skip to main content


This content will become publicly available on December 1, 2024

Title: Emergent layer stacking arrangements in c-axis confined MoTe2
Abstract

The layer stacking order in 2D materials strongly affects functional properties and holds promise for next-generation electronic devices. In bulk, octahedral MoTe2possesses two stacking arrangements, the ferroelectric Weyl semimetal Tdphase and the higher-order topological insulator 1T′ phase. However, in thin flakes of MoTe2, it is unclear if the layer stacking follows the Td, 1T′, or an alternative stacking sequence. Here, we use atomic-resolution scanning transmission electron microscopy to directly visualize the MoTe2layer stacking. In thin flakes, we observe highly disordered stacking, with nanoscale 1T′ and Tddomains, as well as alternative stacking arrangements not found in the bulk. We attribute these findings to intrinsic confinement effects on the MoTe2stacking-dependent free energy. Our results are important for the understanding of exotic physics displayed in MoTe2flakes. More broadly, this work suggestsc-axis confinement as a method to influence layer stacking in other 2D materials.

 
more » « less
Award ID(s):
2039380
NSF-PAR ID:
10488987
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
SpringerNature
Date Published:
Journal Name:
Nature Communications
Volume:
14
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Two-dimensional (2D) molybdenum ditelluride (MoTe 2 ) is an interesting material for fundamental study and applications, due to its ability to exist in different polymorphs of 2H, 1T, and 1T′, their phase change behavior, and unique electronic properties. Although much progress has been made in the growth of high-quality flakes and films of 2H and 1T′-MoTe 2 phases, phase-selective growth of all three phases remains a huge challenge, due to the lack of enough information on their growth mechanism. Herein, we present a novel approach to growing films and geometrical-shaped few-layer flakes of 2D 2H-, 1T-, and 1T′-MoTe 2 by atmospheric-pressure chemical vapor deposition (APCVD) and present a thorough understanding of the phase-selective growth mechanism by employing the concept of thermodynamics and chemical kinetics involved in the growth processes. Our approach involves optimization of growth parameters and understanding using thermodynamical software, HSC Chemistry. A lattice strain-mediated mechanism has been proposed to explain the phase selective growth of 2D MoTe 2 , and different chemical kinetics-guided strategies have been developed to grow MoTe 2 flakes and films. 
    more » « less
  2. Two-dimensional materials, such as transition metal dichalcogenides, have generated much interest due to their strain-sensitive electronic, optical, magnetic, superconducting, or topological properties. Harnessing control over their strain state may enable new technologies that operate by controlling these materials’ properties in devices such as straintronic transistors. Piezoelectric oxides have been proposed as one method to control such strain states on the device scale. However, there are few studies of how conformal 2D materials remain on oxide materials with respect to dynamic applications of the strain. Non-conformality may lead to non-optimal strain transfer. In this work, we explore this aspect of oxide-2D adhesion in the nanoscale switching of the substrate structural phase in thin 1T′-MoTe 2 attached to a mixed-phase thin-film BiFeO 3 (BFO), a multiferroic oxide with an electric-field induced structural phase transition that can generate mechanical strains of up to 2%. We observe that flake thickness impacts the conformality of 1T′-MoTe 2 to structural changes in BFO, but below four layers, 1T′-MoTe 2 fully conforms to the nanoscale BFO structural changes. The conformality of few-layer 1T′-MoTe 2 suggests that BFO is an excellent candidate for deterministic, nanoscale strain control for 2D materials. 
    more » « less
  3. The fabrication of in‐plane 2H‐1T′ MoTe2homojunctions by the flux‐controlled, phase‐engineering of few‐layer MoTe2from Mo nanoislands is reported. The phase of few‐layer MoTe2is controlled by simply changing Te atomic flux controlled by the temperature of the reaction vessel. Few‐layer 2H MoTe2is formed with high Te flux, while few‐layer 1T′ MoTe2is obtained with low Te flux. With medium flux, few‐layer in‐plane 2H‐1T′ MoTe2homojunctions are synthesized. As‐synthesized MoTe2is characterized by Raman spectroscopy and X‐ray photoelectron spectroscopy. Kelvin probe force microscopy and Raman mapping confirm that in‐plane 2H‐1T′ MoTe2homojunctions have abrupt interfaces between 2H and 1T′ MoTe2domains, possessing a potential difference of about 100 mV. It is further shown that this method can be extended to create patterned metal–semiconductor junctions in MoTe2in a two‐step lithographic synthesis. The flux‐controlled phase engineering method could be utilized for the large‐scale controlled fabrication of 2D metal–semiconductor junctions for next‐generation electronic and optoelectronic devices.

     
    more » « less
  4. Abstract

    Piezoelectricity in low‐dimensional materials and metal–semiconductor junctions has attracted recent attention. Herein, a 2D in‐plane metal–semiconductor junction made of multilayer 2H and 1T′ phases of molybdenum(IV) telluride (MoTe2) is investigated. Strong piezoelectric response is observed using piezoresponse force microscopy at the 2H–1T′ junction, despite that the multilayers of each individual phase are weakly piezoelectric. The experimental results and density functional theory calculations suggest that the amplified piezoelectric response observed at the junction is due to the charge transfer across the semiconducting and metallic junctions resulting in the formation of dipoles and excess charge density, allowing the engineering of piezoelectric response in atomically thin materials.

     
    more » « less
  5. Abstract

    Crystal phase control still remains a challenge for the precise synthesis of 2D layered metal dichalcogenide (LMD) materials. The T′ phase structure has profound influences on enhancing electrical conductivity, increasing active sites, and improving intrinsic catalytic activity, which are urgently needed for enhancing hydrogen evolution reaction (HER) activity. Theoretical calculations suggest that metastable T′ phase 2D Sn1−xWxS2alloys can be formed by combining W with 1T tin disulfide (SnS2) as a template to achieve a semiconductor‐to‐metallic transition. Herein, 2D Sn1−xWxS2alloys with varyingxare prepared by adjusting the molar ratio of reactants via hydrothermal synthesis, among which Sn0.3W0.7S2displays a maximum of concentration of 81% in the metallic phase and features a distorted octahedral‐coordinated metastable 1T′ phase structure. The obtained 1T′‐Sn0.3W0.7S2has high intrinsic electrical conductivity, lattice distortion, and defects, showing a prominently improved HER catalytic performance. Metallic Sn0.3W0.7S2coupled with carbon black exhibits at least a 215‐fold improvement compared to pristine SnS2. It has excellent long‐term durability and HER activity. This work reveals a general phase transition strategy by using T phase materials as templates and merging heteroatoms to achieve synthetic metastable phase 2D LMDs that have a significantly improved HER catalytic performance.

     
    more » « less