Strong evidence suggests that transformative correlated electron behavior may exist only in unrealized clean-limit 2D materials such as 1T-TaS2. Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers impedes correlation-driven quantum behavior. Here we demonstrate a new route to realizing fragile 2D quantum states through epitaxial polytype engineering of van der Waals materials. The isolation of truly 2D charge density waves (CDWs) between metallic layers stabilizes commensurate long-range order and lifts the coupling between neighboring CDW layers to restore mirror symmetries via interlayer CDW twinning. The twinned-commensurate charge density wave (tC-CDW) reported herein has a single metal-insulator phase transition at ~350 K as measured structurally and electronically. Fast in-situ transmission electron microscopy and scanned nanobeam diffraction map the formation of tC-CDWs. This work introduces epitaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication.
Motivated by recent advances in the fabrication of Josephson junctions in which the weak link is made of a low-dimensional non-superconducting material, we present here a systematic theoretical study of the local density of states (LDOS) in a clean 2D normal metal (N) coupled to two s-wave superconductors (S). To be precise, we employ the quasiclassical theory of superconductivity in the clean limit, based on Eilenbergers equations, to investigate the phase-dependent LDOS as function of factors such as the length or the width of the junction, a finite reflectivity, and a weak magnetic field. We show how the the spectrum of Andeeev bound states that appear inside the gap shape the phase-dependent LDOS in short and long junctions. We discuss the circumstances when a gap appears in the LDOS and when the continuum displays a significant phase-dependence. The presence of a magnetic flux leads to a complex interference behavior, which is also reflected in the supercurrent-phase relation. Our results agree qualitatively with recent experiments on graphene SNS junctions. Finally, we show how the LDOS is connected to the supercurrent that can flow in these superconducting heterostructures and present an analytical relation between these two basic quantities.
Engineering thermal transport in two dimensional materials, alloys and heterostructures is critical for the design of next-generation flexible optoelectronic and energy harvesting devices. Direct experimental characterization of lattice thermal conductivity in these ultra-thin systems is challenging and the impact of dopant atoms and hetero-phase interfaces, introduced unintentionally during synthesis or as part of deliberate material design, on thermal transport properties is not understood. Here, we use non-equilibrium molecular dynamics simulations to calculate lattice thermal conductivity of (Mo|W)Se$_2$ monolayer crystals including Mo$_{1-x}$W$_x$Se$_2$ alloys with substitutional point defects, periodic MoSe$_2$|WSe$_2$ heterostructures with characteristic length scales and scale-free fractal MoSe$_2$|WSe$_2$ heterostructures. Each of these features has a distinct effect on phonon propagation in the crystal, which can be used to design fractal and periodic alloy structures with highly tunable thermal conductivities. This control over lattice thermal conductivity will enable applications ranging from thermal barriers to thermoelectrics.
Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted much interest and shown promise in many applications. However, it is challenging to obtain uniform TMDCs with clean surfaces, because of the difficulties in controlling the way the reactants are supplied to the reaction in the current chemical vapor deposition (CVD) growth process. Here, we report a new growth approach called dissolution-precipitation (DP) growth, where the metal sources are sealed inside glass substrates to control their feeding to the reaction. Noteworthy, the diffusion of metal source inside glass to its surface provides a uniform metal source on the glass surface, and restricts the TMDC growth to only a surface reaction while eliminates unwanted gas-phase reaction. This feature gives rise to highly-uniform monolayer TMDCs with a clean surface on centimeter-scale substrates. The DP growth works well for a large variety of TMDCs and their alloys, providing a solid foundation for the controlled growth of clean TMDCs by the fine control of the metal source.
The discovery of two-dimensional superconductivity in Bi2Te3/FeTe heterostructure provides a new platform for the search of Majorana fermions in condensed matter systems. Since Majorana fermions are expected to reside at the core of the vortices, a close examination of the vortex dynamics in superconducting interface is of paramount importance. Here, we report the robustness of the interfacial superconductivity and 2D vortex dynamics in four as-grown and aged Bi2Te3/FeTe heterostructure with different Bi2Te3 epilayer thickness (3, 5, 7, 14 nm). After two years air exposure, superconductivity remains robust even when the thickness of Bi2Te3 epilayer is down to 3 nm. Meanwhile, a new feature at ~13 K is induced in the aged samples, and the high field studies reveal its relevance to superconductivity. The resistance of all as-grown and aged heterostructures, just below the superconducting transition temperature follows the Arrhenius relation, indicating the thermally activated flux flow behavior at the interface of Bi2Te3 and FeTe. Moreover, the activation energy exhibits a logarithmic dependence on the magnetic field, providing a compelling evidence for the 2D vortex dynamics in this novel system. The weak disorder associated with aging-induced Te vacancies is possibly responsible for these observed phenomena.
Layered heterostructure materials with two different functional building blocks can teach us about emergent physical properties and phenomena arising from interactions between the layers. We report the intergrowth compounds KLa$M$$_{1-x}$Te$_{4}$ ($M$ = Mn, Zn; $xapprox$ 0.35) featuring two chemically distinct alternating layers [LaTe$_3$] and [K$M$$_{1-x}$Te]. Their crystal structures are incommensurate, determined by single X-ray diffraction for the Mn compound and transmission electron microscope (TEM) study for the Zn compound. KLaMn$_{1-x}$Te$_{4}$ crystallizes in the orthorhombic superspace group $Pmnm$(01/2${gamma}$)$s$00 with lattice parameters $a$ = 4.4815(3) {AA}, $b$ = 21.6649(16) {AA} and $c$ = 4.5220(3) {AA}. It exhibits charge density wave (CDW) order at room temperature with a modulation wave vector $mathbf{q}$ = 1/2$mathbf{b}$* + 0.3478$mathbf{c}$* originating from electronic instability of Te-square nets in [LaTe$_{3}$] layers. The Mn analog exhibits a cluster spin glass behavior with spin freezing temperature $T_{mathrm{f}}$ $approx$ 5 K attributed to disordered Mn vacancies and competing magnetic interactions in the [Mn$_{1-x}$Te] layers. The Zn analog also has charge density wave order at room temperature with a similar $mathbf{q}$-vector having the $mathbf{c}$* component ~ 0.346 confirmed by selected-area electron diffraction (SAED). Electron transfer from [K$M_{1-x}$Te] to [LaTe$_{3}$] layers exists in KLa$M_{1-x}$Te$_{4}$, leading to an enhanced electronic specific heat coefficient. The resistivities of KLa$M_{1-x}$Te$_{4}$ ($M$ = Mn, Zn) exhibit metallic behavior at high temperatures and an upturn at low temperatures, suggesting partial localization of carriers in the [LaTe$_{3}$] layers with some degree of disorder associated with the $M$ atom vacancies in the [$M_{1-x}$Te] layers.