Superconductivity in Freestanding Infinite-Layer Nickelate Membranes.

The observation of superconductivity in infinite-layer nickelates has attracted significant attention due to its potential as a new platform for exploring high-Tc superconductivity. However, thus far, superconductivity has only been observed in epitaxial thin films, which limits the manipulation capabilities and modulation methods compared to two-dimensional exfoliated materials. Given the exceptionally giant strain tunability and stacking capability of freestanding membranes, separating superconducting nickelates from the as-grown substrate is a novel way to engineer the superconductivity and uncover the underlying physics. Herein, this work reports the synthesis of the superconducting freestanding La0.8Sr0.2NiO2 membranes ( T c zero = 10.6 K ${T}_{\mathrm{c}}^{\mathrm{zero}}\ =\ 10.6\ \mathrm{K}$ ), emphasizing the crucial roles of the interface engineering in the precursor phase film growth and the quick transfer process in achieving superconductivity. This work offers a new versatile platform for investigating superconductivity in nickelates, such as the pairing symmetry via constructing Josephson tunneling junctions and higher Tc values via high-pressure experiments.

Tip-induced nanoscale domain engineering in x-cut lithium niobate on insulator.

Nanodomain engineering in lithium niobate on insulator (LNOI) is critical to realize advanced photonic circuits. Here, we investigate the tip-induced nanodomain formation in x-cut LNOI. The effective electric field exhibits a mirror symmetry, which can be divided into preceding and sequential halves according to the tip movement. Under our configuration, the preceding electric field plays a decisive role rather than the sequential one as in previous reports. The mechanism is attributed to the screening field formed by the preceding field counteracting the effect of the subsequent one. In experiment, we successfully fabricate nanodomain dots, lines, and periodic arrays. Our work offers a useful approach for nanoscale domain engineering in x-cut LNOI, which has potential applications in integrated optoelectronic devices.

In Situ Preparation of Superconducting Infinite-Layer Nickelate Thin Films with Atomically Flat Surface.

Since their discovery, the infinite-layer nickelates have been regarded as an appealing system for gaining deeper insights into high-temperature superconductivity (HTSC). However, the synthesis of superconducting samples has been proven to be challenging. Here, an ultrahigh vacuum (UHV) in situ ${\mathrm{\text{in situ}}}$ reduction method is developed using atomic hydrogen as a reducing agent and is applied in the lanthanum nickelate system. The reduction parameters, including the reduction temperature (TR) and hydrogen pressure (PH), are systematically explored. It is found that the reduction window for achieving superconducting transition is quite wide, reaching nearly 80°C in TR and three orders of magnitude in PH when the reduction time is set to 30 min. And there exists an optimal PH for achieving the highest Tc if both TR and reduction time are fixed. More prominently, as confirmed by atomic force microscopy and scanning transmission electron microscopy, the atomically flat surface can be preserved during the in situ ${\mathrm{\text{in situ}}}$ reduction process, providing advantages over the ex situ ${\mathrm{\text{ex situ}}}$ CaH2 method for surface-sensitive experiments.

Sr4Al2O7: A New Sacrificial Layer with High Water Dissolution Rate for the Synthesis of Freestanding Oxide Membranes.

Freestanding perovskite oxide membranes have drawn great attention recently since they offer exceptional structural tunability and stacking ability, providing new opportunities in fundamental research and potential device applications in silicon-based semiconductor technology. Among different types of sacrificial layers, the (Ca, Sr, Ba)3Al2O6 compounds are most widely used since they can be dissolved in water and prepare high-quality perovskite oxide membranes with clean and sharp surfaces and interfaces; However, the typical transfer process takes a long time (up to hours) in obtaining millimeter-size freestanding membranes, let alone realize wafer-scale samples with high yield. Here, a new member of the SrO-Al2O3 family, Sr4Al2O7 is introduced, and its high dissolution rate, ≈10 times higher than that of Sr3Al2O6 is demonstrated. The high-dissolution-rate of Sr4Al2O7 is most likely related to the more discrete Al-O networks and higher concentration of water-soluble Sr-O species in this compound. This work significantly facilitates the preparation of freestanding membranes and sheds light on the integration of multifunctional perovskite oxides in practical electronic devices.

Fabrication of 100-nm-period domain structure in lithium niobate on insulator.

Lithium niobate on insulator (LNOI) is a powerful platform for integrated photonic circuits. Recently, advanced applications in nonlinear and quantum optics require to controllably fabricate nano-resolution domain structures in LNOI. Here, we report on the fabrication of stable domain structures with sub-100 nm feature size through piezoelectric force microscopy (PFM) tip poling in a z-cut LNOI. In experiment, the domain dot with an initial diameter of 80 nm and the domain line with an initial width of 50 nm can survive after a storage of more than 3 months. Particularly, we demonstrate the successful fabrication of 1D stable domain array with a period down to 100 nm and a duty cycle of ∼50%. Our method paves the way to precisely manipulate frequency conversion and quantum entanglement on an LNOI chip.

A Bifunctional Optoelectronic Device for Photodetection and Photoluminescence Switching Based on Graphene/ZnTe/Graphene van der Waals Heterostructures.

Controlling the dynamic processes, such as generation, separation, transport, and recombination, of photoexcited carriers in a semiconductor is foundational in the design of various devices for optoelectronic applications. One may imagine that if different processes can be manipulated in one single device and thus generate useful signals, a multifunctional device can be realized, and the toolbox for integrated optoelectronics will be expanded. Here, we revealed that in a graphene/ZnTe/graphene van der Waals (vdW) heterostructure, the carriers can be generated by illumination from visible to infrared frequencies, and thus, the detected spectrum range extends to the communication band, well beyond the band gap of ZnTe (2.26 eV). More importantly, we are able to control the competition between separation and recombination of the photoexcited carriers by an electric bias along the thickness-defined channel of the ZnTe flake: as the bias increases, the photodetecting performance, e.g. response speed and photocurrent, are improved due to the efficient separation of carriers; synchronously, the photoluminescence (PL) intensity decreases and even switches off due to the suppressed recombination process. The ZnTe-based vdW heterostructure device thus integrates both photodetection and PL switching functions by manipulating the generation, separation, transport, and recombination of carriers, which may inspire the design of the next generation of miniaturized optoelectronic devices based on the vdW heterostructures made by various thin flakes.

Stacking transfer of wafer-scale graphene-based van der Waals superlattices.

High-quality graphene-based van der Waals superlattices are crucial for investigating physical properties and developing functional devices. However, achieving homogeneous wafer-scale graphene-based superlattices with controlled twist angles is challenging. Here, we present a flat-to-flat transfer method for fabricating wafer-scale graphene and graphene-based superlattices. The aqueous solution between graphene and substrate is removed by a two-step spinning-assisted dehydration procedure with the optimal wetting angle. Proton-assisted treatment is further used to clean graphene surfaces and interfaces, which also decouples graphene and neutralizes the doping levels. Twist angles between different layers are accurately controlled by adjusting the macroscopic stacking angle through their wafer flats. Transferred films exhibit minimal defects, homogeneous morphology, and uniform electrical properties over wafer scale. Even at room temperature, robust quantum Hall effects are observed in graphene films with centimetre-scale linewidth. Our stacking transfer method can facilitate the fabrication of graphene-based van der Waals superlattices and accelerate functional device applications.

Growth of wafer-scale chromium sulphide and selenide semiconductor films.

Two-dimensional (2D) transition metal chalcogenides have attracted enormous attention due to their stunning properties and great prospects for applications. Most of the reported 2D materials have layered structure, and non-layered transition metal chalcogenides are rare. Particularly, chromium chalcogenides are highly complexed in terms of structural phases. Researches on their representative chalcogenides, Cr2S3and Cr2Se3, are insufficient and most of them focus on individual crystal grains. In this study, large-scale Cr2S3and Cr2Se3films with controllable thickness are successfully grown, and their crystalline qualities are confirmed by multiple characterizations. Moreover, the thickness-dependent Raman vibrations are investigated systematically, presenting slight redshift with increasing thickness. The fundamental physical properties of grown Cr2S3and Cr2Se3films, including optical bandgap, activation energy and electrical properties, are measured with different thicknesses. The 1.9 nm thick Cr2S3and Cr2Se3films show narrow optical bandgap of 0.732 and 0.672 eV, respectively. The electrical properties of Cr2S3films demonstratep-type semiconductor behaviours, while the Cr2Se3films exhibit no gate response. This work can provide a feasible method for growing large-scale Cr2S3and Cr2Se3films, and reveal fundamental information of their physical properties, which is helpful for future applications.

Evidence for Anisotropic Superconductivity Beyond Pauli Limit in Infinite-Layer Lanthanum Nickelates.

After being expected to be a promising analog to cuprates for decades, superconductivity has recently been discovered in infinite-layer nickelates, providing new opportunities to explore mechanisms of high-temperature superconductivity. However, in sharp contrast to the single-band and anisotropic superconductivity in cuprates, nickelates exhibit a multi-band electronic structure and an unexpected isotropic superconductivity as reported recently, which challenges the cuprate-like picture in nickelates. Here, it is shown that strong anisotropic magnetotransport behaviors exist in La-based nickelate films with enhanced crystallinity and superconductivity ( T c onset $T_{\rm{c}}^{{\rm{onset}}}$ = 18.8 K, T c zero $T_{\rm{c}}^{{\rm{zero}}}$ = 16.5 K). The upper critical fields are anisotropic and violate the estimated Bardeen-Cooper-Schrieffer (BCS) Pauli limit ( H Pauli , µ = 1 µ B = 1.86 × T c , H = 0 ${H}_{\mathrm{Pauli},\mu =1{\mu}_{B}}=1.86\ensuremath{\times{}}{T}_{\mathrm{c},H=0}$ ) for in-plane magnetic fields. Moreover, the anisotropic superconductivity is further manifested by the cusp-like peak of the angle-dependent Tc and the vortex motion anisotropy under external magnetic fields.

Prominent Size Effects without a Depolarization Field Observed in Ultrathin Ferroelectric Oxide Membranes.

The increasing miniaturization of electronics requires a better understanding of material properties at the nanoscale. Many studies have shown that there is a ferroelectric size limit in oxides, below which the ferroelectricity will be strongly suppressed due to the depolarization field, and whether such a limit still exists in the absence of the depolarization field remains unclear. Here, by applying uniaxial strain, we obtain pure in-plane polarized ferroelectricity in ultrathin SrTiO_{3} membranes, providing a clean system with high tunability to explore ferroelectric size effects especially the thickness-dependent ferroelectric instability with no depolarization field. Surprisingly, the domain size, ferroelectric transition temperature, and critical strain for room-temperature ferroelectricity all exhibit significant thickness dependence. These results indicate that the stability of ferroelectricity is suppressed (enhanced) by increasing the surface or bulk ratio (strain), which can be explained by considering the thickness-dependent dipole-dipole interactions within the transverse Ising model. Our study provides new insights into ferroelectric size effects and sheds light on the applications of ferroelectric thin films in nanoelectronics.

Tuning Piezoelectricity via Thermal Annealing at a Freestanding Ferroelectric Membrane.

Tuning the ferroelectric domain structure by a combination of elastic and electrostatic engineering provides an effective route for enhanced piezoelectricity. However, for epitaxial thin films, the clamping effect imposed by the substrate does not allow aftergrowth tuning and also limits the electromechanical response. In contrast, freestanding membranes, which are free of substrate constraints, enable the tuning of a subtle balance between elastic and electrostatic energies, giving new platforms for enhanced and tunable functionalities. Here, highly tunable piezoelectricity is demonstrated in freestanding PbTiO3 membranes, by varying the ferroelectric domain structures from c-dominated to c/a and a domains via aftergrowth thermal treatment. Significantly, the piezoelectric coefficient of the c/a domain structure is enhanced by a factor of 2.5 compared with typical c domain PbTiO3. This work presents a new strategy to manipulate the piezoelectricity in ferroelectric membranes, highlighting their great potential for nano actuators, transducers, sensors and other NEMS device applications.

Approaching the quantum limit in two-dimensional semiconductor contacts.

The development of next-generation electronics requires scaling of channel material thickness down to the two-dimensional limit while maintaining ultralow contact resistance1,2. Transition-metal dichalcogenides can sustain transistor scaling to the end of roadmap, but despite a myriad of efforts, the device performance remains contact-limited3-12. In particular, the contact resistance has not surpassed that of covalently bonded metal-semiconductor junctions owing to the intrinsic van der Waals gap, and the best contact technologies are facing stability issues3,7. Here we push the electrical contact of monolayer molybdenum disulfide close to the quantum limit by hybridization of energy bands with semi-metallic antimony ([Formula: see text]) through strong van der Waals interactions. The contacts exhibit a low contact resistance of 42 ohm micrometres and excellent stability at 125 degrees Celsius. Owing to improved contacts, short-channel molybdenum disulfide transistors show current saturation under one-volt drain bias with an on-state current of 1.23 milliamperes per micrometre, an on/off ratio over 108 and an intrinsic delay of 74 femtoseconds. These performances outperformed equivalent silicon complementary metal-oxide-semiconductor technologies and satisfied the 2028 roadmap target. We further fabricate large-area device arrays and demonstrate low variability in contact resistance, threshold voltage, subthreshold swing, on/off ratio, on-state current and transconductance13. The excellent electrical performance, stability and variability make antimony ([Formula: see text]) a promising contact technology for transition-metal-dichalcogenide-based electronics beyond silicon.

Synthesis of Oxide Interface-Based Two-Dimensional Electron Gas on Si.

Two-dimensional electron gas (2DEG) at the interface of amorphous Al2O3/SrTiO3 (aAO/STO) heterostructures has received considerable attention owing to its convenience of fabrication and relatively high mobility. The integration of these 2DEG heterostructures on a silicon wafer is highly desired for electronic applications but remains challanging up to date. Here, conductive aAO/STO heterostructures have been synthesized on a silicon wafer via a growth-and-transfer method. A scanning transmission electron microscopy image shows flat and close contact between STO membranes and a Si wafer. Electron energy loss spectroscopic measurements reveal the interfacial Ti valence state evolution, which identifies the formation of 2D charge carriers confined at the interface of aAO/STO. This work provides a feasible strategy for the integration of 2DEG on a silicon wafer and other desired substrates for potential functional and flexible electronic devices.

Enhanced polarization and abnormal flexural deformation in bent freestanding perovskite oxides.

Recent realizations of ultrathin freestanding perovskite oxides offer a unique platform to probe novel properties in two-dimensional oxides. Here, we observe a giant flexoelectric response in freestanding BiFeO3 and SrTiO3 in their bent state arising from strain gradients up to 3.5 × 107 m-1, suggesting a promising approach for realizing ultra-large polarizations. Additionally, a substantial change in membrane thickness is discovered in bent freestanding BiFeO3, which implies an unusual bending-expansion/shrinkage effect in the ferroelectric membrane that has never been seen before in crystalline materials. Our theoretical model reveals that this unprecedented flexural deformation within the membrane is attributable to a flexoelectricity-piezoelectricity interplay. The finding unveils intriguing nanoscale electromechanical properties and provides guidance for their practical applications in flexible nanoelectromechanical systems.

Nonvolatile ferroelectric domain wall memory integrated on silicon.

Ferroelectric domain wall memories have been proposed as a promising candidate for nonvolatile memories, given their intriguing advantages including low energy consumption and high-density integration. Perovskite oxides possess superior ferroelectric prosperities but perovskite-based domain wall memory integrated on silicon has rarely been reported due to the technical challenges in the sample preparation. Here, we demonstrate a domain wall memory prototype utilizing freestanding BaTiO3 membranes transferred onto silicon. While as-grown BaTiO3 films on (001) SrTiO3 substrate are purely c-axis polarized, we find they exhibit distinct in-plane multidomain structures after released from the substrate and integrated onto silicon due to the collective effects from depolarizing field and strain relaxation. Based on the strong in-plane ferroelectricity, conductive domain walls with reading currents up to nanoampere are observed and can be both created and erased artificially, highlighting the great potential of the integration of perovskite oxides with silicon for ferroelectric domain wall memories.

Uniform nucleation and epitaxy of bilayer molybdenum disulfide on sapphire.

Two-dimensional transition-metal dichalcogenides (TMDs) are of interest for beyond-silicon electronics1,2. It has been suggested that bilayer TMDs, which combine good electrostatic control, smaller bandgap and higher mobility than monolayers, could potentially provide improvements in the energy-delay product of transistors3-5. However, despite advances in the growth of monolayer TMDs6-14, the controlled epitaxial growth of multilayers remains a challenge15. Here we report the uniform nucleation (>99%) of bilayer molybdenum disulfide (MoS2) on c-plane sapphire. In particular, we engineer the atomic terrace height on c-plane sapphire to enable an edge-nucleation mechanism and the coalescence of MoS2 domains into continuous, centimetre-scale films. Fabricated field-effect transistor (FET) devices based on bilayer MoS2 channels show substantial improvements in mobility (up to 122.6 cm2 V-1 s-1) and variation compared with FETs based on monolayer films. Furthermore, short-channel FETs exhibit an on-state current of 1.27 mA µm-1, which exceeds the 2028 roadmap target for high-performance FETs16.

High-density switchable skyrmion-like polar nanodomains integrated on silicon.

Topological domains in ferroelectrics1-5 have received much attention recently owing to their novel functionalities and potential applications6,7 in electronic devices. So far, however, such topological polar structures have been observed only in superlattices grown on oxide substrates, which limits their applications in silicon-based electronics. Here we report the realization of room-temperature skyrmion-like polar nanodomains in lead titanate/strontium titanate bilayers transferred onto silicon. Moreover, an external electric field can reversibly switch these nanodomains into the other type of polar texture, which substantially modifies their resistive behaviours. The polar-configuration-modulated resistance is ascribed to the distinct band bending and charge carrier distribution in the core of the two types of polar texture. The integration of high-density (more than 200 gigabits per square inch) switchable skyrmion-like polar nanodomains on silicon may enable non-volatile memory applications using topological polar structures in oxides.

Giant Thermal Transport Tuning at a Metal/Ferroelectric Interface.

Interfacial thermal transport plays a prominent role in the thermal management of nanoscale objects and is of fundamental importance for basic research and nanodevices. At metal/insulator interfaces, a configuration commonly found in electronic devices, heat transport strongly depends upon the effective energy transfer from thermalized electrons in the metal to the phonons in the insulator. However, the mechanism of interfacial electron-phonon coupling and thermal transport at metal/insulator interfaces is not well understood. Here, the observation of a substantial enhancement of the interfacial thermal resistance and the important role of surface charges at the metal/ferroelectric interface in an Al/BiFeO3 membrane are reported. By applying uniaxial strain, the interfacial thermal resistance can be varied substantially (up to an order of magnitude), which is attributed to the renormalized interfacial electron-phonon coupling caused by the charge redistribution at the interface due to the polarization rotation. These results imply that surface charges at a metal/insulator interface can substantially enhance the interfacial electron-phonon-mediated thermal coupling, providing a new route to optimize the thermal transport performance in next-generation nanodevices, power electronics, and thermal logic devices.

Commensurate Stacking Phase Transitions in an Intercalated Transition Metal Dichalcogenide.

Intercalation and stacking-order modulation are two active ways in manipulating the interlayer interaction of transition metal dichalcogenides (TMDCs), which lead to a variety of emergent phases and allow for engineering material properties. Herein, the growth of Pb-intercalated TMDCs-Pb(Ta1+x Se2 )2 , the first 124-phase, is reported. Pb(Ta1+x Se2 )2 exhibits a unique two-step first-order structural phase transition at around 230 K. The transitions are solely associated with the stacking degree of freedom, evolving from a high-temperature (high-T) phase with ABC stacking and R3m symmetry to an intermediate phase with AB stacking and P3m1, and finally to a low-temperature (low-T) phase again with R3msymmetry, but with ACB stacking. Each step involves a rigid slide of building blocks by a vector [1/3, 2/3, 0]. Intriguingly, gigantic lattice contractions occur at the transitions on warming. At low-T, bulk superconductivity with Tc  ≈ 1.8 K is observed. The underlying physics of the structural phase transitions are discussed from first-principle calculations. The symmetry analysis reveals topological nodal lines in the band structure. The results demonstrate the possibility of realizing higher-order metal-intercalated phases of TMDCs and advance the knowledge of polymorphic transitions, and may inspire stacking-order engineering in TMDCs and beyond.

Epitaxial growth of wafer-scale molybdenum disulfide semiconductor single crystals on sapphire.

Two-dimensional (2D) semiconductors, in particular transition metal dichalcogenides (TMDCs), have attracted great interest in extending Moore's law beyond silicon1-3. However, despite extensive efforts4-25, the growth of wafer-scale TMDC single crystals on scalable and industry-compatible substrates has not been well demonstrated. Here we demonstrate the epitaxial growth of 2 inch (~50 mm) monolayer molybdenum disulfide (MoS2) single crystals on a C-plane sapphire. We designed the miscut orientation towards the A axis (C/A) of sapphire, which is perpendicular to the standard substrates. Although the change of miscut orientation does not affect the epitaxial relationship, the resulting step edges break the degeneracy of nucleation energy for the antiparallel MoS2 domains and lead to more than a 99% unidirectional alignment. A set of microscopies, spectroscopies and electrical measurements consistently showed that the MoS2 is single crystalline and has an excellent wafer-scale uniformity. We fabricated field-effect transistors and obtained a mobility of 102.6 cm2 V-1 s-1 and a saturation current of 450 µA µm-1, which are among the highest for monolayer MoS2. A statistical analysis of 160 field-effect transistors over a centimetre scale showed a >94% device yield and a 15% variation in mobility. We further demonstrated the single-crystalline MoSe2 on C/A sapphire. Our method offers a general and scalable route to produce TMDC single crystals towards future electronics.