Seeded growth of large single-crystal copper foils with high-index facets.

The production of large single-crystal metal foils with various facet indices has long been a pursuit in materials science owing to their potential applications in crystal epitaxy, catalysis, electronics and thermal engineering1-5. For a given metal, there are only three sets of low-index facets ({100}, {110} and {111}). In comparison, high-index facets are in principle infinite and could afford richer surface structures and properties. However, the controlled preparation of single-crystal foils with high-index facets is challenging, because they are neither thermodynamically6,7 nor kinetically3 favourable compared to low-index facets6-18. Here we report a seeded growth technique for building a library of single-crystal copper foils with sizes of about 30 × 20 square centimetres and more than 30 kinds of facet. A mild pre-oxidation of polycrystalline copper foils, followed by annealing in a reducing atmosphere, leads to the growth of high-index copper facets that cover almost the entire foil and have the potential of growing to lengths of several metres. The creation of oxide surface layers on our foils means that surface energy minimization is not a key determinant of facet selection for growth, as is usually the case. Instead, facet selection is dictated randomly by the facet of the largest grain (irrespective of its surface energy), which consumes smaller grains and eliminates grain boundaries. Our high-index foils can be used as seeds for the growth of other Cu foils along either the in-plane or the out-of-plane direction. We show that this technique is also applicable to the growth of high-index single-crystal nickel foils, and we explore the possibility of using our high-index copper foils as substrates for the epitaxial growth of two-dimensional materials. Other applications are expected in selective catalysis, low-impedance electrical conduction and heat dissipation.

Non-Steady-State Symmetry Breaking Growth of Multilayered SnSe2 Nanoplates.

The use of non-equilibrium growth modes with non-steady dynamics is extensively explored in bulk materials such as amorphous and polycrystalline materials. Yet, research into the non-steady-state (NSS) growth of two-dimensional (2D) materials is still in its infancy. In this study, multilayered tin selenide (SnSe2 ) nanoplates are grown by chemical vapor deposition under NSS conditions (modulating carrier gas flow and temperature). Given the facile diffusion and inherent instability of SnSe2 , it proves to be an apt candidate for nucleation and growth in NSS scenarios. This leads to the emergence of SnSe2 nanoplates with distinct features (self-growth twisting, symmetry transformation, interlayer decoupling, homojunction, and large-area 2D domain), exhibiting pronounced second harmonic generation. The authors' findings shed light on the growth dynamics of 2D materials, broadening their potential applications in various fields.

Designed growth of large bilayer graphene with arbitrary twist angles.

The production of large-area twisted bilayer graphene (TBG) with controllable angles is a prerequisite for proceeding with its massive applications. However, most of the prevailing strategies to fabricate twisted bilayers face great challenges, where the transfer methods are easily stuck by interfacial contamination, and direct growth methods lack the flexibility in twist-angle design. Here we develop an effective strategy to grow centimetre-scale TBG with arbitrary twist angles (accuracy, <1.0°). The success in accurate angle control is realized by an angle replication from two prerotated single-crystal Cu(111) foils to form a Cu/TBG/Cu sandwich structure, from which the TBG can be isolated by a custom-developed equipotential surface etching process. The accuracy and consistency of the twist angles are unambiguously illustrated by comprehensive characterization techniques, namely, optical spectroscopy, electron microscopy, photoemission spectroscopy and photocurrent spectroscopy. Our work opens an accessible avenue for the designed growth of large-scale two-dimensional twisted bilayers and thus lays the material foundation for the future applications of twistronics at the integration level.

Control over Berry Curvature Dipole with Electric Field in WTe_{2}.

Berry curvature dipole plays an important role in various nonlinear quantum phenomena. However, the maximum symmetry allowed for nonzero Berry curvature dipole in the transport plane is a single mirror line, which strongly limits its effects in materials. Here, via probing the nonlinear Hall effect, we demonstrate the generation of Berry curvature dipole by applied dc electric field in WTe_{2}, which is used to break the symmetry constraint. A linear dependence between the dipole moment of Berry curvature and the dc electric field is observed. The polarization direction of the Berry curvature is controlled by the relative orientation of the electric field and crystal axis, which can be further reversed by changing the polarity of the dc field. Our Letter provides a route to generate and control Berry curvature dipole in broad material systems and to facilitate the development of nonlinear quantum devices.

Evidence of abnormal hot carrier thermalization at van Hove singularity of twisted bilayer graphene.

Interlayer twist evokes revolutionary changes to the optical and electronic properties of twisted bilayer graphene (TBG) for electronics, photonics and optoelectronics. Although the ground state responses in TBG have been vastly and clearly studied, the dynamic process of its photoexcited carrier states mainly remains elusive. Here, we unveil the photoexcited hot carrier dynamics in TBG by time-resolved ultrafast photoluminescence (PL) autocorrelation spectroscopy. We demonstrate the unconventional ultrafast PL emission between the van Hove singularities (VHSs) with a ∼4 times prolonged relaxation lifetime. This intriguing photoexcited carrier behavior is ascribed to the abnormal hot carrier thermalization brought by bottleneck effects at VHSs and interlayer charge distribution process. Our study on hot carrier dynamics in TBG offers new insights into the excited states and correlated physics of graphene twistronics systems.

Robust Piezoelectricity with Spontaneous Polarization in Monolayer Tellurene and Multilayer Tellurium Film at Room Temperature for Reliable Memory.

Robust neuromorphic computing in the Big Data era calls for long-term stable crossbar-array memory cells; however, the elemental segregation in the switch unit and memory unit that inevitably occurs upon cycling breaks the compositional and structural stability, making the whole memory cell a failure. Searching for a novel material without segregation that can be used for both switch and memory units is the major concern to fabricate robust and reliable nonvolatile cross-array memory cells. Tellurium (Te) is found recently to be the only peculiar material without segregation for switching, but the memory function has not been demonstrated yet. Herein, apparent piezoelectricity is experimentally confirmed with spontaneous polarization behaviors in elementary 2D Te, even in monolayer tellurene (0.4 nm), due to the highly oriented polarization of the molecular structure and the non-centrosymmetric lattice structure. A large memory window of 7000, a low working voltage of 2 V, and high on switching current up to 36.6 µA µm-1 are achieved in the as-fabricated Te-based memory device, revealing the great promise of Te for both switching and memory units in one cell without segregation. The piezoelectric Te with spontaneous polarization provides a platform to build robust, reliable, and high-density logic-in-memory chips in neuromorphic computing.

Sandwiched graphene/hBN/graphene photonic crystal fibers with high electro-optical modulation depth and speed.

Graphene-photonic crystal fibers (PCFs) are obtained by integrating the broadband optical response and electro-optic tunability of graphene with the high-quality waveguide capacity and easy-integrability of the PCF, and this has been proven to be an important step towards multimaterial multifunctional fiber and all-fiber integrated circuits. However, the reported electro-optic modulator based on directly-grown graphene-PCF suffers from very low response speed (below 100 Hz) due to the slow response of ionic liquid. Here, we propose new functional PCFs with a sandwiched graphene/hBN/graphene (Gr/hBN/Gr) film attached to the hole walls of the fibers, and theoretically demonstrate that the in-line modulator based on it can achieve simultaneous single-mode transmission ranging from 1260 nm to 1700 nm (covering all optical communication bands), significant modulation depth (e.g. ∼42 dB mm-1 at 1550 nm) and high modulation speed (up to ∼0.1 GHz). Furthermore, various device functions can be designed by changing the structure of the fiber, including the length, the hole diameter and the layer numbers of graphene and hBN films. This proposed approach directs a viable path to obtain high-performance all-fiber devices based on hybrid two-dimensional material optical fibers.