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.

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.

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.

Correlated metals as transparent conductors.

The fundamental challenge for designing transparent conductors used in photovoltaics, displays and solid-state lighting is the ideal combination of high optical transparency and high electrical conductivity. Satisfying these competing demands is commonly achieved by increasing carrier concentration in a wide-bandgap semiconductor with low effective carrier mass through heavy doping, as in the case of tin-doped indium oxide (ITO). Here, an alternative design strategy for identifying high-conductivity, high-transparency metals is proposed, which relies on strong electron-electron interactions resulting in an enhancement in the carrier effective mass. This approach is experimentally verified using the correlated metals SrVO3 and CaVO3, which, despite their high carrier concentration (>2.2 × 10(22) cm(-3)), have low screened plasma energies (<1.33 eV), and demonstrate excellent performance when benchmarked against ITO. A method is outlined to rapidly identify other candidates among correlated metals, and strategies are proposed to further enhance their performance, thereby opening up new avenues to develop transparent conductors.

Finite-Size and Composition-Driven Topological Phase Transition in (Bi1-xInx)2Se3 Thin Films.

In a topological insulator (TI), if its spin-orbit coupling (SOC) strength is gradually reduced, the TI eventually transforms into a trivial insulator beyond a critical point of SOC, at which point the bulk gap closes: this is the standard description of the topological phase transition (TPT). However, this description of TPT, driven solely by the SOC (or something equivalent) and followed by closing and reopening of the bulk band gap, is valid only for infinite-size samples, and little is known how TPT occurs for finite-size samples. Here, using both systematic transport measurements on interface-engineered (Bi1-xInx)2Se3 thin films and theoretical simulations (with animations in the Supporting Information), we show that description of TPT in finite-size samples needs to be substantially modified from the conventional picture of TPT due to surface-state hybridization and bulk confinement effects. We also show that the finite-size TPT is composed of two separate transitions, topological-normal transition (TNT) and metal-insulator transition (MIT), by providing a detailed phase diagram in the two-dimensional phase space of sample size and SOC strength.

Record Surface State Mobility and Quantum Hall Effect in Topological Insulator Thin Films via Interface Engineering.

Material defects remain as the main bottleneck to the progress of topological insulators (TIs). In particular, efforts to achieve thin TI samples with dominant surface transport have always led to increased defects and degraded mobilities, thus making it difficult to probe the quantum regime of the topological surface states. Here, by utilizing a novel buffer layer scheme composed of an In2Se3/(Bi0.5In0.5)2Se3 heterostructure, we introduce a quantum generation of Bi2Se3 films with an order of magnitude enhanced mobilities than before. This scheme has led to the first observation of the quantum Hall effect in Bi2Se3.

Topological Surface States Originated Spin-Orbit Torques in Bi(2)Se(3).

The three dimensional topological insulator bismuth selenide (Bi(2)Se(3)) is expected to possess strong spin-orbit coupling and spin-textured topological surface states and, thus, exhibit a high charge to spin current conversion efficiency. We evaluate spin-orbit torques in Bi(2)Se(3)/Co(40)Fe(40)B(20) devices at different temperatures by spin torque ferromagnetic resonance measurements. As the temperature decreases, the spin-orbit torque ratio increases from ∼0.047 at 300 K to ∼0.42 below 50 K. Moreover, we observe a significant out-of-plane torque at low temperatures. Detailed analysis indicates that the origin of the observed spin-orbit torques is topological surface states in Bi(2)Se(3). Our results suggest that topological insulators with strong spin-orbit coupling could be promising candidates as highly efficient spin current sources for exploring the next generation of spintronic applications.

Transferring MBE-grown topological insulator films to arbitrary substrates and metal-insulator transition via Dirac gap.

Mechanical exfoliation of bulk crystals has been widely used to obtain thin topological insulator (TI) flakes for device fabrication. However, such a process produces only microsized flakes that are highly irregular in shape and thickness. In this work, we developed a process to transfer the entire area of TI Bi2Se3 thin films grown epitaxially on Al2O3 and SiO2 to arbitrary substrates, maintaining their pristine morphology and crystallinity. Transport measurements show that these transferred films have lower carrier concentrations and comparable or higher mobilities than before the transfer. Furthermore, using this process we demonstrated a clear metal-insulator transition in an ultrathin Bi2Se3 film by gate-tuning its Fermi level into the hybridization gap formed at the Dirac point. The ability to transfer large area TI films to any substrate will facilitate fabrication of TI heterostructure devices, which will help explore exotic phenomena such as Majorana fermions and topological magnetoelectricity.

Emergence of decoupled surface transport channels in bulk insulating Bi(2)Se(3) thin films.

In ideal topological insulator (TI) films the bulk state, which is supposed to be insulating, should not provide any electric coupling between the two metallic surfaces. However, transport studies on existing TI films show that the topological states on opposite surfaces are electrically tied to each other at thicknesses far greater than the direct coupling limit where the surface wave functions overlap. Here, we show that as the conducting bulk channels are suppressed, the parasitic coupling effect diminishes, and the decoupled surface channels emerge as expected for ideal TIs. In Bi(2)Se(3) thin films with fully suppressed bulk states, the two surfaces, which are directly coupled below ∼10 QL, become gradually isolated with increasing thickness and are completely decoupled beyond ∼20 QL. On such a platform, it is now feasible to implement transport devices whose functionality relies on accessing the individual surface layers without any deleterious coupling effects.

Hidden transport phenomena in an ultraclean correlated metal.

Advancements in materials synthesis have been key to unveil the quantum nature of electronic properties in solids by providing experimental reference points for a correct theoretical description. Here, we report hidden transport phenomena emerging in the ultraclean limit of the archetypical correlated electron system SrVO3. The low temperature, low magnetic field transport was found to be dominated by anisotropic scattering, whereas, at high temperature, we find a yet undiscovered phase that exhibits clear deviations from the expected Landau Fermi liquid, which is reminiscent of strange-metal physics in materials on the verge of a Mott transition. Further, the high sample purity enabled accessing the high magnetic field transport regime at low temperature, which revealed an anomalously high Hall coefficient. Taken with the strong anisotropic scattering, this presents a more complex picture of SrVO3 that deviates from a simple Landau Fermi liquid. These hidden transport anomalies observed in the ultraclean limit prompt a theoretical reexamination of this canonical correlated electron system beyond the Landau Fermi liquid paradigm, and more generally serves as an experimental basis to refine theoretical methods to capture such nontrivial experimental consequences emerging in correlated electron systems.

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.

Interplay between Topological States and Rashba States as Manifested on Surface Steps at Room Temperature.

The unique spin texture of quantum states in topological materials underpins many proposed spintronic applications. However, realizations of such great potential are stymied by perturbations, such as temperature and local fields imposed by impurities and defects, that can render a promising quantum state uncontrollable. Here, we report room-temperature scanning tunneling microscopy/spectroscopy observation of interaction between Rashba states and topological surface states, which manifests local electronic structure along step edges controllable by the layer thickness of thin films. The first-principles theoretical calculation elucidates the robust Rashba states coexisting with topological surface states along the surface steps with characteristic spin textures in momentum space. Furthermore, the Rashba edge states can be switched off by reducing the thickness of a topological insulator Bi2Se3 to bolster their interaction with the hybridized topological surface states. The study unveils a manipulating mechanism of the spin textures at room temperature, reinforcing the necessity of thin film technology in controlling the quantum states.

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, a new approach is reported for increasing the superconducting transition temperature ( T C onset ) $( {T_{\mathrm{C}}^{{\mathrm{onset}}}} )$ 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 onset $T_{\mathrm{C}}^{{\mathrm{onset}}}$ 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 onset $T_{\mathrm{C}}^{{\mathrm{onset}}}$ 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.

Realization of a two-dimensional Weyl semimetal and topological Fermi strings.

A two-dimensional (2D) Weyl semimetal, akin to a spinful variant of graphene, represents a topological matter characterized by Weyl fermion-like quasiparticles in low dimensions. The spinful linear band structure in two dimensions gives rise to distinctive topological properties, accompanied by the emergence of Fermi string edge states. We report the experimental realization of a 2D Weyl semimetal, bismuthene monolayer grown on SnS(Se) substrates. Using spin and angle-resolved photoemission and scanning tunneling spectroscopies, we directly observe spin-polarized Weyl cones, Weyl nodes, and Fermi strings, providing consistent evidence of their inherent topological characteristics. Our work opens the door for the experimental study of Weyl fermions in low-dimensional materials.

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.

Thickness-independent transport channels in topological insulator Bi(2)Se(3) thin films.

With high quality topological insulator Bi(2)Se(3) thin films, we report thickness-independent transport properties over wide thickness ranges. Conductance remained nominally constant as the sample thickness changed from 256 to ∼8 QL (where QL refers to quintuple layer, 1 QL≈1 nm). Two surface channels of very different behaviors were identified. The sheet carrier density of one channel remained constant at ∼3.0×10(13) cm(-2) down to 2 QL, while the other, which exhibited quantum oscillations, remained constant at ∼8×10(12) cm(-2) only down to ∼8 QL. The weak antilocalization parameters also exhibited similar thickness independence. These two channels are most consistent with the topological surface states and the surface accumulation layers, respectively.

Topological-metal to band-insulator transition in (Bi(1-x)In(x))2Se3 thin films.

By combining transport and photoemission measurements on (Bi(1-x)In(x))(2)Se(3) thin films, we report that this system transforms from a topologically nontrivial metal into a topologically trivial band insulator through three quantum phase transitions. At x ≈ 3%-7%, there is a transition from a topologically nontrivial metal to a trivial metal. At x ≈ 15%, the metal becomes a variable-range-hopping insulator. Finally, above x ≈ 25%, the system becomes a true band insulator with its resistance immeasurably large even at room temperature. This material provides a new venue to investigate topologically tunable physics and devices with seamless gating or tunneling insulators.

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.

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.