of Atomic Roughness at The Uncompensated Fe/CoO (111) Interface on Exchange Bias Effect

The effect of interface roughness of ferromagnetic and antiferromagnetic layers on exchange bias is still not well understood. In this report we have investigated the effect of surface roughness in (111)-oriented antiferromagnetic CoO films on exchange bias with ferromagnetic Fe grown on top. The surface roughness is controlled at the atomic scale, over a range below ~ 0.35 nm, by varying layer thickness of the CoO films. It is observed that both exchange bias field ($H_{E}$) and coercivity ($H_{C}$) extensively depend on the atomic scale roughness of the CoO (111) at the interface with Fe film. An opposite dependence of $H_{E}$ and $H_{C}$ on interface roughness was found, which was ascribed to partially compensated spin states induced by the atomic roughness at the fully uncompensated CoO (111) surfaces and was corroborated using the Monte Carlo simulations. Moreover, the onset temperature for $H_{C}$ is found to be up to ~ 80 K below the blocking temperature ($T_{B}$) and the temperature dependence of $H_{C}$ follows the power law with a critical exponent equal to one, which indicates that, in this system, $H_{C}$ is more of an interface-related property than $H_{E}$.

cond-mat.mtrl-sci↗

arXiv2019

Strong Performance Enhancement in Lead-Halide Perovskite Solar Cells through Rapid, Atmospheric Deposition of n-type Buffer Layer Oxides

Thin (approximately 10 nm) oxide buffer layers grown over lead-halide perovskite device stacks are critical for protecting the perovskite against mechanical and environmental damage. However, the limited perovskite stability restricts the processing methods and temperatures (<=110 C) that can be used to deposit the oxide overlayers, with the latter limiting the electronic properties of the oxides achievable. In this work, we demonstrate an alternative to existing methods that can grow pinhole-free TiOx (x = 2.00+/-0.05) films with the requisite thickness in <1 min without vacuum. This technique is atmospheric pressure chemical vapor deposition (AP-CVD). The rapid but soft deposition enables growth temperatures of >=180 °C to be used to coat the perovskite. This is >=70 °C higher than achievable by current methods and results in more conductive TiOx films, boosting solar cell efficiencies by >2%. Likewise, when AP-CVD SnOx (x ~ 2) is grown on perovskites, there is also minimal damage to the perovskite beneath. The SnOx layer is pinhole-free and conformal, which reduces shunting in devices, and increases steady-state efficiencies from 16.5% (no SnOx) to 19.4% (60 nm SnOx), with fill factors reaching 84%. This work shows AP-CVD to be a versatile technique for growing oxides on thermally-sensitive materials.

physics.app-ph↗

arXiv2019

Topological semimetallic phase in PbO$_2$ promoted by temperature

Materials exhibiting topological order host exotic phenomena that could form the basis for novel developments in areas ranging from low-power electronics to quantum computers. The past decade has witnessed multiple experimental realizations and thousands of predictions of topological materials. However, it has been determined that increasing temperature destroys topological order, restricting many topological materials to very low temperatures and thus hampering practical applications. Here, we propose a material realization of temperature promoted topological order. We show that a semiconducting oxide that has been widely used in lead-acid batteries, $β$-PbO$_2$, hosts a topological semimetallic phase driven by both thermal expansion and electron-phonon coupling upon increasing temperature. We identify the interplay between the quasi-two-dimensional nature of the charge distribution of the valence band with the three-dimensional nature of the charge distribution of the conduction band as the microscopic mechanism driving this unconventional temperature dependence. Thus, we propose a general principle to search for and design novel topological materials whose topological order is stabilized by increasing temperature. This provides a clear roadmap for taking topological materials from the laboratory to technological devices.

cond-mat.mtrl-sci↗

arXiv2018

Origin of Improved Photoelectrochemical Water Splitting in Mixed Perovskite Oxides

Owing to the versatility in their chemical and physical properties, transition metal perovskite oxides have emerged as a new category of highly efficient photocatalysts for photoelectrochemical water splitting. Here, to understand the underlying mechanism for the enhanced photoelectrochemical water splitting in mixed perovskites, we explore ideal epitaxial thin films of the BiFeO3-SrTiO3 system. The electronic struture and carrier dynamics are determined from both experiment and density-functional theory calculations. The intrinsic phenomena are measured in this ideal sytem, contrasting to commonly studied polycrstalline solid solutions where extrinsic structural features obscure the intrinsic phenomena. We determined that when SrTiO3 is added to BiFeO3 the conduction band minimum position is raised and an exponential tail of trap states from hybridized Ti 3d and Fe 3d orbitals emerges near the conduction band edge. The presence of these trap states strongly suppresses the fast electron-hole recombination and improves the photocurrent density in the visible-light region, up to 16 times at 0 VRHE compared to the pure end member compositions. Our work provides a new design approach for optimising the photoelectrochemical performance in mixed perovksite oxides.

cond-mat.mtrl-sci↗

arXiv2017

Insulating-to-Conducting Behavior and Band Profile Across the La0.9Ba0.1MnO3/Nb:SrTiO3 Epitaxial Interface

La0.9Ba0.1MnO3 is a ferromagnetic insulator in its bulk form, but exhibits metallicity in thin film form. It has a wide potential in a range of spintronic-related applications, and hence it is critical to understand thickness-dependent electronic structure in thin films as well as substrate/film interface effects. Here, using electrical and in-situ photoemission spectroscopy measurements, we report the electronic structure and interface band profile of high-quality layer-by-layer-grown La0.9Ba0.1MnO3 on single crystal Nb:SrTiO3 substrates. A transition from insulating-to-conducting was observed with increasing La0.9Ba0.1MnO3 thickness, which was explained by the determined interface band diagram of La0.9Ba0.1MnO3/Nb: SrTiO3, where a type II heterojunction was formed.

cond-mat.str-el↗

arXiv2011

Depairing critical current achieved in superconducting thin films with through-thickness arrays of artificial pinning centers

Large area arrays of through-thickness nanoscale pores have been milled into superconducting Nb thin films via a process utilizing anodized aluminum oxide thin film templates. These pores act as artificial flux pinning centers, increasing the superconducting critical current, Jc, of the Nb films. By optimizing the process conditions including anodization time, pore size and milling time, Jc values approaching and in some cases matching the Ginzburg-Landau depairing current of 30 MA/cm^2 at 5 K have been achieved - a Jc enhancement over as-deposited films of more than 50 times. In the field dependence of Jc, a matching field corresponding to the areal pore density has also been clearly observed. The effect of back-filling the pores with magnetic material has then been investigated. While back-filling with Co has been successfully achieved, the effect of the magnetic material on Jc has been found to be largely detrimental compared to voids, although a distinct influence of the magnetic material in producing a hysteretic Jc versus applied field behavior has been observed. This behavior has been tested for compatibility with currently proposed models of magnetic pinning and found to be most closely explained by a model describing the magnetic attraction between the flux vortices and the magnetic inclusions.

cond-mat.supr-con↗

arXiv2009

Superconductor-ferromagnet nanocomposites created by co-deposition of niobium and dysprosium

We have created superconductor-ferromagnet composite films in order to test the enhancement of critical current density, Jc, due to magnetic pinning. We co-sputter the type-II superconductor niobium (Nb) and the low-temperature ferromagnet dysprosium (Dy) onto a heated substrate; the immiscibility of the two materials leads to a phase-separated composite of magnetic regions within a superconducting matrix. Over a range of compositions and substrate temperatures, we achieve phase separation on scales from 5 nm to 1 micron. The composite films exhibit simultaneous superconductivity and ferromagnetism. Transport measurements show that while the self-field Jc is reduced in the composites, the in-field Jc is greatly enhanced up to the 3 T saturation field of Dy. In one instance, the phase separation orders into stripes, leading to in-plane anisotropy in Jc.

cond-mat.supr-con↗

arXiv2006

Alignment of Carbon Nanotube Additives for Improved Performance of Magnesium Diboride Superconductors

The rapid progress on MgB2 superconductor since its discovery[1] has made this material a strong competitor to low and high temperature superconductors (HTS) for applications with a great potential to catch the niche market such as in magnetic resonant imaging (MRI). Thanks to the lack of weak links and the two-gap superconductivity of MgB2 [2,3] a number of additives have been successfully used to enhance the critical current density, Jc and the upper critical field, Hc2.[4-12] Carbon nanotubes (CNTs) have unusually electrical, mechanical and thermal properties[13-16] and hence is an ideal component to fabricate composites for improving their performance. To take advantages of the extraordinary properties of CNTs it is important to align CNTs in the composites. Here we report a method of alignment of CNTs in the CNT/MgB2 superconductor composite wires through a readily scalable drawing technique. The aligned CNT doped MgB2 wires show an enhancement in magnetic Jc(H) by more than an order of magnitude in high magnetic fields, compared to the undoped ones. The CNTs have also significantly enhanced the heat transfer and dissipation. CNTs have been used mainly in structural materials, but here the advantage of their use in functional composites is shown and this has wider ramifications for other functional materials.

cond-mat.supr-con↗