Nanocrystal superlattices (NC SLs) have long been sought as promising metamaterials, with nanoscale-engineered properties arising from collective and synergistic effects among the constituent building blocks. Lead halide perovskite (LHP) NCs come across as outstanding candidates for SL design, as they demonstrate collective light emission, known as superfluorescence, in single- and multicomponent SLs. Thus far, LHP NCs have only been assembled in single-component SLs or coassembled with dielectric NC building blocks acting solely as spacers between luminescent NCs.
View Article and Find Full Text PDFRecently, a highly ordered Moiré dislocation lattice was identified at the interface between a SrTiO (STO) thin film and the (LaAlO)(SrTaAlO) (LSAT) substrate. A fundamental understanding of the local ionic and electronic structures around the dislocation cores is crucial to further engineer the properties of these complex multifunctional heterostructures. Here, we combine experimental characterization via analytical scanning transmission electron microscopy with results of molecular dynamics and density functional theory calculations to gain insights into the structure and defect chemistry of these dislocation arrays.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2023
Proteins unfold in chaotropic salt solutions, a process that is difficult to observe at the single protein level. The work presented here demonstrates that a liquid-based atomic force microscope and graphene liquid-cell-based scanning transmission electron microscope make it possible to observe chemically induced protein unfolding. To illustrate this capability, ferritin proteins were deposited on a graphene surface, and the concentration-dependent urea- or guanidinium-induced changes of morphology were monitored for holo-ferritin with its ferrihydrite core as well as apo-ferritin without this core.
View Article and Find Full Text PDFMaterial surfaces encompass structural and chemical discontinuities that often lead to the loss of the property of interest in so-called dead layers. It is particularly problematic in nanoscale oxide electronics, where the integration of strongly correlated materials into devices is obstructed by the thickness threshold required for the emergence of their functionality. Here we report the stabilization of ultrathin out-of-plane ferroelectricity in oxide heterostructures through the design of an artificial flux-closure architecture.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2023
Improper ferroelectrics are expected to be more robust than conventional ferroelectrics against depolarizing field effects and to exhibit a much-desired absence of critical thickness. Recent studies, however, revealed the loss of ferroelectric response in epitaxial improper ferroelectric thin films. Here, we investigate improper ferroelectric hexagonal YMnO thin films and find that the polarization suppression, and hence functionality, in the thinner films is due to oxygen off-stoichiometry.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2022
Within the emerging field of proton-conducting fuel cells, BaZrYO (BZY10) is an attractive material due to its high conductivity and stability. The fundamentals of conduction in sintered pellets and thin films heterostructures have been explored in several studies; however, the role of crystallographic orientation, grains, and grain boundaries is poorly understood for proton conduction. This article reports proton conduction in a self-assembled multi-oriented BZY10 thin film grown on top of a (110) NdGaO substrate.
View Article and Find Full Text PDFPhase transition points can be used to critically reduce the ionic migration activation energy, which is important for realizing high-performance electrolytes at low temperatures. Here, we demonstrate a route toward low-temperature thermionic conduction in solids, by exploiting the critically lowered activation energy associated with oxygen transport in Ca-substituted bismuth ferrite (BiCaFeO) films. Our demonstration relies on the finding that a compositional phase transition occurs by varying Ca doping ratio across x ≃ 0.
View Article and Find Full Text PDFThe performance and suitability of a new electron energy filter in combination with a hybrid pixel, direct electron detector for analytical (scanning) transmission electron microscopy are demonstrated using four examples. The STEM-EELS capabilities of the CEOS Energy Filtering and Imaging Device (CEFID) were tested with focus on weak signals and high spatio-temporal resolution. A multiferroic, multilayer structure of REMnO (RE = Yb, Er, Tb, Y), grown on yttria-stabilized zirconia (YSZ), is used to exemplify that this new instrumental setup produces valuable electron energy-loss spectroscopy (EELS) data at high energy losses even when using short acquisition times, providing detailed chemical information about the interfaces in this complex multilayer sample.
View Article and Find Full Text PDFCharge-transfer phenomena at heterointerfaces are a promising pathway to engineer functionalities absent in bulk materials but can also lead to degraded properties in ultrathin films. Mitigating such undesired effects with an interlayer reshapes the interface architecture, restricting its operability. Therefore, developing less-invasive methods to control charge transfer will be beneficial.
View Article and Find Full Text PDFFerroic order is characterized by hystereses with two remanent states and therefore inherently binary. The increasing interest in materials showing non-discrete responses, however, calls for a paradigm shift towards continuously tunable remanent ferroic states. Device integration for oxide nanoelectronics furthermore requires this tunability at the nanoscale.
View Article and Find Full Text PDFFerrimagnetic alloys are model systems for understanding the ultrafast magnetization switching in materials with antiferromagnetically coupled sublattices. Here we investigate the dynamics of the rare-earth and transition-metal sublattices in ferrimagnetic GdFeCo and TbCo dots excited by spin-orbit torques with combined temporal, spatial and elemental resolution. We observe distinct switching regimes in which the magnetizations of the two sublattices either remain synchronized throughout the reversal process or switch following different trajectories in time and space.
View Article and Find Full Text PDFSemiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35-65 meV (vs.
View Article and Find Full Text PDFIncreased data storage densities are required for the next generation of nonvolatile random access memories and data storage devices based on ferroelectric materials. Yet, with intensified miniaturization, these devices face a loss of their ferroelectric properties. Therefore, a full microscopic understanding of the impact of the nanoscale defects on the ferroelectric switching dynamics is crucial.
View Article and Find Full Text PDFWe review the concept of surface charge, first, in the context of the polarization in ferroelectric materials and, second, in the context of layers of charged ions in ionic insulators. While the former is traditionally discussed in the ferroelectrics community and the latter in the surface science community, we remind the reader that the two descriptions are conveniently unified within the modern theory of polarization. In both cases, the surface charge leads to electrostatic instability-the so-called "polar catastrophe"-if it is not compensated, and we review the range of phenomena that arise as a result of different compensation mechanisms.
View Article and Find Full Text PDFInversion-symmetry breaking is a ubiquitous concept in condensed-matter science: It is a prerequisite for technologically relevant effects such as piezoelectricity, nonlinear optical properties, and spin-transport phenomena. It also determines abstract properties, like the electronic topology in quantum materials. Therefore, the creation of materials where inversion symmetry can be turned on or off by design may be a versatile approach for controlling parity-related functionalities.
View Article and Find Full Text PDFThe sintering of alumina (AlO) traditionally occurs at high temperatures (up to ca. 1700 °C) and in significantly long times (up to several hours), which are required for the consolidation of the material by diffusion processes. Here we investigate the photonic sintering of alumina particles using millisecond flash lamp irradiation with extreme heating rates up to 10 K/min.
View Article and Find Full Text PDFThe optimization of novel transparent conductive oxides (TCOs) implies a better understanding of the role that the dopant plays on the optoelectronic properties of these materials. In this work, we perform a systematic study of the homologous series ZnInO (IZO) by characterizing the specific location of indium in the structure that leads to a nanodomain framework to release structural strain. Through a systematic study of different terms of the series, we have been able to observe the influence of the value in the nano-structural features of this homologous series.
View Article and Find Full Text PDFThe development of energy-efficient nanoelectronics based on ferroelectrics is hampered by a notorious polarization loss in the ultrathin regime caused by the unscreened polar discontinuity at the interfaces. So far, engineering charge screening at either the bottom or the top interface has been used to optimize the polarization state. Yet, it is expected that the combined effect of both interfaces determines the final polarization state; in fact the more so the thinner a film is.
View Article and Find Full Text PDFDirect epitaxial growth of III-Vs on silicon for optical emitters and detectors is an elusive goal. Nanowires enable the local integration of high-quality III-V material, but advanced devices are hampered by their high-aspect ratio vertical geometry. Here, we demonstrate the in-plane monolithic integration of an InGaAs nanostructure p-i-n photodetector on Si.
View Article and Find Full Text PDFSolution-processed lead sulfide quantum dots (PbS QDs) are very attractive as NIR-active semiconductors for the fabrication of cost-efficient optoelectronic devices. To control the thin film carrier transport, as well as stability, surface passivation is of crucial importance. Here, we present the successful surface passivation of PbS QDs by the formamidinium lead iodide (FAPbI) ligand.
View Article and Find Full Text PDFFour-terminal (4-T) tandem solar cells (.., perovskite/CuInSe (CIS)) rely on three transparent conductive oxide electrodes with high mobility and low free carrier absorption in the near-infrared (NIR) region.
View Article and Find Full Text PDFCharged domain walls in ferroelectrics hold great promise for the design of novel electronic devices due to their enhanced local conductivity. In fact, charged domain walls show unique properties including the possibility of being created, moved and erased by an applied voltage. Here, we demonstrate that the charged domain walls are constituted by a core region where most of the screening charge is localized and such charge accumulation is responsible for their enhanced conductivity.
View Article and Find Full Text PDFDual-ion batteries (DIBs) are electrochemical energy storage devices that operate by the simultaneous participation of two different ion species at the anode and cathode and rely on the use of an electrolyte that can withstand the high operation potential of the cathode. Under such conditions at the cathode, issues associated with the irreversible capacity loss and the formation of solid-electrolyte interphase at the surface of highly porous electrode materials are far less significant than at lower potentials, permitting the exploration of high surface area, permanently porous framework materials as effective charge storage media. This concept is investigated herein by employing zeolite-templated carbon (ZTC) as a cathode in a dual-ion battery based on a potassium bis(fluorosulfonyl)imide (KFSI) electrolyte.
View Article and Find Full Text PDFThe interfacial Dzyaloshinskii-Moriya interaction (DMI) is important for chiral domain walls (DWs) and for stabilizing magnetic skyrmions. We study the effects of introducing increasing thicknesses of Ir, from zero to 2 nm, into a Pt/Co/Ta multilayer between the Co and Ta layers. There is a marked increase in magnetic moment, due to the suppression of the dead layer at the interface with Ta, but the perpendicular anisotropy is hardly affected.
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