An official website of the United States government
Abstract Compelling evidence suggests distinct correlated electron behavior may exist only in clean 2D materials such as 1T-TaS 2 . Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers disrupts correlation-driven quantum behavior. Here we demonstrate a route to realizing fragile 2D quantum states through endotaxial polytype engineering of van der Waals materials. The true isolation of 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 endotaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication.
more »
« less
Light–Matter Interaction in Quantum Confined 2D Polar Metals
Abstract This work is a systematic experimental and theoretical study of the in‐plane dielectric functions of 2D gallium and indium films consisting of two or three atomic metal layers confined between silicon carbide and graphene with a corresponding bonding gradient from covalent to metallic to van der Waals type.k‐space resolved free electron and bound electron contributions to the optical response are identified, with the latter pointing towards the existence of thickness dependent quantum confinement phenomena. The resonance energies in the dielectric functions and the observed epsilon near‐zero behavior in the near infrared to visible spectral range, are dependent on the number of atomic metal layers and properties of the metal involved. A model‐based spectroscopic ellipsometry approach is used to estimate the number of atomic metal layers, providing a convenient route over expensive invasive characterization techniques. A strong thickness and metal choice dependence of the light–matter interaction makes these half van der Waals 2D polar metals attractive for quantum engineered metal films, tunable (quantum‐)plasmonics and nano‐photonics.
more »
« less
- Award ID(s):
- 2002651
- PAR ID:
- 10454582
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 31
- Issue:
- 4
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract The transition metal selenides M1+ySe2(M = V, Ti) have intriguing quantum properties, which make them target materials for controlling properties by thinning them to the ultrathin limit. An appropriate approach for the synthesis of such ultrathin films is by molecular beam epitaxy. Here, it is shown that such synthesized V‐ and Ti‐Se2films can undergo a compositional change by vacuum annealing. Combined scanning tunneling and photoemission spectroscopy is used to determine compositional and structural changes of ultrathin films as a function of annealing temperature. Loss of selenium from the film is accompanied by a morphology change of monolayer height islands to predominantly bilayer height. In addition, crystal periodicity and atomic structure changes are observed. These changes are consistent with a transition from a layered transition metal dichalcogenide (TMDC) to ordered intercalation compounds with V or Ti intercalated in between two layers of their respective TMDCs. These observations may clear up misconception of the nature of previously reported high‐temperature grown transition metal selenides. More significantly, the demonstrated control of the formation of intercalation compounds is a key step toward modifying properties in van der Waals systems and toward expanding material systems for van der Waals heterostructures.more » « less
-
Abstract Recently, 2D electron gases have been observed in atomically thin semiconducting crystals, enabling the observation of rich physical phenomena at the quantum level within the ultimate thickness limit. However, the observation of 2D electron gases and subsequent quantum Hall effect require exceptionally high crystalline quality, rendering mechanical exfoliation as the only method to produce high‐quality 2D semiconductors of black phosphorus and indium selenide (InSe), which hinder large‐scale device applications. Here, the controlled one‐step synthesis of high‐quality 2D InSe thin films via chemical vapor transport method is reported. The carrier Hall mobility of hexagonal boron nitride (hBN) encapsulated InSe flakes can be up to 5000 cm2V−1s−1at 1.5 K, enabling to observe the quantum Hall effect in a synthesized van der Waals semiconductor. The existence of the quantum Hall effect in directly synthesized 2D semiconductors indicates a high quality of the chemically synthesized 2D semiconductors, which hold promise in quantum devices and applications with high mobility.more » « less
-
Abstract The graphene boom has triggered a widespread search for novel elemental van der Waals materials thanks to their simplicity for theoretical modeling and easy access for material growth. Group VI element tellurium is an unintentionally p-type doped narrow bandgap semiconductor featuring a one-dimensional chiral atomic structure which holds great promise for next-generation electronic, optoelectronic, and piezoelectric applications. In this paper, we first review recent progress in synthesizing atomically thin Te two-dimensional (2D) films and one-dimensional (1D) nanowires. Its applications in field-effect transistors and potential for building ultra-scaled Complementary metal–oxide–semiconductor (CMOS) circuits are discussed. We will also overview the recent study on its quantum transport in the 2D limit and progress in exploring its topological features and chiral-related physics. We envision that the breakthrough in obtaining high-quality 2D Te films will inspire a revisit of the fundamental properties of this long-forgotten material in the near future.more » « less
-
Abstract Large‐scale synthesis of van der Waals (vdW) metal–organic framework (MOF) nanosheets with controlled crystallinity and interlayer coupling strength is one of the bottlenecks in 2D materials that has limited its successful transition to large‐scale applications. Here, scalable synthesis of mBDC (m = Zn and Cu) 2D MOFs at large scales through a biphase method is demonstrated. The results show replacing water molecules with pyridine eliminates hydrogen bond formation at metal cluster sites. This prohibits tight coupling across adjacent MOF layers and sustains controllable 2D vdW MOF growth. It is further shown that control over the growth speed, crystallinity, and thickness can be achieved by addition of a controlled amount of triethylamine and formic acid to achieve highly crystalline vdW MOF nanosheets with extraordinarily high aspect ratio. The described synthesis route can easily be scaled up for large‐scale production either by deposition onto desired substrates or in crystalline layered powder form. Owing to its large lateral size, vdW nature, and high crystallinity, it is possible to perform atomic force microscopy, Kelvin probe force microscopy, and Raman measurements on the 2D MOFs. The results not only establish their vibrational properties and layer‐dependent responses but also show striking differences from other 2D inorganic materials.more » « less
