Interfacially enhanced superconductivity in Fe(Te,Se)/Bi4Te3 heterostructures.

Realizing topological superconductivity by integrating high-transition-temperature (TC) superconductors with topological insulators can open new paths for quantum computing applications. Here, we report a new approach for increasing the superconducting transition temperature ( T C o n s e t ) $( {T_C^{onset}} )$ by interfacing the unconventional superconductor Fe(Te,Se) with the topological insulator Bi-Te system in the low-Se doping regime, near where superconductivity vanishes in the bulk. The critical finding is that the T C o n s e t $T_C^{onset}$ of Fe(Te,Se) increases from nominally non-superconducting to as high as 12.5 K when Bi2Te3 is replaced with the topological phase Bi4Te3. Interfacing Fe(Te,Se) with Bi4Te3 is also found to be critical for stabilizing superconductivity in monolayer films where T C o n s e t $T_C^{onset}$ can be as high as 6 K. Measurements of the electronic and crystalline structure of the Bi4Te3 layer reveal that a large electron transfer, epitaxial strain, and novel chemical reduction processes are critical factors for the enhancement of superconductivity. This novel route for enhancing TC in an important epitaxial system provides new insight on the nature of interfacial superconductivity and a platform to identify and utilize new electronic phases. This article is protected by copyright. All rights reserved.

Angular-Momentum Transfer Mediated by a Vibronic-Bound-State.

The notion that phonons can carry pseudo-angular momentum has many major consequences, including topologically protected phonon chirality, Berry curvature of phonon band structure, and the phonon Hall effect. When a phonon is resonantly coupled to an orbital state split by its crystal field environment, a so-called vibronic bound state forms. Here, a vibronic bound state is observed in NaYbSe2 , a quantum spin liquid candidate. In addition, field and polarization dependent Raman microscopy is used to probe an angular momentum transfer of ΔJz = ±â„ between phonons and the crystalline electric field mediated by the vibronic bound stat. This angular momentum transfer between electronic and lattice subsystems provides new pathways for selective optical addressability of phononic angular momentum via electronic ancillary states.

Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO2.

The current challenge to realizing continuously tunable magnetism lies in our inability to systematically change properties, such as valence, spin, and orbital degrees of freedom, as well as crystallographic geometry. Here, we demonstrate that ferromagnetism can be externally turned on with the application of low-energy helium implantation and can be subsequently erased and returned to the pristine state via annealing. This high level of continuous control is made possible by targeting magnetic metastability in the ultrahigh-conductivity, nonmagnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.

Monolayer Superconductivity and Tunable Topological Electronic Structure at the Fe(Te,Se)/Bi2 Te3 Interface.

The interface between 2D topological Dirac states and an s-wave superconductor is expected to support Majorana-bound states (MBS) that can be used for quantum computing applications. Realizing these novel states of matter and their applications requires control over superconductivity and spin-orbit coupling to achieve spin-momentum-locked topological interface states (TIS) which are simultaneously superconducting. While signatures of MBS have been observed in the magnetic vortex cores of bulk FeTe0.55 Se0.45 , inhomogeneity and disorder from doping make these signatures unclear and inconsistent between vortices. Here superconductivity is reported in monolayer (ML) FeTe1-y Sey (Fe(Te,Se)) grown on Bi2 Te3 by molecular beam epitaxy (MBE). Spin and angle-resolved photoemission spectroscopy (SARPES) directly resolve the interfacial spin and electronic structure of Fe(Te,Se)/Bi2 Te3 heterostructures. For y = 0.25, the Fe(Te,Se) electronic structure is found to overlap with the Bi2 Te3 TIS and the desired spin-momentum locking is not observed. In contrast, for y = 0.1, reduced inhomogeneity measured by scanning tunneling microscopy (STM) and a smaller Fe(Te,Se) Fermi surface with clear spin-momentum locking in the topological states are found. Hence, it is demonstrated that the Fe(Te,Se)/Bi2 Te3 system is a highly tunable platform for realizing MBS where reduced doping can improve characteristics important for Majorana interrogation and potential applications.

Superconducting Fourfold Fe(Te,Se) Film on Sixfold Magnetic MnTe via Hybrid Symmetry Epitaxy.

Epitaxial Fe(Te,Se) thin films have been grown on various substrates but never been grown on magnetic layers. Here we report the epitaxial growth of fourfold Fe(Te,Se) film on a sixfold antiferromagnetic insulator, MnTe. The Fe(Te,Se)/MnTe heterostructure shows a clear superconducting transition at around 11 K, and the critical magnetic field measurement suggests the origin of the superconductivity to be bulk-like. Structural characterizations suggest that the uniaxial lattice match between Fe(Te,Se) and MnTe allows a hybrid symmetry epitaxy mode, which was recently discovered between Fe(Te,Se) and Bi2Te3. Furthermore, the Te/Fe flux ratio during deposition of the Fe(Te,Se) layer is found to be critical for its superconductivity. Now that superconducting Fe(Te,Se) can be grown on two related hexagonal platforms, Bi2Te3 and MnTe, this result opens a new possibility of combining topological superconductivity of Fe(Te,Se) with the rich physics in the intrinsic magnetic topological materials (MnTe)n(Bi2Te3)m family.

Reversible Hydrogen-Induced Phase Transformations in La0.7Sr0.3MnO3 Thin Films Characterized by In Situ Neutron Reflectometry.

We report on the mechanism for hydrogen-induced topotactic phase transitions in perovskite (PV) oxides using La0.7Sr0.3MnO3 as a prototypical example. Hydrogenation starts with lattice expansion confirmed by X-ray diffraction (XRD). The strain- and oxygen-vacancy-mediated electron-phonon coupling in turn produces electronic structure changes that manifest through the appearance of a metal insulator transition accompanied by a sharp increase in resistivity. The ordering of initially randomly distributed oxygen vacancies produces a PV to brownmillerite phase (La0.7Sr0.3MnO2.5) transition. This phase transformation proceeds by the intercalation of oxygen vacancy planes confirmed by in situ XRD and neutron reflectometry (NR) measurements. Despite the prevailing picture that hydrogenation occurs by reaction with lattice oxygen, NR results are not consistent with deuterium (hydrogen) presence in the La0.7Sr0.3MnO3 lattice at steady state. The film can reach a highly oxygen-deficient La0.7Sr0.3MnO2.1 metastable state that is reversible to the as-grown composition simply by annealing in air. Theoretical calculations confirm that hydrogenation-induced oxygen vacancy formation is energetically favorable in La0.7Sr0.3MnO3. The hydrogenation-driven changes of the oxygen sublattice periodicity and the electrical and magnetic properties similar to interface effects induced by oxygen-deficient cap layers persist despite hydrogen not being present in the lattice.

Designing Magnetism in High Entropy Oxides.

In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder are lacking. Here, it is demonstrated that high entropy oxides present a previously unexplored route to designing materials in which the presence of strong local compositional disorder may be exploited to generate tunable magnetic behaviors-from macroscopically ordered states to frustration-driven dynamic spin interactions. Single-crystal La(Cr0.2 Mn0.2 Fe0.2 Co0.2 Ni0.2 )O3 films are used as a model system hosting a magnetic sublattice with a high degree of microstate disorder in the form of site-to-site spin and exchange type inhomogeneity. A classical Heisenberg model simplified to represent the highest probability microstates well describes how compositionally disordered systems can paradoxically host magnetic uniformity and demonstrates a path toward continuous control over ordering types and critical temperatures. Model-predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition, this leads to highly controllable exchange bias behaviors previously accessible only in intentionally designed bilayer heterojunctions.

High Entropy Oxide Relaxor Ferroelectrics.

Relaxor ferroelectrics are important in technological applications due to strong electromechanical response, energy storage capacity, electrocaloric effect, and pyroelectric energy conversion properties. Current efforts to discover and design materials in this class generally rely on substitutional doping as slight changes to local compositional order can significantly affect the Curie temperature, morphotropic phase boundary, and electromechanical responses. In this work, we demonstrate that moving to the strong limit of compositional complexity in an ABO3 perovskite allows stabilization of relaxor responses that do not rely on a single narrow phase transition region. Entropy-assisted synthesis approaches are utilized to synthesize single-crystal Ba(Ti0.2Sn0.2Zr0.2Hf0.2Nb0.2)O3 [Ba(5B)O] films. The high levels of configurational disorder present in this system are found to influence dielectric relaxation, phase transitions, nanopolar domain formation, and Curie temperature. Temperature-dependent dielectric, Raman spectroscopy, and second-harmonic generation measurements reveal multiple phase transitions, a high Curie temperature of 570 K, and the relaxor ferroelectric nature of Ba(5B)O films. The first-principles theory calculations are used to predict possible combinations of cations to design relaxor ferroelectrics and quantify the relative feasibility of synthesizing these highly disordered single-phase perovskite systems. The ability to stabilize single-phase perovskites with various cations on the B-sites offers possibilities for designing high-performance relaxor ferroelectric materials for piezoelectric, pyroelectric, and electrocaloric applications.

Hybrid Symmetry Epitaxy of the Superconducting Fe(Te,Se) Film on a Topological Insulator.

It is challenging to grow an epitaxial 4-fold compound superconductor (SC) on a 6-fold topological insulator (TI) platform due to the stringent lattice-matching requirement. Here, we demonstrate that Fe(Te,Se) can grow epitaxially on a TI (Bi2Te3) layer due to accidental, uniaxial lattice match, which is dubbed as "hybrid symmetry epitaxy". This new growth mode is critical to stabilizing robust superconductivity with TC as high as 13 K. Furthermore, the superconductivity in this FeTe1-xSex/Bi2Te3 system survives in the Te-rich phase with Se content as low as x = 0.03 but vanishes at Se content above x = 0.56, exhibiting a phase diagram that is quite different from that of the conventional Fe(Te,Se) systems. This unique heterostructure platform that can be formed in both TI-on-SC and SC-on-TI sequences opens a route to unprecedented topological heterostructures.

Magnetic Texture in Insulating Single Crystal High Entropy Oxide Spinel Films.

Magnetic insulators are important materials for a range of next-generation memory and spintronic applications. Structural constraints in this class of devices generally require a clean heterointerface that allows effective magnetic coupling between the insulating layer and the conducting layer. However, there are relatively few examples of magnetic insulators that can be synthesized with surface qualities that would allow these smooth interfaces and precisely tuned interfacial magnetic exchange coupling, which might be applicable at room temperature. In this work, we demonstrate an example of how the configurational complexity in the magnetic insulator layer can be used to realize these properties. The entropy-assisted synthesis is used to create single-crystal (Mg0.2Ni0.2Fe0.2Co0.2Cu0.2)Fe2O4 films on substrates spanning a range of strain states. These films show smooth surfaces, high resistivity, and strong magnetic responses at room temperature. Local and global magnetic measurements further demonstrate how strain can be used to manipulate the magnetic texture and anisotropy. These findings provide insight into how precise magnetic responses can be designed using compositionally complex materials that may find application in next-generation magnetic devices.

Criteria for Realizing Room-Temperature Electrical Transport Applications of Topological Materials.

The unusual electronic states found in topological materials can enable a new generation of devices and technologies, yet a long-standing challenge has been finding materials without deleterious parallel bulk conduction. This can arise either from defects or thermally activated carriers. Here, the criteria that materials need to meet to realize transport properties dominated by the topological states, a necessity for a topological device, are clarified. This is demonstrated for 3D topological insulators, 3D Dirac materials, and 1D quantum anomalous Hall insulators, though this can be applied to similar systems. The key parameters are electronic bandgap, dielectric constant, and carrier effective mass, which dictate under what circumstances (defect density, temperature, etc.) the unwanted bulk state will conduct in parallel to the topological states. As these are fundamentally determined by the basic atomic properties, simple chemical arguments can be used to navigate the phase space to ultimately find improved materials. This will enable rapid identification of new systems with improved properties, which is crucial to designing new material systems and push a new generation of topological technologies.

Interfacial tuning of chiral magnetic interactions for large topological Hall effects in LaMnO3/SrIrO3 heterostructures.

Chiral interactions in magnetic systems can give rise to rich physics manifested, for example, as nontrivial spin textures. The foremost interaction responsible for chiral magnetism is the Dzyaloshinskii-Moriya interaction (DMI), resulting from inversion symmetry breaking in the presence of strong spin-orbit coupling. However, the atomistic origin of DMIs and their relationship to emergent electrodynamic phenomena, such as topological Hall effect (THE), remain unclear. Here, we investigate the role of interfacial DMIs in 3d-5d transition metal-oxide-based LaMnO3/SrIrO3 superlattices on THE from a chiral spin texture. By additively engineering the interfacial inversion symmetry with atomic-scale precision, we directly link the competition between interfacial collinear ferromagnetic interactions and DMIs to an enhanced THE. The ability to control the DMI and resulting THE points to a pathway for harnessing interfacial structures to maximize the density of chiral spin textures useful for developing high-density information storage and quantum magnets for quantum information science.

Applying Configurational Complexity to the 2D Ruddlesden-Popper Crystal Structure.

The layered Ruddlesden-Popper crystal structure can host a broad range of functionally important behaviors. Here we establish extraordinary configurational disorder in a layered Ruddlesden-Popper (RP) structure using entropy stabilization assisted synthesis. A protype A2CuO4 RP cuprate oxide with five cations on the A-site sublattice is designed and fabricated into epitaxial single crystal films using pulsed laser deposition. When grown on a near lattice matched substrate, the (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)2CuO4 film features a T'-type RP structure with uniform A-site cation mixing and square-planar CuO4 units. These observations are made with a range of combined characterizations using X-ray diffraction, atomic-resolution scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray absorption spectroscopy measurements. It is further found that heteroepitaxial strain plays an important role in crystal phase formation during synthesis. Compressive strain over ∼1.5% results in the formation of a non-RP cubic phase consistent with a CuX2O4 spinel structure. The ability to manipulate configurational complexity and move between 2D layered RP and 3D cubic crystal structures in cuprate and related materials promises to enable flexible design strategies for a range of functionalities, such as magnetoresistance, unconventional superconductivity, ferroelectricity, catalysis, and ion transport.

Scaling growth rates for perovskite oxide virtual substrates on silicon.

The availability of native substrates is a cornerstone in the development of microelectronic technologies relying on epitaxial films. If native substrates are not available, virtual substrates - crystalline buffer layers epitaxially grown on a structurally dissimilar substrate - offer a solution. Realizing commercially viable virtual substrates requires the growth of high-quality films at high growth rates for large-scale production. We report the stoichiometric growth of SrTiO3 exceeding 600 nm hr-1. This tenfold increase in growth rate compared to SrTiO3 grown on silicon by conventional methods is enabled by a self-regulated growth window accessible in hybrid molecular beam epitaxy. Overcoming the materials integration challenge for complex oxides on silicon using virtual substrates opens a path to develop new electronic devices in the More than Moore era and silicon integrated quantum computation hardware.

Structural dynamics of LaVO3 on the nanosecond time scale.

Due to the strong dependence of electronic properties on the local bonding environment, a full characterization of the structural dynamics in ultrafast experiments is critical. Here, we report the dynamics and structural refinement at nanosecond time scales of a perovskite thin film by combining optical excitation with time-resolved X-ray diffraction. This is achieved by monitoring the temporal response of both integer and half-integer diffraction peaks of LaVO3 in response to an above-band-gap 800 nm pump pulse. We find that the lattice expands by 0.1% out of plane, and the relaxation is characterized by a biexponential decay with 2 and 12 ns time scales. We analyze the relative intensity change in half-integer peaks and show that the distortions to the substructure are small: the oxygen octahedral rotation angles decrease by ∼0.3° and La displacements decrease by ∼0.2 pm, which directly corresponds to an ∼0.8° increase in the V-O-V bond-angles, an in-plane V-O bond length reduction of ∼0.3 pm, and an unchanged out-of-plane bond length. This demonstration of tracking the atomic positions in a pump-probe experiment provides experimentally accessible values for structural and electronic tunability in this class of materials and will stimulate future experiments.

Continuously Tuning Epitaxial Strains by Thermal Mismatch.

Strain engineering of thin films is a conventionally employed approach to enhance material properties and to energetically prefer ground states that would otherwise not be attainable. Controlling strain states in perovskite oxide thin films is usually accomplished through coherent epitaxy by using lattice-mismatched substrates with similar crystal structures. However, the limited choice of suitable oxide substrates makes certain strain states experimentally inaccessible and a continuous tuning impossible. Here, we report a strategy to continuously tune epitaxial strains in perovskite films grown on Si(001) by utilizing the large difference of thermal expansion coefficients between the film and the substrate. By establishing an adsorption-controlled growth window for SrTiO3 thin films on Si using hybrid molecular beam epitaxy, the magnitude of strain can be solely attributed to thermal expansion mismatch, which only depends on the difference between growth and room temperature. Second-harmonic generation measurements revealed that structure properties of SrTiO3 films could be tuned by this method using films with different strain states. Our work provides a strategy to generate continuous strain states in oxide/semiconductor pseudomorphic buffer structures that could help achieve desired material functionalities.

Terahertz plasmonic excitations in Bi2Se3 topological insulator.

After the discovery of Dirac electrons in condensed matter physics, more specifically in graphene and its derivatives, their potentialities in the fields of plasmonics and photonics have been readily recognized, leading to a plethora of applications in active and tunable optical devices. Massless Dirac carriers have been further found in three-dimensional topological insulators. These exotic quantum systems have an insulating gap in the bulk and intrinsic Dirac metallic states at any surface, sustaining not only single-particle excitations but also plasmonic collective modes. In this paper we will review the plasmon excitations in different microstructures patterned on Bi2Se3 topological insulator thin films as measured by terahertz spectroscopy. We discuss the dependence of the plasmon absorption versus the microstructure shape, wavevector, and magnetic field. Finally we will discuss the topological protection of both the Dirac single-particle and plasmon excitations.

A novel artificial condensed matter lattice and a new platform for one-dimensional topological phases.

Engineered lattices in condensed matter physics, such as cold-atom optical lattices or photonic crystals, can have properties that are fundamentally different from those of naturally occurring electronic crystals. We report a novel type of artificial quantum matter lattice. Our lattice is a multilayer heterostructure built from alternating thin films of topological and trivial insulators. Each interface within the heterostructure hosts a set of topologically protected interface states, and by making the layers sufficiently thin, we demonstrate for the first time a hybridization of interface states across layers. In this way, our heterostructure forms an emergent atomic chain, where the interfaces act as lattice sites and the interface states act as atomic orbitals, as seen from our measurements by angle-resolved photoemission spectroscopy. By changing the composition of the heterostructure, we can directly control hopping between lattice sites. We realize a topological and a trivial phase in our superlattice band structure. We argue that the superlattice may be characterized in a significant way by a one-dimensional topological invariant, closely related to the invariant of the Su-Schrieffer-Heeger model. Our topological insulator heterostructure demonstrates a novel experimental platform where we can engineer band structures by directly controlling how electrons hop between lattice sites.

High-Quality LaVO3 Films as Solar Energy Conversion Material.

Mott insulating oxides and their heterostructures have recently been identified as potential photovoltaic materials with favorable absorption properties and an intrinsic built-in electric field that can efficiently separate excited electron-hole pairs. At the same time, they are predicted to overcome the Shockley-Queisser limit due to strong electron-electron interaction present. Despite these premises a high concentration of defects commonly observed in Mott insulating films acting as recombination centers can derogate the photovoltaic conversion efficiency. With use of the self-regulated growth kinetics in hybrid molecular beam epitaxy, this obstacle can be overcome. High-quality, stoichiometric LaVO3 films were grown with defect densities of in-gap states up to 2 orders of magnitude lower compared to the films in the literature, and a factor of 3 lower than LaVO3 bulk single crystals. Photoconductivity measurements revealed a significant photoresponsivity increase as high as tenfold of stoichiometric LaVO3 films compared to their nonstoichiometric counterparts. This work marks a critical step toward the realization of high-performance Mott insulator solar cells beyond conventional semiconductors.