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Bourret, Edith

Publications and source records attributed to Bourret, Edith.

Local p‐ and n‐Type Doping of an Oxide Semiconductor via Electric‐Field‐Driven Defect Migration

Layered oxides exhibit high ionic mobility and chemical flexibility, attracting interest as cathode materials for lithium-ion batteries and the pairing of hydrogen production and carbon capture. Recently, layered oxides emerged as highly tunable semiconductors. For example, by introducing anti-Frenkel defects, the electronic hopping conductance in hexagonal manganites is increased locally by orders of magnitude. Here, local acceptor and donor doping in Er(Mn,Ti)O3 is demonstrated, facilitated by the controlled splitting of anti-Frenkel defects under applied d.c. voltage. By combining density functional theory calculations, scanning probe microscopy, atom probe tomography, and scanning transmission electron microscopy, it is shown that the oxygen defects can readily be moved through the layered crystal structure, leading to nano-sized interstitial-rich (p-type) and vacancy-rich (n-type) regions. The resulting pattern is comparable to dipolar npn-junctions and stable on the timescale of days. These findings reveal the possibility of temporarily functionalizing oxide semiconductors at the nanoscale, giving additional opportunities for the field of oxide electronics and the development of transient electronics in general.

He, Jiali↗

Probing the optical properties and toxicological profile of zinc tungstate nanorods

Zinc tungstate is a semiconductor known for its favorable photocatalytic, photoluminescence, and scintillation properties, coupled with its relatively low cost, reduced toxicity, and high stability in biological and catalytic environments. In particular, zinc tungstate evinces scintillation properties, namely the ability to emit visible light upon absorption of energetic radiation such as x rays, which has led to applications not only as radiation detectors but also for biomedical applications involving the delivery of optical light to deep tissue, such as photodynamic therapy and optogenetics. Here, we report on the synthesis of zinc tungstate nanorods generated via an optimized but facile method, which allows for synthetic control over the aspect ratio of the as-synthesized anisotropic motifs via rational variation of the solution pH. Additionally, we investigate the effect of aspect ratio on their resulting photoluminescent and radioluminescent properties. We further demonstrate the potential of these zinc tungstate nanorods for biomedical applications, such as photodynamic therapy for cancer treatment, by analyzing their toxicological profile within cell lines and neurons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Imaging and structure analysis of ferroelectric domains, domain walls, and vortices by scanning electron diffraction

Direct electron detectors in scanning transmission electron microscopy give unprecedented possibilities for structure analysis at the nanoscale. In electronic and quantum materials, this new capability gives access to, for example, emergent chiral structures and symmetry-breaking distortions that underpin functional properties. Quantifying nanoscale structural features with statistical significance, however, is complicated by the subtleties of dynamic diffraction and coexisting contrast mechanisms, which often results in a low signal-to-noise ratio and the superposition of multiple signals that are challenging to deconvolute. Here we apply scanning electron diffraction to explore local polar distortions in the uniaxial ferroelectric Er(Mn,Ti)O 3 . Using a custom-designed convolutional autoencoder with bespoke regularization, we demonstrate that subtle variations in the scattering signatures of ferroelectric domains, domain walls, and vortex textures can readily be disentangled with statistical significance and separated from extrinsic contributions due to, e.g., variations in specimen thickness or bending. The work demonstrates a pathway to quantitatively measure symmetry-breaking distortions across large areas, mapping structural changes at interfaces and topological structures with nanoscale spatial resolution.

36 MATERIALS SCIENCE↗

Triple-mode detector for fast neutrons, slow neutrons, and gamma ray spectroscopy

This disclosure provides systems, methods, and apparatus related to neutron detection and gamma ray detection. In one aspect, a detector comprises a scintillator structure that comprises an organic scintillator and an inorganic scintillator. The organic scintillator is in the form of one or more elements of a specified length. The inorganic scintillator is in the form of one or more elements of the specified length. First ends of the one or more organic scintillator elements and first ends of the one or more inorganic scintillator elements define a first surface. Second ends of the one or more organic scintillator elements and second ends of the one or more inorganic scintillator elements define a second surface.

Derenzo, Stephen↗

Investigation of the photoluminescent properties, scintillation behaviour and toxicological profile of various magnesium tungstate nanoscale motifs

We have synthesized several morphologies and crystal structures of MgWO 4 using a one-pot hydrothermal method, producing not only monoclinic stars and large nanoparticles but also triclinic wool balls and sub-10 nm nanoparticles. Herein we describe the importance of reaction parameters in demonstrating morphology control of as-prepared MgWO 4 . Moreover, we correlate structure and composition with the resulting photoluminescence and radioluminescence properties. Specifically, triclinic-phase samples yielded a photoluminescence emission of 421 nm, whereas monoclinic-phase materials gave rise to an emission maximum of 515 nm. The corresponding radioluminescence data were characterized by a broad emission peak, located at 500 nm for all samples. Annealing the wool balls and sub-10 nm particles to transform the crystal structure from a triclinic to a monoclinic phase yielded a radioluminescence (RL) emission signal that was two orders of magnitude greater than that of their unannealed counterparts. Finally, to confirm the practical utility of these materials for biomedical applications, a series of sub-10 nm particles, including as-prepared and annealed samples, were functionalized with biocompatible PEG molecules, and subsequently were found to be readily taken up by various cell lines as well as primary cultured hippocampal neurons with low levels of toxicity, thereby highlighting for the first time the potential of this particular class of metal oxides as viable and readily generated platforms for a range of biomedical applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

The Third Dimension of Ferroelectric Domain Walls

Abstract Ferroelectric domain walls are quasi‐2D systems that show great promise for the development of nonvolatile memory, memristor technology, and electronic components with ultrasmall feature size. Electric fields, for example, can change the domain wall orientation relative to the spontaneous polarization and switch between resistive and conductive states, controlling the electrical current. Being embedded in a 3D material, however, the domain walls are not perfectly flat and can form networks, which leads to complex physical structures. In this work, the importance of the nanoscale structure for the emergent transport properties is demonstrated, studying electronic conduction in the 3D network of neutral and charged domain walls in ErMnO 3 . By combining tomographic microscopy techniques and finite element modeling, the contribution of domain walls within the bulk is clarified and the significance of curvature effects for the local conduction is shown down to the nanoscale. The findings provide insights into the propagation of electrical currents in domain wall networks, reveal additional degrees of freedom for their control, and provide quantitative guidelines for the design of domain‐wall‐based technology.

36 MATERIALS SCIENCE↗

Charged Ferroelectric Domain Walls for Deterministic ac Signal Control at the Nanoscale

The direct current (dc) conductivity and emergent functionalities at ferroelectric domain walls are closely linked to the local polarization charges. Depending on the charge state, the walls can exhibit unusual dc conduction ranging from insulating to metallic-like, which is leveraged in domain-wall-based memory, multilevel data storage, and synaptic devices. In contrast to the functional dc behaviors at charged walls, their response to alternating currents (ac) remains to be resolved. Here, we reveal ac characteristics at positively and negatively charged walls in ErMnO 3 , distinctly different from the response of the surrounding domains. By combining voltage-dependent spectroscopic measurements on macroscopic and local scales, we demonstrate a pronounced nonlinear response at the electrode-wall junction, which correlates with the domain-wall charge state. The dependence on the ac drive voltage enables reversible switching between uni- and bipolar output signals, providing conceptually new opportunities for the application of charged walls as functional nanoelements in ac circuitry.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Investigation of the competition between Tl + and Ce 3+ scintillation in Tl2LiYCl6:Ce, an elpasolite scintillator

Li-containing elpasolite scintillators are currently investigated for their ability to detect both thermal neutrons and gamma photons with a single inorganic crystal. The scintillation is typically triggered by using an activator such as Ce. However, when Tl, also a luminescent ion, is present in the matrix, competition between the two centers Tl and Ce can occur. In this study, we are using Ce doped Tl 2 LiYCl 6 to investigate this competition. To this end, the Ce (which substitutes Y) concentration is varied from 0 to 1 in the Tl 2 LiY 1-x CexCl 6 composition. In the low concentration range in which Ce remains a dopant, the photo- and radioluminescence spectra show that the scintillation of Tl 2 LiYCl 6 :Ce is mostly dominated by recombination on intrinsic luminescent centers. For cerium concentrations higher than x = 0.02, very different emissions can be easily distinguished from the photo- and radioluminescence of undoped and low Ce doped Tl 2 LiYCl 6 crystals. These emissions are attributed to the formation of a second phase Tl 2 CeCl 5 , identified by X-ray diffraction. We conclude that the intrinsic luminescence related to Tl dominates the scintillation in the range of concentration for which Ce does substitute on the Y-site.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗