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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 SrTiO 3 exceeding 600 nm hr −1 . This tenfold increase in growth rate compared to SrTiO 3 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. A scalable method for the growth of perovskite oxides thin films on silicon is desirable for integration of buffer layers in devices. Here the authors demonstrate the stoichiometric growth of thin SrTiO 3 layers on silicon at high growth rates by hybrid molecular beam epitaxy.

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. 2D Weyl semimetals are spin-polarized analogues of graphene that promise access to various topological properties of matter. Here, the authors evidence spin-polarized Weyl cones, Weyl nodes, and Fermi strings in monolayer bismuthene.

Electrons with a linear energy/momentum dispersion are called massless Dirac electrons and represent the low-energy excitations in exotic materials such as graphene and topological insulators. Dirac electrons are characterized by notable properties such as a high mobility, a tunable density and, in topological insulators, a protection against backscattering through the spin–momentum locking mechanism. All those properties make graphene and topological insulators appealing for plasmonics applications. However, Dirac electrons are expected to present also a strong nonlinear optical behaviour. This should mirror in phenomena such as electromagnetic-induced transparency and harmonic generation. Here we demonstrate that in Bi 2 Se 3 topological insulator, an electromagnetic-induced transparency is achieved under the application of a strong terahertz electric field. This effect, concomitantly determined by harmonic generation and charge-mobility reduction, is exclusively related to the presence of Dirac electron at the surface of Bi 2 Se 3 , and opens the road towards tunable terahertz nonlinear optical devices based on topological insulator materials. The terahertz response of topological insulator surface states, in which relativistic electrons are protected from backscattering, possesses potential optic and plasmonic applications. Here, the authors demonstrate a nonlinear absorption response of Bi 2 Se 3 to terahertz electric fields.

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 SrVO 3 . 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 SrVO 3 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. A correlated material SrVO 3 has been considered to be a Fermi liquid, however previous studies have been limited to disordered samples. Here the authors study transport in ultraclean films of SrVO 3 , finding deviations from the Fermi liquid picture.

Modulating light via coherent charge oscillations in solids is the subject of intense research topics in opto-plasmonics. Although a variety of methods are proposed to increase such modulation efficiency, one central challenge is to achieve a high modulation depth (defined by a ratio of extinction with/without light) under small photon-flux injection, which becomes a fundamental trade-off issue both in metals and semiconductors. Here, by fabricating simple micro-ribbon arrays of topological insulator Bi 2 Se 3 , we report an unprecedentedly large modulation depth of 2,400% at 1.5 THz with very low optical fluence of 45 μJ cm −2 . This was possible, first because the extinction spectrum is nearly zero due to the Fano-like plasmon–phonon-destructive interference, thereby contributing an extremely small denominator to the extinction ratio. Second, the numerator of the extinction ratio is markedly increased due to the photoinduced formation of massive two-dimensional electron gas below the topological surface states, which is another contributor to the ultra-high modulation depth. For optical control of plasmons metals require a large amount of power in the control pulse, yielding a small modulation depth. Here, Sim et al. fabricate arrays of Bi 2 Se 3 and report a modulation depth of 2,400% at 1.5 THz with an optical fluence of 45 μJ/cm 2 , demonstrating a novel route for controlling plasmons.

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(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)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 oxides provide a previously unexplored route to designing magnetic behaviors not possible in less complex materials. Theoretical predictive models are developed and used to inform single‐crystal film synthesis to gain continuously tunable access to a full range of magnetic states—from antiferromagnetism to ferromagnetism to frustrated dynamical magnetism.

High quality thin films of topological insulators （TI） such as Bi2Se3 have been successfully synthesized by molecular beam epitaxy （MBE）. Although the surface of MBE films can be protected by capping with inert materials such as amorphous Se, restoring an atomically clean pristine surface after decapping has never been demonstrated, which prevents in-depth investigations of the intrinsic properties of TI thin films with ex situ tools. Using high resolution scanning tunneling microscopy/spectroscopy （STM/STS）, we demonstrate a simple and highly reproducible Se decapping method that allows recovery of the pristine surface of extremely high quality Bi2Se3 thin films grown and capped with Se in a separate MBE system then exposed to the atmosphere during transfer into the STM system. The crucial step of our decapping process is the removal of the surface contaminants on top of amorphous Se before thermal desorption of Se at a mild temperature （-210 ~C）. This effective Se decapping process opens up the possibility of ex situ characterizations of pristine surfaces of interesting selenide materials and beyond using cutting-edge techniques.

When a three-dimensional material is constructed by stacking different two-dimensional layers into an ordered structure, new and unique physical properties can emerge. An example is the delafossite PdCoO 2 , which consists of alternating layers of metallic Pd and Mott-insulating CoO 2 sheets. To understand the nature of the electronic coupling between the layers that gives rise to the unique properties of PdCoO 2 , we revealed its layer-resolved electronic structure combining standing-wave X-ray photoemission spectroscopy and ab initio many-body calculations. Experimentally, we have decomposed the measured VB spectrum into contributions from Pd and CoO 2 layers. Computationally, we find that many-body interactions in Pd and CoO 2 layers are highly different. Holes in the CoO 2 layer interact strongly with charge-transfer excitons in the same layer, whereas holes in the Pd layer couple to plasmons in the Pd layer. Interestingly, we find that holes in states hybridized across both layers couple to both types of excitations (charge-transfer excitons or plasmons), with the intensity of photoemission satellites being proportional to the projection of the state onto a given layer. This establishes satellites as a sensitive probe for inter-layer hybridization. These findings pave the way towards a better understanding of complex many-electron interactions in layered quantum materials. PdCoO 2 belongs to a class of materials where both weakly and strongly correlated electrons co-exist side-by-side in different layers of the crystal structure. Here, the authors investigate PdCoO 2 using standing wave photoemission spectroscopy and many-body calculations reporting layer-specific details about the electronic structure.

Quantum materials with novel spin textures from strong spin‐orbit coupling (SOC) are essential components for a wide array of proposed spintronic devices. Topological insulators have a necessary strong SOC that imposes a unique spin texture on topological states and Rashba states that arise on the boundary, but there is no established methodology to control the spin texture reversibly. Here, it is demonstrated that functionalizing Bi2Se3 films by altering the step‐edge termination directly changes the strength of SOC and thereby modifies the Rashba strength of 1D edge states. Scanning tunneling microscopy/spectroscopy shows that these Rashba edge states arise and subsequently vanish through the Se functionalization and reduction process of the step edges. The observations are corroborated by density functional theory calculations, which show that a subtle chemical change of edge termination fundamentally alters the underlying electronic structure. Importantly, fully reversible and repeatable switching of Rashba edge states across multiple cycles at room temperature is experimentally demonstrated. The results imply Se functionalization as a practical method to control SOC and spin texture of quantum states in topological insulators. The Rashba edge states at the step edges of Bi2Se3 display switching behavior, according to the functionalization and defunctionalization of step edges with Se atoms that are achieved by annealing in UHV and Se flux conditions, respectively.

Developing novel lead‐free ferroelectric materials is crucial for next‐generation microelectronic technologies that are energy efficient and environment friendly. However, materials discovery and property optimization are typically time‐consuming due to the limited throughput of traditional synthesis methods. In this work, we use a high‐throughput combinatorial synthesis approach to fabricate lead‐free ferroelectric superlattices and solid solutions of (Ba0.7Ca0.3)TiO3 (BCT) and Ba(Zr0.2Ti0.8)O3 (BZT) phases with continuous variation of composition and layer thickness. High‐resolution x‐ray diffraction (XRD) and analytical scanning transmission electron microscopy (STEM) demonstrate high film quality and well‐controlled compositional gradients. Ferroelectric and dielectric property measurements identify the “optimal property point” achieved at the composition of 48BZT–52BCT. Displacement vector maps reveal that ferroelectric domain sizes are tunable by varying BCT–BZTN superlattice geometry. This high‐throughput synthesis approach can be applied to many other material systems to expedite new materials discovery and properties optimization, allowing for the exploration of a large area of phase space within a single growth. A high‐throughput combinatorial pulsed laser deposition (cPLD) technique is used to grow BCT–BZT ferroelectric thin films with superlattice structure and mixed solid solution phase. Location‐dependent properties measurement results enable the selection of the “optimal property point” of the nanocomposite films and identify its phase transition composition from a single specimen. This cPLD approach can be applied many other materials systems to expedite the materials discovery and property optimization processes.