Polar metals by geometric design.

Gauss's law dictates that the net electric field inside a conductor in electrostatic equilibrium is zero by effective charge screening; free carriers within a metal eliminate internal dipoles that may arise owing to asymmetric charge distributions. Quantum physics supports this view, demonstrating that delocalized electrons make a static macroscopic polarization, an ill-defined quantity in metals--it is exceedingly unusual to find a polar metal that exhibits long-range ordered dipoles owing to cooperative atomic displacements aligned from dipolar interactions as in insulating phases. Here we describe the quantum mechanical design and experimental realization of room-temperature polar metals in thin-film ANiO3 perovskite nickelates using a strategy based on atomic-scale control of inversion-preserving (centric) displacements. We predict with ab initio calculations that cooperative polar A cation displacements are geometrically stabilized with a non-equilibrium amplitude and tilt pattern of the corner-connected NiO6 octahedral--the structural signatures of perovskites--owing to geometric constraints imposed by the underlying substrate. Heteroepitaxial thin-films grown on LaAlO3 (111) substrates fulfil the design principles. We achieve both a conducting polar monoclinic oxide that is inaccessible in compositionally identical films grown on (001) substrates, and observe a hidden, previously unreported, non-equilibrium structure in thin-film geometries. We expect that the geometric stabilization approach will provide novel avenues for realizing new multifunctional materials with unusual coexisting properties.

Anisotropic spin-orbit torque generation in epitaxial SrIrO3 by symmetry design.

Spin-orbit coupling (SOC), the interaction between the electron spin and the orbital angular momentum, can unlock rich phenomena at interfaces, in particular interconverting spin and charge currents. Conventional heavy metals have been extensively explored due to their strong SOC of conduction electrons. However, spin-orbit effects in classes of materials such as epitaxial 5d-electron transition-metal complex oxides, which also host strong SOC, remain largely unreported. In addition to strong SOC, these complex oxides can also provide the additional tuning knob of epitaxy to control the electronic structure and the engineering of spin-to-charge conversion by crystalline symmetry. Here, we demonstrate room-temperature generation of spin-orbit torque on a ferromagnet with extremely high efficiency via the spin-Hall effect in epitaxial metastable perovskite SrIrO3 We first predict a large intrinsic spin-Hall conductivity in orthorhombic bulk SrIrO3 arising from the Berry curvature in the electronic band structure. By manipulating the intricate interplay between SOC and crystalline symmetry, we control the spin-Hall torque ratio by engineering the tilt of the corner-sharing oxygen octahedra in perovskite SrIrO3 through epitaxial strain. This allows the presence of an anisotropic spin-Hall effect due to a characteristic structural anisotropy in SrIrO3 with orthorhombic symmetry. Our experimental findings demonstrate the heteroepitaxial symmetry design approach to engineer spin-orbit effects. We therefore anticipate that these epitaxial 5d transition-metal oxide thin films can be an ideal building block for low-power spintronics.

Terahertz Second-Harmonic Generation from Lightwave Acceleration of Symmetry-Breaking Nonlinear Supercurrents.

We report terahertz (THz) light-induced second harmonic generation, in superconductors with inversion symmetry that forbid even-order nonlinearities. The THz second harmonic emission vanishes above the superconductor critical temperature and arises from precession of twisted Anderson pseudospins at a multicycle, THz driving frequency that is not allowed by equilibrium symmetry. We explain the microscopic physics by a dynamical symmetry breaking principle at sub-THz-cycle by using quantum kinetic modeling of the interplay between strong THz-lightwave nonlinearity and pulse propagation. The resulting nonzero integrated pulse area inside the superconductor leads to light-induced nonlinear supercurrents due to subcycle Cooper pair acceleration, in contrast to dc-biased superconductors, which can be controlled by the band structure and THz driving field below the superconducting gap.

Terahertz-light quantum tuning of a metastable emergent phase hidden by superconductivity.

'Sudden' quantum quench and prethermalization have become a cross-cutting theme for discovering emergent states of matter1-4. Yet this remains challenging in electron matter5-9, especially superconductors10-14. The grand question of what is hidden underneath superconductivity (SC) 15 appears universal, but poorly understood. Here we reveal a long-lived gapless quantum phase of prethermalized quasiparticles (QPs) after a single-cycle terahertz (THz) quench of a Nb3Sn SC gap. Its conductivity spectra is characterized by a sharp coherent peak and a vanishing scattering rate that decreases almost linearly towards zero frequency, which is most pronounced around the full depletion of the condensate and absent for a high-frequency pump. Above a critical pump threshold, such a QP phase with coherent transport and memory persists as an unusual prethermalization plateau, without relaxation to normal and SC thermal states for an order of magnitude longer than the QP recombination and thermalization times. Switching to this metastable 'quantum QP fluid' signals non-thermal quench of coupled SC and charge-density-wave (CDW)-like orders and hints quantum control beneath the SC.

Direct observation of a two-dimensional hole gas at oxide interfaces.

The discovery of a two-dimensional electron gas (2DEG) at the LaAlO3/SrTiO3 interface 1 has resulted in the observation of many properties2-5 not present in conventional semiconductor heterostructures, and so become a focal point for device applications6-8. Its counterpart, the two-dimensional hole gas (2DHG), is expected to complement the 2DEG. However, although the 2DEG has been widely observed 9 , the 2DHG has proved elusive. Herein we demonstrate a highly mobile 2DHG in epitaxially grown SrTiO3/LaAlO3/SrTiO3 heterostructures. Using electrical transport measurements and in-line electron holography, we provide direct evidence of a 2DHG that coexists with a 2DEG at complementary heterointerfaces in the same structure. First-principles calculations, coherent Bragg rod analysis and depth-resolved cathodoluminescence spectroscopy consistently support our finding that to eliminate ionic point defects is key to realizing a 2DHG. The coexistence of a 2DEG and a 2DHG in a single oxide heterostructure provides a platform for the exciting physics of confined electron-hole systems and for developing applications.

Observation of magnetic vortex pairs at room temperature in a planar α-Fe2O3/Co heterostructure.

Vortices, occurring whenever a flow field 'whirls' around a one-dimensional core, are among the simplest topological structures, ubiquitous to many branches of physics. In the crystalline state, vortex formation is rare, since it is generally hampered by long-range interactions: in ferroic materials (ferromagnetic and ferroelectric), vortices are observed only when the effects of the dipole-dipole interaction are modified by confinement at the nanoscale1-3, or when the parameter associated with the vorticity does not couple directly with strain 4 . Here, we observe an unprecedented form of vortices in antiferromagnetic haematite (α-Fe2O3) epitaxial films, in which the primary whirling parameter is the staggered magnetization. Remarkably, ferromagnetic topological objects with the same vorticity and winding number as the α-Fe2O3 vortices are imprinted onto an ultra-thin Co ferromagnetic over-layer by interfacial exchange. Our data suggest that the ferromagnetic vortices may be merons (half-skyrmions, carrying an out-of plane core magnetization), and indicate that the vortex/meron pairs can be manipulated by the application of an in-plane magnetic field, giving rise to large-scale vortex-antivortex annihilation.

Coherent Magnetoelastic Domains in Multiferroic BiFeO_{3} Films.

The physical properties of epitaxial films can fundamentally differ from those of bulk single crystals even above the critical thickness. By a combination of nonresonant x-ray magnetic scattering, neutron diffraction and vector-mapped x-ray magnetic linear dichroism photoemission electron microscopy, we show that epitaxial (111)-BiFeO_{3} films support submicron antiferromagnetic domains, which are magnetoelastically coupled to a coherent crystallographic monoclinic twin structure. This unique texture, which is absent in bulk single crystals, should enable control of magnetism in BiFeO_{3} film devices via epitaxial strain.

Mechanical Tuning of LaAlO3/SrTiO3 Interface Conductivity.

In recent years, complex-oxide heterostructures and their interfaces have become the focus of significant research activity, primarily driven by the discovery of emerging states and functionalities that open up opportunities for the development of new oxide-based nanoelectronic devices. The highly conductive state at the interface between insulators LaAlO3 and SrTiO3 is a prime example of such emergent functionality, with potential application in high electron density transistors. In this report, we demonstrate a new paradigm for voltage-free tuning of LaAlO3/SrTiO3 (LAO/STO) interface conductivity, which involves the mechanical gating of interface conductance through stress exerted by the tip of a scanning probe microscope. The mechanical control of channel conductivity and the long retention time of the induced resistance states enable transistor functionality with zero gate voltage.

Artificially engineered superlattices of pnictide superconductors.

Significant progress has been achieved in fabricating high-quality bulk and thin-film iron-based superconductors. In particular, artificial layered pnictide superlattices offer the possibility of tailoring the superconducting properties and understanding the mechanism of the superconductivity itself. For high-field applications, large critical current densities (J(c)) and irreversibility fields (H(irr)) are indispensable along all crystal directions. On the other hand, the development of superconducting devices such as tunnel junctions requires multilayered heterostructures. Here we show that artificially engineered undoped Ba-122/Co-doped Ba-122 compositionally modulated superlattices produce ab-aligned nanoparticle arrays. These layer and self-assemble along c-axis-aligned defects, and combine to produce very large J(c) and H(irr) enhancements over a wide angular range. We also demonstrate a structurally modulated SrTiO3(STO)/Co-doped Ba-122 superlattice with sharp interfaces. Success in superlattice fabrication involving pnictides will aid the progress of heterostructured systems exhibiting new interfacial phenomena and device applications.

Spin structure in an interfacially coupled epitaxial ferromagnetic oxide heterostructure.

We report the spin structure of an exchange-biased ferromagnetic oxide heterostructure, La(0.67)Sr(0.33)MnO(3)/SrRuO(3), through magnetization and polarized neutron reflectometry measurements. We reveal that the magnetization reversal process of the La(0.67)Sr(0.33)MnO(3) biased layer critically depends on the frozen-in spin structure of the SrRuO(3) biasing layer during the cooling process. Furthermore, we observe unexpected double-shifted hysteresis loops of the biased layer that originates from the formation of lateral 180° magnetic domains within the biasing layer, a new mechanism not found in conventional exchange-bias systems.

Temperature evolution of itinerant ferromagnetism in SrRuO3 probed by optical spectroscopy.

The temperature (T) dependence of the optical conductivity spectra σ(ω) of a single crystal SrRuO(3) thin film is studied over a T range from 5 to 450 K. We observed significant T dependence of the spectral weights of the charge transfer and interband d-d transitions across the ferromagnetic Curie temperature (T(c) ∼ 150 K). Such T dependence was attributed to the increase in the Ru spin moment, which is consistent with the results of density functional theory calculations. T scans of σ(Ω,T) at fixed frequencies Ω reveal a clear T(2) dependence below T(c), demonstrating that the Stoner mechanism is involved in the evolution of the electronic structure. In addition, σ(Ω,T) continues to evolve at temperatures above T(c), indicating that the local spin moment persists in the paramagnetic state. This suggests that SrRuO(3) is an intriguing oxide system with itinerant ferromagnetism.

Mechanically-induced resistive switching in ferroelectric tunnel junctions.

Recent advances in atomic-precision processing of oxide ferroelectrics-materials with a stable polarization that can be switched by an external electric field-have generated considerable interest due to rich physics associated with their fundamental properties and high potential for application in devices with enhanced functionality. One of the particularly promising phenomena is the tunneling electroresistance (TER) effect-polarization-dependent bistable resistance behavior of ferroelectric tunnel junctions (FTJ). Conventionally, the application of an electric field above the coercive field of the ferroelectric barrier is required to observe this phenomenon. Here, we report a mechanically induced TER effect in ultrathin ferroelectric films of BaTiO(3) facilitated by a large strain gradient induced by a tip of a scanning probe microscope (SPM). The obtained results represent a new paradigm for voltage-free control of electronic properties of nanoscale ferroelectrics and, more generally, complex oxide materials.

Ferroelectric tunnel memristor.

Strong interest in resistive switching phenomena is driven by a possibility to develop electronic devices with novel functional properties not available in conventional systems. Bistable resistive devices are characterized by two resistance states that can be switched by an external voltage. Recently, memristors-electric circuit elements with continuously tunable resistive behavior-have emerged as a new paradigm for nonvolatile memories and adaptive electronic circuit elements. Employment of memristors can radically enhance the computational power and energy efficiency of electronic systems. Most of the existing memristor prototypes involve transition metal oxide resistive layers where conductive filaments formation and/or the interface contact resistance control the memristive behavior. In this paper, we demonstrate a new type of memristor that is based on a ferroelectric tunnel junction, where the tunneling conductance can be tuned in an analogous manner by several orders of magnitude by both the amplitude and the duration of the applied voltage. The ferroelectric tunnel memristors exhibit a reversible hysteretic nonvolatile resistive switching with a resistance ratio of up to 10(5) % at room temperature. The observed memristive behavior is attributed to the field-induced charge redistribution at the ferroelectric/electrode interface, resulting in the modulation of the interface barrier height.

Switchable induced polarization in LaAlO3/SrTiO3 heterostructures.

Demonstration of a tunable conductivity of the LaAlO(3)/SrTiO(3) interfaces drew significant attention to the development of oxide electronic structures where electronic confinement can be reduced to the nanometer range. While the mechanisms for the conductivity modulation are quite different and include metal-insulator phase transition and surface charge writing, generally it is implied that this effect is a result of electrical modification of the LaAlO(3) surface (either due to electrochemical dissociation of surface adsorbates or free charge deposition) leading to the change in the two-dimensional electron gas (2DEG) density at the LaAlO(3)/SrTiO(3) (LAO/STO) interface. In this paper, using piezoresponse force microscopy we demonstrate a switchable electromechanical response of the LAO overlayer, which we attribute to the motion of oxygen vacancies through the LAO layer thickness. These electrically induced reversible changes in bulk stoichiometry of the LAO layer are a signature of a possible additional mechanism for nanoscale oxide 2DEG control on LAO/STO interfaces.

Spin injection/detection using an organic-based magnetic semiconductor.

The new paradigm of electronics, 'spintronics', promises to extend the functionality of information storage and processing in conventional electronics. The principal spintronics device, the 'spin valve', consists of two magnetic layers decoupled by a spin-transporting spacer, which allows parallel (on) and antiparallel (off) alignment of the magnetizations (spins) of the two magnetic layers. The device resistance then depends on the spin alignment controlled by the external magnetic field. In pursuit of semiconductor spintronics, there have been intensive efforts devoted to develop room-temperature magnetic semiconductors and also to incorporate both inorganic semiconductors and carbon-based materials as the spin-transporting channels. Molecule/organic-based magnets, which allow chemical tuning of electronic and magnetic properties, are a promising new class of magnetic materials for future spintronic applications. Here, we report the realization of an organic-based magnet as an electron spin polarizer in the standard spintronics device geometry. A thin non-magnetic organic semiconductor layer and an epitaxial ferromagnetic oxide film were employed to form a hybrid magnetic tunnel junction. The results demonstrate the spin-polarizing nature of the organic-based magnetic semiconductor, vanadium(TCNE: tetracyanoethylene)(x) (x approximately 2; T(c) approximately 400 K), and its function as a spin injector/detector in hybrid magnetic multilayer devices.

Ferroelastic switching for nanoscale non-volatile magnetoelectric devices.

Multiferroics, where (anti-) ferromagnetic, ferroelectric and ferroelastic order parameters coexist, enable manipulation of magnetic ordering by an electric field through switching of the electric polarization. It has been shown that realization of magnetoelectric coupling in a single-phase multiferroic such as BiFeO(3) requires ferroelastic (71 degrees, 109 degrees) rather than ferroelectric (180 degrees) domain switching. However, the control of such ferroelastic switching in a single-phase system has been a significant challenge as elastic interactions tend to destabilize small switched volumes, resulting in subsequent ferroelastic back-switching at zero electric field, and thus the disappearance of non-volatile information storage. Guided by our phase-field simulations, here we report an approach to stabilize ferroelastic switching by eliminating the stress-induced instability responsible for back-switching using isolated monodomain BiFeO(3) islands. This work demonstrates a critical step to control and use non-volatile magnetoelectric coupling at the nanoscale. Beyond magnetoelectric coupling, it provides a framework for exploring a route to control multiple order parameters coupled to ferroelastic order in other low-symmetry materials.

Template engineering of Co-doped BaFe2As2 single-crystal thin films.

Understanding new superconductors requires high-quality epitaxial thin films to explore intrinsic electromagnetic properties and evaluate device applications. So far, superconducting properties of ferropnictide thin films seem compromised by imperfect epitaxial growth and poor connectivity of the superconducting phase. Here we report new template engineering using single-crystal intermediate layers of (001) SrTiO(3) and BaTiO(3) grown on various perovskite substrates that enables genuine epitaxial films of Co-doped BaFe(2)As(2) with a high transition temperature (T(c,rho=0) of 21.5 K, where rho=resistivity), a small transition width (DeltaT(c)=1.3 K), a superior critical current density J(c) of 4.5 MA cm(-2) (4.2 K) and strong c-axis flux pinning. Implementing SrTiO(3) or BaTiO(3) templates to match the alkaline-earth layer in the Ba-122 with the alkaline-earth/oxygen layer in the templates opens new avenues for epitaxial growth of ferropnictides on multifunctional single-crystal substrates. Beyond superconductors, it provides a framework for growing heteroepitaxial intermetallic compounds on various substrates by matching interfacial layers between templates and thin-film overlayers.

Coherent Brillouin spectroscopy in a strongly scattering liquid by picosecond ultrasonics.

In a modification of a picosecond ultrasonic technique, a short acoustic pulse is launched into a liquid sample by a laser pulse absorbed in a semitransparent transducer film and is detected via coherent Brillouin scattering of a time-delayed probe pulse. With both excitation and probing performed from the transducer side, the arrangement is suitable for in vivo study of biological tissues. The signal is collected from a micrometer-thick layer next to the transducer and is not affected by the diffuse scattering of probe light deeper in the sample. The setup, utilizing a 33 nm thick single crystal SrRuO(3) transducer film, is tested on a full fat milk sample, with 11 GHz acoustic frequency recorded.

Coexistence of superconductivity and ferromagnetism in two dimensions.

Ferromagnetism is usually considered to be incompatible with conventional superconductivity, as it destroys the singlet correlations responsible for the pairing interaction. Superconductivity and ferromagnetism are known to coexist in only a few bulk rare-earth materials. Here we report evidence for their coexistence in a two-dimensional system: the interface between two bulk insulators, LaAlO(3) (LAO) and SrTiO(3) (STO), a system that has been studied intensively recently. Magnetoresistance, Hall, and electric-field dependence measurements suggest that there are two distinct bands of charge carriers that contribute to the interface conductivity. The sensitivity of properties of the interface to an electric field makes this a fascinating system for the study of the interplay between superconductivity and magnetism.

Light quantum control of persisting Higgs modes in iron-based superconductors.

The Higgs mechanism, i.e., spontaneous symmetry breaking of the quantum vacuum, is a cross-disciplinary principle, universal for understanding dark energy, antimatter and quantum materials, from superconductivity to magnetism. Unlike one-band superconductors (SCs), a conceptually distinct Higgs amplitude mode can arise in multi-band, unconventional superconductors  via strong interband Coulomb interaction, but is yet to be accessed. Here we discover such hybrid Higgs mode and demonstrate its quantum control by light in iron-based high-temperature SCs. Using terahertz (THz) two-pulse coherent spectroscopy, we observe a tunable amplitude mode coherent oscillation of the complex order parameter from coupled lower and upper bands. The nonlinear dependence of the hybrid Higgs mode on the THz driving fields is distinct from any known SC results: we observe a large reversible modulation of resonance strength, yet with a persisting mode frequency. Together with quantum kinetic modeling of a hybrid Higgs mechanism, distinct from charge-density fluctuations and without invoking phonons or disorder, our result provides compelling evidence for a light-controlled coupling between the electron and hole amplitude modes assisted by strong interband quantum entanglement. Such light-control of Higgs hybridization can be extended to probe many-body entanglement and hidden symmetries in other complex systems.