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A promising mechanism for achieving colossal dielectric constants is to use insulating internal barrier layers, which typically form during synthesis and then remain in the material. It has recently been shown that insulating domain walls in ferroelectrics can act as such barriers. One advantage domain walls have, in comparison to stationary interfaces, is that they can be moved, offering the potential of post-synthesis control of the dielectric constant. However, to date, direct imaging of how changes in domain wall pattern cause a change in dielectric constant within a single sample has not been realized. In this work, we demonstrate that changing the domain wall density allows the engineering of the dielectric constant in hexagonal-ErMnO3 single crystals. The changes of the domain wall density are quantified via microscopy techniques, while the dielectric constant is determined via macroscopic dielectric spectroscopy measurements. The observed changes in the dielectric constant are quantitatively consistent with the observed variation in domain wall density, implying that the insulating domain walls behave as 'ideal' capacitors connected in series. Our approach to engineer the domain wall density can be readily extended to other control methods, e.g., electric fields or mechanical stresses, providing a novel degree of flexibility to in-situ tune the dielectric constant.

Engineering of ferroelectric domain structures enables direct control over the switching dynamics and is crucial for tuning the functional properties of ferroelectrics for various applications, ranging from capacitors to future nanoelectronics. Here, we investigate domain formation in poly- and single crystalline improper ferroelectric DyMnO3. We show that a non-uniform grain-size distribution in the polycrystals facilitates the coexistence of multi-scale domains, varying by up to one order of magnitude in size. This unusual domain structure originates from an inverted domain-size/grain-size dependence that is intrinsic to the hexagonal manganite polycrystals, expanding previous studies towards non-uniform grain-size distributions. Our results demonstrate that the micrometer-sized grains in DyMnO3 represent individual ferroelectric units with a characteristic domain structure, giving a new dimension to domain engineering in ferroelectric polycrystals with non-uniform microstructures.

Moir\'e physics plays an important role for the characterization of functional materials and the engineering of physical properties in general, ranging from strain-driven transport phenomena to superconductivity. Here, we report the observation of moir\'e fringes in conductive atomic force microscopy (cAFM) scans gained on the model ferroelectric Er(Mn,Ti)O$_3$. By performing a systematic study of the impact of key experimental parameters on the emergent moir\'e fringes, such as scan angle and pixel density, we demonstrate that the observed fringes arise due to a superposition of the applied raster scanning and sample-intrinsic properties, classifying the measured modulation in conductance as a scanning moir\'e effect. Our findings are important for the investigation of local transport phenomena in moir\'e engineered materials by cAFM, providing a general guideline for distinguishing extrinsic from intrinsic moir\'e effects. Furthermore, the experiments provide a possible pathway for enhancing the sensitivity, pushing the resolution limit of local transport measurements by probing conductance variations at the spatial resolution limit via more long-ranged moir\'e patterns.

The High Energy Physics community can benefit from a natural synergy in research activities into next-generation large-scale water and scintillator neutrino detectors, now being studied for remote reactor monitoring, discovery and exclusion applications in cooperative nonproliferation contexts. Since approximately 2010, US nonproliferation researchers, supported by the National Nuclear Security Administration (NNSA), have been studying a range of possible applications of relatively large (100 ton) to very large (hundreds of kiloton) water and scintillator neutrino detectors. In parallel, the fundamental physics community has been developing detectors at similar scales and with similar design features for a range of high-priority physics topics, primarily in fundamental neutrino physics. These topics include neutrino oscillation studies at beams and reactors, solar, and geological neutrino measurements, supernova studies, and others. Examples of ongoing synergistic work at U.S. national laboratories and universities include prototype gadolinium-doped water and water-based and opaque scintillator test-beds and demonstrators, extensive testing and industry partnerships related to large area fast position-sensitive photomultiplier tubes, and the development of concepts for a possible underground kiloton-scale water-based detector for reactor monitoring and technology demonstrations. Some opportunities for engagement between the two communities include bi-annual Applied Antineutrino Physics conferences, collaboration with U.S. National Laboratories engaging in this research, and occasional NNSA funding opportunities supporting a blend of nonproliferation and basic science R&D, directed at the U.S. academic community., Comment: contribution to Snowmass 2021

Theia would be a novel, "hybrid" optical neutrino detector, with a rich physics program. This paper is intended to provide a brief overview of the concepts and physics reach of Theia. Full details can be found in the Theia white paper [1]., Comment: Contribution to Snowmass 2021

A small percentage of dopant atoms can completely change the physical properties of the host material. For example, chemical doping controls the electronic transport behavior of semiconductors and gives rise to a wide range of emergent electric and magnetic phenomena in oxides. Imaging of individual dopant atoms in lightly doped systems, however, remains a major challenge, hindering characterization of the site-specific effects and local dopant concentrations that determine the atomic-scale physics. Here, we apply atom-probe tomography (APT) to resolve individual Ti atoms in the narrow band gap semiconductor ErMnO3 with a nominal proportion of 0.04 atomic percent. Our 3D imaging measures the Ti concentration at the unit cell level, providing quantitative information about the dopant distribution within the ErMnO3 crystal lattice. High-resolution APT maps reveal the 3D lattice position of individual Ti atoms, showing that they are located within the Mn layers with no signs of clustering or other chemical inhomogeneities. The 3D atomic-scale visualization of individual dopant atoms provides new opportunities for the study of local structure-property relations in complex oxides, representing an important step toward controlling dopant-driven quantum phenomena in next-generation oxide electronics.

The direct current (d.c.) 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 d.c. conduction ranging from insulating to metallic-like, which is leveraged in domain-wall-based memory, multi-level data storage, and synaptic devices. In contrast to the functional d.c. behaviors at charged walls, their response to alternating currents (a.c.) remains to be resolved. Here, we reveal a.c. characteristics at positively and negatively charged walls in ErMnO3, distinctly different from the response of the surrounding domains. By combining voltage-dependent spectroscopic measurements on macroscopic and local scales, we demonstrate a pronounced non-linear response at the electrode-wall junction, which correlates with the domain-wall charge state. The dependence on the a.c. 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 a.c. circuitry.

An organic glass scintillator developed by Sandia National Laboratories was characterized in terms of its light output and pulse shape discrimination (PSD) properties and compared to commercial liquid (EJ-309) and plastic (EJ-276) organic scintillators. The electron light output was determined through relative comparison of the $^{137}$Cs Compton edge location. The proton light yield was measured using a double time-of-flight technique at the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory. Using a tunable broad-spectrum neutron source and an array of pulse-shape-discriminating observation scintillators, a continuous measurement of the proton light yield was performed for EJ-309 (200 keV$-$3.2 MeV), EJ-276 (170 keV$-$4.9 MeV), and the organic glass (50 keV$-$20 MeV). Finally, the PSD properties of the organic glass, EJ-309, and EJ-276 were evaluated using an AmBe source and compared via a figure-of-merit metric. The organic glass exhibited a higher electron light output than both EJ-309 and EJ-276. Its proton light yield and PSD performance were comparable to EJ-309 and superior to that of EJ-276. With these performance characteristics, the organic glass scintillator is well poised to replace current state-of-the-art PSD-capable scintillators in a range of fast neutron detection applications., Comment: 32 pages, 13 figures, 9 tables

Dislocations are one-dimensional (1D) topological line defects where the lattice deviates from the perfect crystal structure. The presence of dislocations transcends condensed matter research and gives rise to a diverse range of emergent phenomena [1-6], ranging from geological effects [7] to light emission from diodes [8]. Despite their ubiquity, to date, the controlled formation of dislocations is usually achieved via strain fields, applied either during growth [9,10] or retrospectively via deformation, e.g., (nano [11-14])-indentation [15]. Here we show how partial dislocations can be induced using local electric fields, altering the structure and electronic response of the material where the field is applied. By combining high-resolution imaging techniques and density functional theory calculations, we directly image these dislocations in the ferroelectric hexagonal manganite Er(Ti,Mn)O3 and study their impact on the local electric transport behaviour. The use of an electric field to induce partial dislocations is a conceptually new approach to the burgeoning field of emergent defect-driven phenomena and enables local property control without the need of external macroscopic strain fields. This control is an important step towards integrating and functionalising dislocations in practical devices for future oxide electronics., Comment: 20 pages, 7 figures

Conductive and electrostatic atomic force microscopy (cAFM and EFM) are used to investigate the electric conduction at nominally neutral domain walls in hexagonal manganites. The EFM measurements reveal a propensity of mobile charge carriers to accumulate at the nominally neutral domain walls in ErMnO3, which is corroborated by cAFM scans showing locally enhanced d.c. conductance. Our findings are explained based on established segregation enthalpy profiles for oxygen vacancies and interstitials, providing a microscopic model for previous, seemingly disconnected observations ranging from insulating to conducting domain wall behavior. In addition, we observe variations in conductance between different nominally neutral walls that we attribute to deviations from the ideal charge-neutral structure within the bulk, leading to a superposition of extrinsic and intrinsic contributions. Our study clarifies the complex transport properties at nominally neutral domain walls in hexagonal manganites and establishes new possibilities for tuning their electronic response based on oxidation conditions, opening the door for domain-wall based sensor technology., Comment: 5 pages, 3 figures

Low-temperature X-ray photoemission electron microscopy (X-PEEM) is used to measure the electric potential at domain walls in improper ferroelectric Er0.99Ca0.01MnO3. By combining X-PEEM with scanning probe microscopy and theory, we develop a model that relates the detected X-PEEM contrast to the emergence of uncompensated bound charges, explaining the image formation based on intrinsic electronic domain-wall properties. In contrast to previously applied low-temperature electrostatic force microscopy (EFM), X-PEEM readily distinguishes between positive and negative bound charges at domain walls. Our study introduces an X-PEEM based approach for low-temperature electrostatic potential mapping, facilitating nanoscale spatial resolution and data acquisition times in the order of 0.1-1 sec., Comment: 15 pages, 6 figures

The optical and scintillation properties of undoped, Si-doped, and Si, B co-doped GaAs samples were studied. The light yield specification and X-ray luminescence of GaAs over a wide IR region by using Si and InGaAs photodetectors are presented. The undoped GaAs demonstrated a narrow emission band at 838 nm (1.48 eV) and a low light output of about 2 ph/keV. The GaAs:Si is characterized by three broad luminescence bands at 830 nm (1.49 eV), 1070 nm (1.16 eV), 1335 nm (0.93 eV) and a light output of about 71 ph/keV. In the case of GaAs:(Si, B), four luminescence bands at 860 nm (1.44 eV), 930 nm (1.33 eV), 1070 nm (1.16 eV) and 1335 nm (0.93 eV) were observed. A high light yield higher than 125 ph/keV was estimated for the co-doped sample. The applications of low energy gap semiconductors as cryogenic scintillators for particle detection are discussed. The GaAs is a promising crystal for a cryogenic scintillator for the dark matter (DM) detection.

Ferroelectric domain walls represent multifunctional 2D-elements with great potential for novel device paradigms at the nanoscale. Improper ferroelectrics display particularly promising types of domain walls, which, due to their unique robustness, are the ideal template for imposing specific electronic behavior. Chemical doping, for instance, induces p- or n-type characteristics and electric fields reversibly switch between resistive and conductive domain-wall states. Here, we demonstrate diode-like conversion of alternating-current (AC) into direct-current (DC) output based on neutral 180$^{\circ}$ domain walls in improper ferroelectric ErMnO$_3$. By combining scanning probe and dielectric spectroscopy, we show that the rectification occurs for frequencies at which the domain walls are fixed to their equilibrium position. The practical frequency regime and magnitude of the output is controlled by the bulk conductivity. Using density functional theory we attribute the transport behavior at the neutral walls to an accumulation of oxygen defects. Our study reveals domain walls acting as 2D half-wave rectifiers, extending domain-wall-based nanoelectronic applications into the realm of AC technology.

This paper is the first report of n-type GaAs as a cryogenic scintillation radiation detector for the detection of electron recoils from interacting dark matter (DM) particles in the poorly explored MeV/c2 mass range. Seven GaAs samples from two commercial suppliers and with different silicon and boron concentrations were studied for their low temperature optical and scintillation properties. All samples are n-type even at low temperatures and exhibit emission between silicon donors and boron acceptors that peaks at 1.33 eV (930 nm). The lowest excitation band peaks at 1.44 eV (860 nm) and the overlap between the emission and excitation bands is small. The X-ray excited luminosities range from 7 to 43 photons/keV. Thermally stimulated luminescence measurements show that n-type GaAs does not accumulate metastable radiative states that could cause afterglow. Further development and use with cryogenic photodetectors promises a remarkable combination of large target size, ultra-low backgrounds, and a sensitivity to electron recoils of a few eV that would be produced by DM particles as light as a few MeV/c2., Comment: Journal of Applied Physics JAP17-AR-07550 (in press) Received 6 December 2017; accepted 13 February 2018 Selected for Editors Pick Feb 16

Acceptor and donor doping is a standard for tailoring semiconductors. More recently, doping was adapted to optimize the behavior at ferroelectric domain walls. In contrast to more than a century of research on semiconductors, the impact of chemical substitutions on the local electronic response at domain walls is largely unexplored. Here, the hexagonal manganite ErMnO$_3$ is donor doped with Ti$^{4+}$. Density functional theory calculations show that Ti$^{4+}$ goes to the B-site, replacing Mn$^{3+}$. Scanning probe microscopy measurements confirm the robustness of the ferroelectric domain template. The electronic transport at both macro- and nanoscopic length scales is characterized. The measurements demonstrate the intrinsic nature of emergent domain wall currents and point towards Poole-Frenkel conductance as the dominant transport mechanism. Aside from the new insight into the electronic properties of hexagonal manganites, B-site doping adds an additional degree of freedom for tuning the domain wall functionality.

The spontaneous transformations associated with symmetry-breaking phase transitions generate domain structures and defects that may be topological in nature. The formation of these defects can be described according to the Kibble-Zurek mechanism, which provides a generic relation that applies from cosmological to interatomic lengthscales. Its verification is challenging, however, in particular at the cosmological scale where experiments are impractical. While it has been demonstrated for selected condensed-matter systems, major questions remain regarding e.g. its degree of universality. Here we develop a global Kibble-Zurek picture from the condensed-matter level. We show theoretically that a transition between two fluctuation regimes (Ginzburg and mean-field) can lead to an intermediate region with reversed scaling, and we verify experimentally this behavior for the structural transition in the series of multiferroic hexagonal manganites. Trends across the series allow us to identify additional intrinsic features of the defect formation beyond the original Kibble-Zurek paradigm., Comment: 8 pages, 4 figures

Historically, the discovery and optimization of doped bulk materials has been predominantly developed through an Edisonian approach. While successful and despite the constant progress in fundamental understanding of detector materials physics, the process has been restricted by its inherent slow pace and low success rate. This poor throughput owes largely to the considerable compositional space that needs to be accounted for to fully comprehend complex material/performance relationship. Here, we present a combinatorial approach where doped bulk scintillator materials can be rapidly optimized for their properties through concurrent extrinsic doping/co-doping strategies. The concept that makes use of Design of Experiment, rapid growth and evaluation techniques, and multivariable regression analysis, has been successfully applied to the engineering of NaI performance, a historical but mediocre performer in scintillation detection. Using this approach, we identified a three-element doping/co-doping strategy that significantly improves the material performance. The composition was uncovered by simultaneously screening for a beneficial co-dopant ion among the alkaline earth metal family and by optimizing its concentration and that of Tl+ and Eu2+ ions. The composition with the best performance was identified as 0.1% mol Tl+, 0.1% mol Eu2+ and 0.2% mol Ca2+. This formulation shows enhancement of energy resolution and light output at 662 keV, from 6.3 to 4.9%, and from 44,000 to 52,000 ph/MeV, respectively. The method, in addition to improving NaI performance, provides a versatile framework for rapidly unveiling complex and concealed correlations between material composition and performance, and should be broadly applicable to optimization of other material properties., Comment: 7 pages, 3 figures

High-resolution X-ray photoemission electron microscopy (X-PEEM) is a well-established method for imaging ferroelectric domain structures. Here, we expand the scope of application of X-PEEM and demonstrate its capability for imaging and investigating domain walls in ferroelectrics with high-spatial resolution. Using ErMnO3 as test system, we show that ferroelectric domain walls can be visualized based on photo-induced charging effects and local variations in their electronic conductance can be mapped by analyzing the energy distribution of photoelectrons. Our results open the door for non-destructive, contract-free, and element-specific studies of the electronic and chemical structure at domain walls in ferroelectrics.