van der Waals Engineering of Charge Density Waves in One-Dimensional Nb6Te6 Nanowires.

One-dimensional (1D) systems have played a crucial role in the development of fundamental physics and practical applications. Recently, transition metal monochalcogenide (TMM) wires based on molybdenum (Mo) and tungsten (W) have emerged as promising platforms for investigating 1D physics in pure van der Waals (vdW) platforms. Here, we report on the bottom-up fabrication of Nb6Te6 wires down to the single-wire limit. The unique properties of Nb6Te6 single wire enable the realization of 1D charge density wave (CDW) phases in an isolated single TMM wire. Moreover, we revealed the appealing regulation of 1D CDW orders by van der Waals interactions at either the 1D-2D interface (i.e., rotation of a single wire along its wire axis) or the 1D-1D interface. Two rotation angles (30° and 0°) give rise to 3 × 1 and zigzag chain CDW morphologies, respectively, which exhibit pronounced differences in atomic displacement by a factor of 2. The interwire vdW coupling overwhelms its counterpart at the 1D-2D interface, thus locking the rotation angle (at 0°) as well as the interwire atomic registries. In contrast, interestingly, the phases of the charge oscillations are independent of the adjacent wires. The ability to tailor 1D charge orders provides a crucial addition to the toll set of vdW integrations beyond two-dimensional materials.

Observations of Charge-Density-Wave States in W6Te6 Wires.

Determining the electronic ground state of a one-dimensional system is crucial to understanding the underlying physics of electronic behavior. Here, we demonstrate the discovery of charge-density wave states in few-wire W6Te6 arrays using scanning tunneling microscopy/spectroscopy. We directly visualize incommensurate charge orders, energy gaps with prominent coherence peaks, and the picometer-scale lattice distortion in nearly disorder-free double-wire systems, thereby demonstrating the existence of Peierls-type charge density waves. In the presence of disorder-induced charge order fluctuations, the coherence peaks resulting from phase correlation disappear and gradually transform the system into the pseudogap states. The power-law zero-bias anomaly and quasi-particle interference analysis further suggest the Tomonaga-Luttinger liquid behavior in such pseudogap region. In addition, we explicitly determined the evolution of the CDW energy gap as a function of stacking-wire numbers. The present study demonstrates the existence of electron-phonon interactions in few-wire W6Te6 that can be tuned by disorders and van der Waals stacking.

Controllable dimensionality conversion between 1D and 2D CrCl3 magnetic nanostructures.

The fabrication of one-dimensional (1D) magnetic systems on solid surfaces, although of high fundamental interest, has yet to be achieved for a crossover between two-dimensional (2D) magnetic layers and their associated 1D spin chain systems. In this study, we report the fabrication of 1D single-unit-cell-width CrCl3 atomic wires and their stacked few-wire arrays on the surface of a van der Waals (vdW) superconductor NbSe2. Scanning tunneling microscopy/spectroscopy and first-principles calculations jointly revealed that the single wire shows an antiferromagnetic large-bandgap semiconducting state in an unexplored structure different from the well-known 2D CrCl3 phase. Competition among the total energies and nanostructure-substrate interfacial interactions of these two phases result in the appearance of the 1D phase. This phase was transformable to the 2D phase either prior to or after the growth for in situ or ex situ manipulations, in which the electronic interactions at the vdW interface play a nontrivial role that could regulate the dimensionality conversion and structural transformation between the 1D-2D CrCl3 phases.

Realization of Multiple Charge-Density Waves in NbTe2 at the Monolayer Limit.

Layered transition-metal dichalcogenides down to the monolayer (ML) limit provide a fertile platform for exploring charge-density waves (CDWs). Here, we experimentally unveil the richness of the CDW phases in ML-NbTe2 for the first time. Not only the theoretically predicted 4 × 4 and 4 × 1 phases but also two unexpected 28×28 and 19×19 phases are realized. For such a complex CDW system, we establish an exhaustive growth phase diagram via systematic efforts in the material synthesis and scanning tunneling microscope characterization. Moreover, the energetically stable phase is the larger-scale order (19×19), which is surprisingly in contradiction to the prior prediction (4 × 4). These findings are confirmed using two different kinetic pathways: i.e., direct growth at proper growth temperatures (T) and low-T growth followed by high-T annealing. Our results provide a comprehensive diagram of the "zoo" of CDW orders in ML-NbTe2.

Approaching strain limit of two-dimensional MoS2 via chalcogenide substitution.

Strain engineering is a promising method for tuning the electronic properties of two-dimensional (2D) materials, which are capable of sustaining enormous strain thanks to their atomic thinness. However, applying a large and homogeneous strain on these 2D materials, including the typical semiconductor MoS2, remains cumbersome. Here we report a facile strategy for the fabrication of highly strained MoS2 via chalcogenide substitution reaction (CSR) of MoTe2 with lattice inheritance. The MoS2 resulting from the sulfurized MoTe2 sustains ultra large in-plane strain (approaching its strength limit ~10%) with great homogeneity. Furthermore, the strain can be deterministically and continuously tuned to ~1.5% by simply varying the processing temperature. Thanks to the fine control of our CSR process, we demonstrate a heterostructure of strained MoS2/MoTe2 with abrupt interface. Finally, we verify that such a large strain potentially allows the modulation of MoS2 bandgap over an ultra-broad range (~1 eV). Our controllable CSR strategy paves the way for the fabrication of highly strained 2D materials for applications in devices.

Two 'braking mechanisms' for tin phthalocyanine molecular rotors on dipolar iron oxide surfaces.

Manipulation of artificial molecular rotors/motors is a key issue in the field of molecular nanomachines. Here we assemble non-planar SnPc molecules on an FeO film to form two kinds of rotors with different apparent morphologies, rotational speeds and stabilities. Both kinds of rotors can switch to each other via external field stimulation and the switch depends on the polarity of the applied bias voltage. Furthermore, we reveal that the molecular fragment has a great influence on the motions of molecules. Combining scanning tunneling microscopy and DFT calculations, two braking mechanisms are addressed for molecular rotors. One is the transformation of adsorption configurations under the external electric field stimulus that enables the molecular rotor to stop/restart its rotation. The other is the introduction of embedded molecular fragments that act as a brake pad and can stop the molecular rotation. We find that the rotation can be recovered by separating the molecule from the fragments. Our study suggests a good system for manipulating molecular rotors' properties in nanophysics and has important value for the design of controllable molecular machines.

Tuning of the Valley Structures in Monolayer In2Se3/WSe2 Heterostructures via Ferroelectricity.

Recent findings of two-dimensional ferroelectric (FE) materials have enabled the integration of nonvolatile FE functions into device applications based on van der Waals (vdW) heterojunctions (HJs), resulting in versatile technological advances. In this paper, we report the results of direct probing of the electronic structures of In2Se3/WSe2 heterostructures at the single-layer limit, where monolayer (ML)-In2Se3 was found to be either antiferroelectric (AFE, ß') or ferroelectric (ß*) at sufficiently low temperatures. A general type-II band alignment was revealed for this heterostructure. Moreover, we observed significant modulations of the valley structures of WSe2, and in situ transformations between the FE and AFE In2Se3 phases demonstrated the dominant role of the polarizations in the top ML-In2Se3 layer. The observed phenomena can be attributed to the combination of both the linear and quadratic Stark shifts from the out-of-plane electric field, which has only been previously theoretically explored for ML-transition metal dichalcogenides (TMDs).

PTCDA Molecular Monolayer on Pb Thin Films: An Unusual π-Electron Kondo System and Its Interplay with a Quantum-Confined Superconductor.

The hybridization of magnetism and superconductivity has been an intriguing playground for correlated electron systems, hosting various novel physical phenomena. Usually, localized d or f electrons are central to magnetism. In this study, by placing a PTCDA (3,4,9,10-perylene tetracarboxylic dianhydride) molecular monolayer on ultrathin Pb films, we built a hybrid magnetism/superconductivity (M/SC) system consisting of only sp electronic levels. The magnetic moments reside in the unpaired molecular orbital originating from interfacial charge transfers. We reported distinctive tunneling spectroscopic features of such a Kondo screened π electron impurity lattice on a superconductor in the regime of T_{K}≫Δ, suggesting the formation of a two-dimensional bound states band. Moreover, moiré superlattices with tunable twist angle and the quantum confinement in the ultrathin Pb films provide easy and flexible implementations to tune the interplay between the Kondo physics and the superconductivity, which are rarely present in M/SC hybrid systems.

Precise Tuning of Band Structures and Electron Correlations by van der Waals Stacking of One-dimensional W6Te6 Wires.

Stacking of two-dimensional (2D) van der Waals (vdW) atomic sheets has been established as a powerful approach to fabricating new materials with broad versatilities and emergent functionalities. Here we demonstrate a bottom-up approach to fabricating isolated single W6Te6 wires and their lateral assemblies, offering a unique platform for investigating the elegant role of vdW coupling in 1D systems with atomic precision. We find experimentally and theoretically a single W6Te6 wire is a 1D semiconductor with a band gap of ∼60 meV, and a semiconductor-to-metal transition takes place upon interwire vdW stacking. The metallic multiwires exhibit strong Tomonaga-Luttinger liquid characteristics with the correlation parameter g varying from g = 0.086 for biwire to g = 0.136 for six-wire assemblies, all much reduced from the Fermi liquid regime (g = 1). The present study demonstrates wire-by-wire vdW stacking is a versatile means for fabrication of 1D systems with tunable electronic properties.