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A combined study of scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES) is conducted to understand the multiple charge density wave (CDW) phases of monolayer (ML) VSe2films manifested by graphene substrates. Submonolayer (â¼0.8 ML) VSe2films are prepared on two different substrates of single-layer graphene (SLG) and bi-layer graphene (BLG) on a 6H-SiC(0001). We find that ML VSe2films are less coupled to the SLG substrate compared to that of ML VSe2/BLG. Then, ML VSe2grown on SLG and BLG substrates reveals a very different topography in STM. While ML VSe2/BLG shows one unidirectional modulation of â3 × 2 and â3 × â7 CDW in topography, ML VSe2/SLG presents a clear modulation of 4 × 1 CDW interfering with â3 × 2 and â3 × â7 CDW which has not been previously observed. We explicitly show that the reciprocal vector of 4 × 1 CDW fits perfectly into the long parallel sections of cigar-shaped Fermi surfaces near the M point in ML VSe2, satisfying Fermi surface nesting. Since bulk VSe2is also well-known for the 4 × 4 × 3 CDW formed by Fermi surface nesting, the 4 × 1 CDW in ML VSe2/SLG is attributed to the planar projection of 4 × 4 × 3 CDW in bulk. Our result clarifies the nature of the 4 × 1 CDW in ML VSe2system and is a good example demonstrating the essential role of substrates in two-dimensional transition metal dichalcogenides.
RESUMO
Emergent phenomena driven by electronic reconstructions in oxide heterostructures have been intensively discussed. However, the role of these phenomena in shaping the electronic properties in van der Waals heterointerfaces has hitherto not been established. By reducing the material thickness and forming a heterointerface, we find two types of charge-ordering transitions in monolayer VSe2 on graphene substrates. Angle-resolved photoemission spectroscopy (ARPES) uncovers that Fermi-surface nesting becomes perfect in ML VSe2. Renormalization-group analysis confirms that imperfect nesting in three dimensions universally flows into perfect nesting in two dimensions. As a result, the charge-density wave-transition temperature is dramatically enhanced to a value of 350 K compared to the 105 K in bulk VSe2. More interestingly, ARPES and scanning tunneling microscopy measurements confirm an unexpected metal-insulator transition at 135 K that is driven by lattice distortions. The heterointerface plays an important role in driving this novel metal-insulator transition in the family of monolayer transition-metal dichalcogenides.
RESUMO
Recently, layered chalcogenide alloys (LCAs) have been extensively investigated for use in various practical applications by selectively controlling the amount of foreign components. However, the alloying behavior of layered chalcogenides has been rarely explored at the atomistic level. Here, we study the microstructural evolution of SnSe1-xSx alloys on the atomic scale by combining scanning tunneling microscopy (STM) measurements with first-principles density functional theory (DFT) calculations. STM topographic images suggest that S atoms substituted in SnSe1-xSx are not randomly distributed, but tend to form local SnS clusters. The degree of S atom alloying was quantitatively estimated to be about 60% from STM images, indicating that homo-atoms (S-S) are a preferred arrangement over hetero-atoms (S-Se). Our DFT calculations further confirmed that the mixing energy of random SnSe1-xSx alloys showed positive behavior over the whole S composition range considered. This result suggests that SnSe1-xSx has a tendency toward local phase segregation into SnSe and SnS rather than random alloys. We expect our atomistic study on the alloying behavior to provide important insight for fabricating optimal SnSe1-xSx alloys with high thermoelectric properties.
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NiTe2, a type-II Dirac semimetal with a strongly tilted Dirac band, has been explored extensively to understand its intriguing topological properties. Here, using density functional theory calculations, we report that the strength of the spin-orbit coupling (SOC) in NiTe2 can be tuned by Se substitution. This results in negative shifts of the bulk Dirac point (BDP) while preserving the type-II Dirac band. Indeed, combined studies using scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy confirm that the BDP in the NiTe2-xSex alloy moves from +0.1 eV (NiTe2) to -0.3 eV (NiTeSe) depending on the Se concentrations, indicating the effective tunability of type-II Dirac Fermions. Our results demonstrate an approach to tailor the type-II Dirac band in NiTe2 by controlling the SOC strength via chalcogen substitution. This approach can be applicable to different types of topological materials.
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Polymorphisms allowing multiple structural phases are among the most fascinating properties of transition metal dichalcogenides (TMDs). Herein, the polymorphic 1T' phase and its lattice dynamics for bilayer VSe2 grown on epitaxial bilayer graphene are investigated via low temperature scanning tunneling microscopy (STM). The 1T' structure, mostly observed in group-6 TMDs, is unexpected in VSe2, which is a group-5 TMD. Emergence of the 1T' structure in bilayer VSe2 suggests the important roles of interface and layer configurations, providing new possibilities regarding the polymorphism of TMDs. Detailed topographical analysis elucidates the microscopic nature of the 1T' structure, confirming that Se-like and V-like surfaces can be resolved depending on the polarity of the sample bias. In addition, bilayer VSe2 can transit from a static state of the 1T' phase to a dynamic state consisting of lattice vibrations, triggered by tunneling current from the STM tip. Topography also shows hysteretic behavior during the static-dynamic transition, which is attributed to latent energy existing between the two states. The observed lattice dynamics involve vibrational motion of the Se atoms and the middle V atoms. Our observations will provide important information to establish in-depth understanding of the microscopic nature of 1T' structures and the polymorphism of two-dimensional TMDs.
RESUMO
Recently SnSe, a layered chalcogenide material, has attracted a great deal of attention for its excellent p-type thermoelectric property showing a remarkable ZT value of 2.6 at 923 K. For thermoelectric device applications, it is necessary to have n-type materials with comparable ZT value. Here, we report that n-type SnSe single crystals were successfully synthesized by substituting Bi at Sn sites. In addition, it was found that the carrier concentration increases with Bi content, which has a great influence on the thermoelectric properties of n-type SnSe single crystals. Indeed, we achieved the maximum ZT value of 2.2 along b axis at 733 K in the most highly doped n-type SnSe with a carrier density of -2.1 × 1019 cm-3 at 773 K.