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Applying long wavelength periodic potentials on quantum materials has recently been demonstrated to be a promising pathway for engineering novel quantum phases of matter. Here, we utilize twisted bilayer boron nitride (BN) as a moir\'e substrate for band structure engineering. Small-angle-twisted bilayer BN is endowed with periodically arranged up and down polar domains, which imprints a periodic electrostatic potential on a target two-dimensional (2D) material placed on top. As a proof of concept, we use Bernal bilayer graphene as the target material. The resulting modulation of the band structure appears as superlattice resistance peaks, tunable by varying the twist angle, and Hofstadter butterfly physics under a magnetic field. Additionally, we demonstrate the tunability of the moir\'e potential by altering the dielectric thickness underneath the twisted BN. Finally, we find that near-60{\deg}-twisted bilayer BN provides a unique platform for studying the moir\'e structural effect without the contribution from electrostatic moir\'e potentials. Tunable moir\'e polar substrates may serve as versatile platforms to engineer the electronic, optical, and mechanical properties of 2D materials and van der Waals heterostructures., Comment: 21 pages, 11 figures

The electrolysis of CO$_2$ in molten carbonate has been introduced as an alternative mechanism to synthesize carbon nanomaterials inexpensively at high yield. Until recently, CO$_2$ was thought to be unreactive, making its removal a challenge. CO$_2$ is the main cause of anthropogenic global warming and its utilization and transformation into a stable, valuable material provides an incentivized pathway to mitigate climate change. This study focuses on controlled electrochemical conditions in molten lithium carbonate to split CO$_2$ absorbed from the atmosphere into into carbon nanotubes, and into various macroscopic assemblies of CNTs,, which may be useful for nano-filtration. Different CNTs, morphologies were prepared electrochemically by variation of the anode and cathode composition and architecture, electrolyte composition pre-electrolysis processing, and the variation of current application and current density. Individual CNT morphologies structures and the CNT molten carbonate growth mechanism are explored by SEM, TEM, HAADF EDX, XRD and Raman. The principle commercial technology for CNT production had been chemical vapor deposition, which is an order of magnitude more expensive, generally requires metallo-organics, rather than CO$_2$ as reactants, and can be highly energy and CO$_2$ emission intensive (carries a high carbon positive, rather than negative, footprint)., Comment: 24 pages, 10 figures

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host "hidden" orders after laser excitation.

Van der Waals (vdW) materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit emergent physical properties absent in the parent compounds through interlayer interactions. Here we report on a new family of emergent, nanometer-thick, semiconductor 2D ferroelectrics, where the individual constituents are well-studied non-ferroelectric monolayer transition metal dichalcogenides (TMDs), namely WSe2, MoSe2, WS2, and MoS2. By stacking two identical monolayer TMDs in parallel, we obtain electrically switchable rhombohedral-stacking configurations, with out-of-plane polarization that is flipped by in-plane sliding motion. Fabricating nearly-parallel stacked bilayers enables the visualization of moir\'e ferroelectric domains as well as electric-field-induced domain wall motion with piezoelectric force microscopy (PFM). Furthermore, by using a nearby graphene electronic sensor in a ferroelectric field transistor geometry, we quantify the ferroelectric built-in interlayer potential, in good agreement with first-principles calculations. The novel semiconducting ferroelectric properties of these four new TMDs opens up the possibility of studying the interplay between ferroelectricity and their rich electric and optical properties., Comment: 16 pages, 4 figures

Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe4. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observed that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge-density-wave (CDW) phase of EuTe4 with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly-coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.

2D ferroelectrics with robust polarization down to atomic thicknesses provide novel building blocks for functional heterostructures. Experimental reports, however, remain scarce because of the requirement of a layered polar crystal. Here, we demonstrate a rational design approach to engineering 2D ferroelectrics from a non-ferroelectric parent compound via employing van der Waals assembly. Parallel-stacked bilayer boron nitride is shown to exhibit out-of-plane electric polarization that reverses depending on the stacking order. The polarization switching is probed via the resistance of an adjacently-stacked graphene sheet. Furthermore, twisting the boron nitride sheets by a small-angle changes the dynamics of switching due to the formation of moir\'e ferroelectricity with staggered polarization. The ferroelectricity persists to room temperature while keeping the high mobility of graphene, paving the way for potential ultrathin nonvolatile memory applications., Comment: Initial draft. The published paper contains piezoelectric force microscopy data

Advanced microscopy and/or spectroscopy tools play indispensable role in nanoscience and nanotechnology research, as it provides rich information about the growth mechanism, chemical compositions, crystallography, and other important physical and chemical properties. However, the interpretation of imaging data heavily relies on the "intuition" of experienced researchers. As a result, many of the deep graphical features obtained through these tools are often unused because of difficulties in processing the data and finding the correlations. Such challenges can be well addressed by deep learning. In this work, we use the optical characterization of two-dimensional (2D) materials as a case study, and demonstrate a neural-network-based algorithm for the material and thickness identification of exfoliated 2D materials with high prediction accuracy and real-time processing capability. Further analysis shows that the trained network can extract deep graphical features such as contrast, color, edges, shapes, segment sizes and their distributions, based on which we develop an ensemble approach topredict the most relevant physical properties of 2D materials. Finally, a transfer learning technique is applied to adapt the pretrained network to other applications such as identifying layer numbers of a new 2D material, or materials produced by a different synthetic approach. Our artificial-intelligence-based material characterization approach is a powerful tool that would speed up the preparation, initial characterization of 2D materials and other nanomaterials and potentially accelerate new material discoveries.

When electrons in a solid are excited with light, they can alter the free energy landscape and access phases of matter that are beyond reach in thermal equilibrium. This accessibility becomes of vast importance in the presence of phase competition, when one state of matter is preferred over another by only a small energy scale that, in principle, is surmountable by light. Here, we study a layered compound, LaTe$_3$, where a small in-plane (a-c plane) lattice anisotropy results in a unidirectional charge density wave (CDW) along the c-axis. Using ultrafast electron diffraction, we find that after photoexcitation, the CDW along the c-axis is weakened and subsequently, a different competing CDW along the a-axis emerges. The timescales characterizing the relaxation of this new CDW and the reestablishment of the original CDW are nearly identical, which points towards a strong competition between the two orders. The new density wave represents a transient non-equilibrium phase of matter with no equilibrium counterpart, and this study thus provides a framework for unleashing similar states of matter that are "trapped" under equilibrium conditions.

We survey the electrical transport properties of the single-crystalline, topological chiral semimetal CoSi which was grown via different methods. High-quality CoSi single crystals were found in the growth from tellurium solution. The sample's high carrier mobility enables us to observe, for the first time, quantum oscillations (QOs) in its thermoelectrical signals. Our analysis of QOs reveals two spherical Fermi surfaces around the R point in the Brillouin zone corner. The extracted Berry phases of these electron orbits are consistent with the -2 chiral charge as reported in DFT calculations. Detailed analysis on the QOs reveals that the spin-orbit coupling induced band-splitting is less than 2 meV near the Fermi level, one order of magnitude smaller than our DFT calculation result. We also report the phonon-drag induced large Nernst effect in CoSi at intermediate temperatures.

Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photo-induced transition of a model charge-density-wave (CDW) compound, LaTe$_3$. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be quantitatively captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.

The recent emergence of 2D van der Waals magnets down to atomic layer thickness provides an exciting platform for exploring quantum magnetism and spintronics applications. The van der Waals nature stabilizes the long-range ferromagnetic order as a result of magnetic anisotropy. Furthermore, giant tunneling magnetoresistance and electrical control of magnetism have been reported. However, the potential of 2D van der Waals magnets for magnonics, magnon-based spintronics, has not been explored yet. Here, we report the experimental observation of long-distance magnon transport in quasi-twodimensional van der Waals antiferromagnet MnPS3, which demonstrates the 2D magnets as promising material candidates for magnonics. As the 2D MnPS3 thickness decreases, a shorter magnon diffusion length is observed, which could be attributed to the surface-impurity-induced magnon scattering. Our results could pave the way for exploring quantum magnonics phenomena and designing future magnonics devices based on 2D van der Waals magnets., Comment: Main paper: 15 pages, 4 figures. Supplementary materials: 11 Figures

The quantum behaviour of electrons in materials lays the foundation for modern electronic and information technology. Quantum materials with novel electronic and optical properties have been proposed as the next frontier, but much remains to be discovered to actualize the promise. Here we report the first observation of topological quantum properties of chiral crystals in the RhSi family. We demonsrate that this material hosts novel phase of matter exhibiting nearly ideal topological surface properties that emerge as a consequence of the crystals' structural chirality or handedness. We also demonstrate that the electrons on the surface of this crystal show a highly unusual helicoid structure that spirals around two high-symmetry momenta signalling its topological electronic chirality. Such helicoid Fermi arcs on the surface experimentally characterize the topological charges of $\pm{2}$, which arise from the bulk chiral fermions. The existence of bulk high-fold degenerate fermions are guaranteed by the crystal symmetries, however, in order to determine the topological charge in the chiral crystals it is essential to identify and study the helical arc states. Remarkably, these topological conductors we discovered exhibit helical Fermi arcs which are of length $\pi$, stretching across the entire Brillouin zone and orders of magnitude larger than those found in all known Weyl semimetals. Our results demonstrate novel electronic topological state of matter on a structurally chiral crystal featuring helicoid Fermi arc surface states. The exotic electronic chiral fermion state realised in these materials can be used to detect a quantised photogalvanic optical response or the chiral magnetic effect and its optical version in future devices as described by G. Chang \textit{et.al.,} `Topological quantum properties of chiral crystals' Nature Mat. 17, 978-985 (2018)., Comment: 28 pages, 12 figures

Ionic liquid gating can markedly modulate the materials' carrier density so as to induce metallization, superconductivity, and quantum phase transitions. One of the main issues is whether the mechanism of ionic liquid gating is an electrostatic field effect or an electrochemical effect, especially for oxide materials. Recent observation of the suppression of the ionic liquid gate-induced metallization in the presence of oxygen for oxide materials suggests the electrochemical effect. However, in more general scenarios, the role of oxygen in ionic liquid gating effect is still unclear. Here, we perform the ionic liquid gating experiments on a non-oxide material: two-dimensional ferromagnetic Cr2Ge2Te6. Our results demonstrate that despite the large increase of the gate leakage current in the presence of oxygen, the oxygen does not affect the ionic liquid gating effect (< 5 % difference), which suggests the electrostatic field effect as the mechanism on non-oxide materials. Moreover, our results show that the ionic liquid gating is more effective on the modulation of the channel resistances compared to the back gating across the 300 nm thick SiO2., Comment: 17 pages, 6 figure. To appear in ACS Applied Materials & Interfaces