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Abstract: As a promising candidate for nonvolatile memory devices, the hafnia‐based ferroelectric system has recently been a hot research topic. Although significant progress has been made over the past decade, the endurance problem is still an obstacle to its final application. In perovskite‐based ferroelectrics, such as the well‐studied Pb[ZrxTi1−x]O3 (PZT) family, polarization fatigue has been discussed within the framework of the interaction of charged defects (such as oxygen vacancies) with the moving domains during the switching process, particularly at the electrode‐ferroelectric interface. Armed with this background, a hypothesis is set out to test that a similar mechanism can be in play with the hafnia‐based ferroelectrics. The conducting perovskite La‐Sr‐Mn‐O is used as the contact electrode to create La0.67Sr0.33MnO3 / Hf0.5Zr0.5O2 (HZO)/ La0.67Sr0.33MnO3 capacitor structures deposited on SrTiO3‐Si substrates. Nanoscale X‐ray diffraction is performed on single capacitors, and a structural phase transition from polar o‐phase toward non‐polar m‐phase is demonstrated during the bipolar switching process. The energy landscape of multiphase HZO has been calculated at varying oxygen vacancy concentrations. Based on both theoretical and experimental results, it is found that a polar to non‐polar phase transformation caused by oxygen vacancy redistribution during electric cycling is a likely explanation for fatigue in HZO.

High-density phase change memory (PCM) storage is proposed for materials with multiple intermediate resistance states, which have been observed in 1T-TaS2 due to charge density wave (CDW) phase transitions. However, the metastability responsible for this behavior makes the presence of multistate switching unpredictable in TaS2 devices. Here, we demonstrate the fabrication of nanothick verti-lateral H-TaS2/1T-TaS2 heterostructures in which the number of endotaxial metallic H-TaS2 monolayers dictates the number of resistance transitions in 1T-TaS2 lamellae near room temperature. Further, we also observe optically active heterochirality in the CDW superlattice structure, which is modulated in concert with the resistivity steps, and we show how strain engineering can be used to nucleate these polytype conversions. This work positions the principle of endotaxial heterostructures as a promising conceptual framework for reliable, non-volatile, and multi-level switching of structure, chirality, and resistance.

Increasing interest in three-dimensional nanostructures adds impetus to electron microscopy techniques capable of imaging at or below the nanoscale in three dimensions. We present a reconstruction algorithm that takes as input a focal series of four-dimensional scanning transmission electron microscopy (4D-STEM) data. We apply the approach to a lead iridate, PbIrO, and yttrium-stabilized zirconia, YZrO, heterostructure from data acquired with the specimen in a single plan-view orientation, with the epitaxial layers stacked along the beam direction. We demonstrate that Pb-Ir atomic columns are visible in the uppermost layers of the reconstructed volume. We compare this approach to the alternative techniques of depth sectioning using differential phase contrast scanning transmission electron microscopy (DPC-STEM) and multislice ptychographic reconstruction.

Atomic-scale control of spins by electric fields is highly desirable for future technological applications. Magnetically doped Aurivillius-phase oxides present one route to achieve this, with magnetic ions substituted into the ferroelectric structure at dilute concentrations, resulting in spin-charge coupling. However, there has been minimal exploration of the ferroelectric switching pathways in this materials class, limiting predictions of the influence of an electric field on magnetic spins in the structure. Here, we determine the ferroelectric switching pathways of the end member of the Aurivillius phase family, Bi2WO6, using a combination of group theoretic analysis and density functional theory calculations. We find that in the ground state P21ab phase, a two-step switching pathway via C2 and Cm intermediate phases provides the lowest energy barrier. Considering iron substitutions on the W site in Bi2WO6, we determine the spin easy axis. By tracking the change in spin directionality during ferroelectric switching, we find that a 90∘ switch in the polarization direction leads to a 112° reorientation of the spin easy axis. The low-symmetry crystal-field environment of Bi2WO6 and magnetoelastic coupling on the magnetic dopant provide a route to spin control via an applied electric field.

We extend the calculation of dark matter direct detection rates via electronic transitions in general dielectric crystal targets, combining state-of-the-art density functional theory calculations of electronic band structures and wave functions near the band gap, with semianalytic approximations to include additional states farther away from the band gap. We show, in particular, the importance of all-electron reconstruction for recovering large momentum components of electronic wave functions, which, together with the inclusion of additional states, has a significant impact on direct detection rates, especially for heavy mediator models and at O(10 eV) and higher energy depositions. Applying our framework to silicon and germanium (that have been established already as sensitive dark matter detectors), we find that our extended calculations can appreciably change the detection prospects. Our calculational framework is implemented in an open-source program exceed-dm (Extended Calculation of Electronic Excitations for Direct detection of Dark Matter), to be released in an upcoming publication.

We propose the use of silicon carbide (SiC) for direct detection of sub-GeV dark matter. SiC has properties similar to both silicon and diamond but has two key advantages: (i) it is a polar semiconductor which allows sensitivity to a broader range of dark matter candidates; and (ii) it exists in many stable polymorphs with varying physical properties and hence has tunable sensitivity to various dark matter models. We show that SiC is an excellent target to search for electron, nuclear and phonon excitations from scattering of dark matter down to 10 keV in mass, as well as for absorption processes of dark matter down to 10 meV in mass. Combined with its widespread use as an alternative to silicon in other detector technologies and its availability compared to diamond, our results demonstrate that SiC holds much promise as a novel dark matter detector.

Magnetoelectrics, materials that exhibit coupling between magnetic and electric degrees of freedom, not only offer a rich environment for studying the fundamental materials physics of spin-charge coupling but also present opportunities for future information technology paradigms. We present results of electric field manipulation of spins in a ferroelectric medium using dilute ferric ion-doped lead titanate as a model system. Combining first-principles calculations and electron paramagnetic resonance (EPR), we show that the ferric ion spins are preferentially aligned perpendicular to the ferroelectric polar axis, which we can manipulate using an electric field. We also demonstrate coherent control of the phase of spin superpositions by applying electric field pulses during time-resolved EPR measurements. Our results suggest a new pathway toward the manipulation of spins for quantum and classical spintronics.

New ideas for low-mass dark matter direct detection suggest that narrow band gap materials, such as Dirac semiconductors, are sensitive to the absorption of meV dark matter or the scattering of keV dark matter. Here we propose spin-orbit semiconductors - materials whose band gap arises due to spin-orbit coupling - as low-mass dark matter targets owing to their O(10 meV) band gaps. We present three material families that are predicted to be spin-orbit semiconductors using density functional theory (DFT), assess their electronic and topological features, and evaluate their use as low-mass dark matter targets. In particular, we find that the tin pnictide compounds are especially suitable having a tunable range of meV-scale band gaps with anisotropic Fermi velocities allowing directional detection. Finally, we address the pitfalls in the DFT methods that must be considered in the ab initio prediction of narrow-gapped materials, including those close to the topological critical point.

Increasing interest in three-dimensional nanostructures adds impetus toelectron microscopy techniques capable of imaging at or below the nanoscale inthree dimensions. We present a reconstruction algorithm that takes as input afocal series of four-dimensional scanning transmission electron microscopy(4D-STEM) data and transcends the prevalent structure retrieval algorithmassumption of a very thin specimen homogenous along the optic axis. Wedemonstrate this approach by reconstructing the different layers of a leadiridate (Pb$_2$Ir$_2$O$_7$) and yttrium-stabilized zirconia(Y$_{0.095}$Zr$_{0.905}$O$_2$) heterostructure from data acquired with thespecimen in a single plan-view orientation, with the epitaxial layers stackedalong the beam direction.

Increasing interest in three-dimensional nanostructures adds impetus toelectron microscopy techniques capable of imaging at or below the nanoscale inthree dimensions. We present a reconstruction algorithm that takes as input afocal series of four-dimensional scanning transmission electron microscopy(4D-STEM) data. We apply the approach to a lead iridate, Pb$_2$Ir$_2$O$_7$, andyttrium-stabilized zirconia,Y$_{0.095}$Zr$_{0.905}$O$_2$ , heterostructure fromdata acquired with the specimen in a single plan-view orientation, with theepitaxial layers stacked along the beam direction. We demonstrate that Pb-Iratomic columns are visible in the uppermost layers of the reconstructed volume.We compare this approach to the alternative techniques of depth sectioningusing differential phase contrast scanning transmission electron microscopy(DPC-STEM) and multislice ptychographic reconstruction.

Direct-detection experiments for light dark matter are making enormous leaps in reaching previously unexplored model space. Several recent proposals rely on collective excitations, where the experimental sensitivity is highly dependent on detailed properties of the target material, well beyond just nucleus mass numbers as in conventional searches. It is thus important to optimize the target choice when considering which experiment to build. We carry out a comparative study of target materials across several detection channels, focusing on electron transitions and single (acoustic or optical) phonon excitations in crystals, as well as the traditional nuclear recoils. We compare materials currently in use in nuclear recoil experiments (Si, Ge, NaI, CsI, CaWO4), a few of which have been proposed for light dark matter experiments (GaAs, Al2O3, diamond), as well as 16 other promising polar crystals across all detection channels. We find that target- and dark-matter-model-dependent reach is largely determined by a small number of material parameters: speed of sound, electronic band gap, mass number, Born effective charge, high-frequency dielectric constant, and optical phonon energies. We showcase, for each of the two benchmark models, an exemplary material that has a better reach than in any currently proposed experiment.

We present a unified theoretical framework for computing spin-independent direct detection rates via various channels relevant for sub-GeV dark matter — nuclear re- coils, electron transitions and single phonon excitations. Despite the very different physics involved, in each case the rate factorizes into the particle-level matrix element squared, and an integral over a target material- and channel-specific dynamic structure factor. We show how the dynamic structure factor can be derived in all three cases following the same procedure, and extend previous results in the literature in several aspects. For electron transitions, we incorporate directional dependence and point out anisotropic target materials with strong daily modulation in the scattering rate. For single phonon excitations, we present a new derivation of the rate formula from first principles for generic spin-independent couplings, and include the first calculation of phonon excitation through electron couplings. We also discuss the interplay between single phonon excitations and nuclear recoils, and clarify the role of Umklapp processes, which can dominate the single phonon production rate for dark matter heavier than an MeV. Our results highlight the complementarity between various search channels in probing different kinematic regimes of dark matter scattering, and provide a common reference to connect dark matter theories with ongoing and future direct detection experiments.

Ferroelectric domain walls are attracting broad attention as atomic-scale switches, diodes, and mobile wires for next-generation nanoelectronics. Charged domain walls in improper ferroelectrics are particularly interesting as they offer multifunctional properties and an inherent stability not found in proper ferroelectrics. Here we study the energetics and structure of charged walls in improper ferroelectric YMnO3,InMnO3, and YGaO3 by first-principles calculations and phenomenological modeling. Positively and negatively charged walls are asymmetric in terms of local structure and width. The wall width scales with the amplitude of the primary structural order parameter and the coupling strength to the polarization, reflecting that polarization is not the driving force for domain formation. We introduce general rules for how to engineer n- and p-type domain wall conductivity based on the domain size, polarization, and electronic band gap. This opens the possibility of fine tuning the local transport properties and designing p-n-junctions for domain wall-based nanocircuitry.

As a promising candidate for nonvolatile memory devices, the hafnia‐based ferroelectric system has recently been a hot research topic. Although significant progress has been made over the past decade, the endurance problem is still an obstacle to its final application. In perovskite‐based ferroelectrics, such as the well‐studied Pb[ZrxTi1−x]O3 (PZT) family, polarization fatigue has been discussed within the framework of the interaction of charged defects (such as oxygen vacancies) with the moving domains during the switching process, particularly at the electrode‐ferroelectric interface. Armed with this background, a hypothesis is set out to test that a similar mechanism can be in play with the hafnia‐based ferroelectrics. The conducting perovskite La‐Sr‐Mn‐O is used as the contact electrode to create La0.67Sr0.33MnO3 / Hf0.5Zr0.5O2 (HZO)/ La0.67Sr0.33MnO3 capacitor structures deposited on SrTiO3‐Si substrates. Nanoscale X‐ray diffraction is performed on single capacitors, and a structural phase transition from polar o‐phase toward non‐polar m‐phase is demonstrated during the bipolar switching process. The energy landscape of multiphase HZO has been calculated at varying oxygen vacancy concentrations. Based on both theoretical and experimental results, it is found that a polar to non‐polar phase transformation caused by oxygen vacancy redistribution during electric cycling is a likely explanation for fatigue in HZO. [ABSTRACT FROM AUTHOR]

The article demonstrates coherent control of the phase of spin superpositions by applying electric field pulses during time-resolved EPR measurements and suggest a new pathway toward the manipulation of spins for quantum and classical spintronics. It discusses the electric field manipulation of spins in a ferroelectric medium using dilute ferric ion doped lead titanate as a model system.

Solid-state materials are currently being explored as a platform for the manipulation of spins for spintronics and quantum information science. More broadly, a wide spectrum of ferroelectric materials, spanning from inorganic oxides to polymeric systems such as PVDF, present a different approach to explore quantum phenomena in which the spins are set and manipulated with electric fields. Using dilute Fe 3+ -doped ferroelectric PbTiO 3 -SrTiO 3 superlattices as a model system, we demonstrate intrinsic spin-polarization control of spin directionality in complex ferroelectric vortices and skyrmions. Electron paramagnetic resonance (EPR) spectra show that the spins in the Fe 3+ ion are strongly coupled to the local polarization and preferentially aligned perpendicular to the ferroelectric polar c axis in this complex vortex structure. The effect of polarization-spin directionality is corroborated by first-principles calculations, demonstrating the variation of the spin directionality with the polar texture and offering the potential for future quantum analogues of macroscopic magnetoelectric devices.