Enhanced Critical Field of Superconductivity at an Oxide Interface.

The nature of superconductivity and its interplay with strong spin-orbit coupling at the KTaO3(111) interfaces remain a subject of debate. To address this problem, we grew epitaxial LaMnO3/KTaO3(111) heterostructures. We show that superconductivity is robust against the in-plane magnetic field, with the critical field of superconductivity reaching ∼25 T in optimally doped heterostructures. The superconducting order parameter is highly sensitive to the carrier density. We argue that spin-orbit coupling drives the formation of anomalous quasiparticles with vanishing magnetic moment, providing significant condensate immunity against magnetic fields beyond the Pauli paramagnetic limit. These results offer design opportunities for superconductors with extreme resilience against the applied magnetic fields.

Thickness-Dependent Thermal Conductivity and Phonon Mean Free Path Distribution in Single-Crystalline Barium Titanate.

Nanosized perovskite ferroelectrics are widely employed in several electromechanical, photonics, and thermoelectric applications. Scaling of ferroelectric materials entails a severe reduction in the lattice (phonon) thermal conductivity, particularly at sub-100 nm length scales. Such thermal conductivity reduction can be accurately predicted using the information of phonon mean free path (MFP) distribution. The current understanding of phonon MFP distribution in perovskite ferroelectrics is still inconclusive despite the critical thermal management implications. Here, high-quality single-crystalline barium titanate (BTO) thin films, a representative perovskite ferroelectric material, are grown at several thicknesses. Using experimental thermal conductivity measurements and first-principles based modeling (including four-phonon scattering), the phonon MFP distribution is determined in BTO. The simulation results agree with the measured thickness-dependent thermal conductivity. The results show that the phonons with sub-100 nm MFP dominate the thermal transport in BTO, and phonons with MFP exceeding 10 nm contribute ≈35% to the total thermal conductivity, in significant contrast to previously published experimental results. The experimentally validated phonon MFP distribution is consistent with the theoretical predictions of other complex crystals with strong anharmonicity. This work paves the way for thermal management in nanostructured and ferroelectric-domain-engineered systems for oxide perovskite-based functional materials.

Anisotropic superconductivity at KTaO3(111) interfaces.

A two-dimensional, anisotropic superconductivity was recently found at the KTaO3(111) interfaces. The nature of the anisotropic superconducting transition remains a subject of debate. To investigate the origins of the observed behavior, we grew epitaxial KTaO3(111)-based heterostructures. We show that the superconductivity is robust against the in-plane magnetic field and violates the Pauli limit. We also show that the Cooper pairs are more resilient when the bias is along [11[Formula: see text]] (I ∥ [11[Formula: see text]]) and the magnetic field is along [1[Formula: see text]0] (B ∥ [1[Formula: see text]0]). We discuss the anisotropic nature of superconductivity in the context of electronic structure, orbital character, and spin texture at the KTaO3(111) interfaces. The results point to future opportunities to enhance superconducting transition temperatures and critical fields in crystalline, two-dimensional superconductors with strong spin-orbit coupling.

Ferroelectric Domain Wall Engineering Enables Thermal Modulation in PMN-PT Single Crystals.

Acting like thermal resistances, ferroelectric domain walls can be manipulated to realize dynamic modulation of thermal conductivity (k), which is essential for developing novel phononic circuits. Despite the interest, little attention has been paid to achieving room-temperature thermal modulation in bulk materials due to challenges in obtaining a high thermal conductivity switching ratio (khigh /klow ), particularly in commercially viable materials. Here, room-temperature thermal modulation in 2.5 mm-thick Pb(Mg1/3 Nb2/3 )O3 -xPbTiO3 (PMN-xPT) single crystals is demonstrated. With the use of advanced poling conditions, assisted by the systematic study on composition and orientation dependence of PMN-xPT, a range of thermal conductivity switching ratios with a maximum of ≈1.27 is observed. Simultaneous measurements of piezoelectric coefficient (d33 ) to characterize the poling state, domain wall density using polarized light microscopy (PLM), and birefringence change using quantitative PLM reveal that compared to the unpoled state, the domain wall density at intermediate poling states (0< d33

Single Atomic Layer Ferroelectric on Silicon.

A single atomic layer of ZrO2 exhibits ferroelectric switching behavior when grown with an atomically abrupt interface on silicon. Hysteresis in capacitance-voltage measurements of a ZrO2 gate stack demonstrate that a reversible polarization of the ZrO2 interface structure couples to the carriers in the silicon. First-principles computations confirm the existence of multiple stable polarization states and the energy shift in the semiconductor electron states that result from switching between these states. This monolayer ferroelectric represents a new class of materials for achieving devices that transcend conventional complementary metal oxide semiconductor (CMOS) technology. Significantly, a single atomic layer ferroelectric allows for more aggressively scaled devices than bulk ferroelectrics, which currently need to be thicker than 5-10 nm to exhibit significant hysteretic behavior (Park, et al. Adv. Mater. 2015, 27, 1811).

Orbital engineering in symmetry-breaking polar heterostructures.

We experimentally demonstrate a novel approach to substantially modify orbital occupations and symmetries in electronically correlated oxides. In contrast to methods using strain or confinement, this orbital tuning is achieved by exploiting charge transfer and inversion symmetry breaking using atomically layered heterostructures. We illustrate the technique in the LaTiO_{3}-LaNiO_{3}-LaAlO_{3} system; a combination of x-ray absorption spectroscopy and ab initio theory reveals electron transfer and concomitant polar fields, resulting in a ∼50% change in the occupation of Ni d orbitals. This change is sufficiently large to remove the orbital degeneracy of bulk LaNiO_{3} and creates an electronic configuration approaching a single-band Fermi surface. Furthermore, we theoretically show that such three-component heterostructuring is robust and tunable by choice of insulator in the heterostructure, providing a general method for engineering orbital configurations and designing novel electronic systems.

Tuning the structure of nickelates to achieve two-dimensional electron conduction.

Metallic electronic transport in nickelate heterostructures can be induced and confined to two dimensions (2D) by controlling the structural parameters of the nickel-oxygen planes.

Active silicon integrated nanophotonics: ferroelectric BaTiO3 devices.

The integration of complex oxides on silicon presents opportunities to extend and enhance silicon technology with novel electronic, magnetic, and photonic properties. Among these materials, barium titanate (BaTiO3) is a particularly strong ferroelectric perovskite oxide with attractive dielectric and electro-optic properties. Here we demonstrate nanophotonic circuits incorporating ferroelectric BaTiO3 thin films on the ubiquitous silicon-on-insulator (SOI) platform. We grow epitaxial, single-crystalline BaTiO3 directly on SOI and engineer integrated waveguide structures that simultaneously confine light and an RF electric field in the BaTiO3 layer. Using on-chip photonic interferometers, we extract a large effective Pockels coefficient of 213 ± 49 pm/V, a value more than six times larger than found in commercial optical modulators based on lithium niobate. The monolithically integrated BaTiO3 optical modulators show modulation bandwidth in the gigahertz regime, which is promising for broadband applications.

Modifying the electronic orbitals of nickelate heterostructures via structural distortions.

We describe a general materials design approach that produces large orbital energy splittings (orbital polarization) in nickelate heterostructures, creating a two-dimensional single-band electronic surface at the Fermi energy. The resulting electronic structure mimics that of the high temperature cuprate superconductors. The two key ingredients are (i) the construction of atomic-scale distortions about the Ni site via charge transfer and internal electric fields, and (ii) the use of three-component (tricomponent) superlattices to break inversion symmetry. We use ab initio calculations to implement the approach, with experimental verification of the critical structural motif that enables the design to succeed.

Surface x-ray diffraction results on the III-V droplet heteroepitaxy growth process for quantum dots: recent understanding and open questions.

In recent years, epitaxial growth of self-assembled quantum dots has offered a way to incorporate new properties into existing solid state devices. Although the droplet heteroepitaxy method is relatively complex, it is quite relaxed with respect to the material combinations that can be used. This offers great flexibility in the systems that can be achieved. In this paper we review the structure and composition of a number of quantum dot systems grown by the droplet heteroepitaxy method, emphasizing the insights that these experiments provide with respect to the growth process. Detailed structural and composition information has been obtained using surface X-ray diffraction analyzed by the COBRA phase retrieval method. A number of interesting phenomena have been observed: penetration of the dots into the substrate ("nano-drilling") is often encountered; interdiffusion and intermixing already start when the group III droplets are deposited, and structure and composition may be very different from the one initially intended.

Atomic-scale mapping of quantum dots formed by droplet epitaxy.

Quantum dots (QDs) have applications in optoelectronic devices, quantum information processing and energy harvesting. Although the droplet epitaxy fabrication method allows for a wide range of material combinations to be used, little is known about the growth mechanisms involved. Here we apply direct X-ray methods to derive sub-ångström resolution maps of QDs crystallized from indium droplets exposed to antimony, as well as their interface with a GaAs (100) substrate. We find that the QDs form coherently and extend a few unit cells below the substrate surface. This facilitates a droplet-substrate exchange of atoms, resulting in core-shell structures that contain a surprisingly small amount of In. The work provides the first atomic-scale mapping of the interface between epitaxial QDs and a substrate, and establishes the usefulness of X-ray phasing techniques for this and similar systems.