The transition metal selenides M1+
TiSe2is an exciting material because it can be tuned between superconducting and charge density wave (CDW) transitions. In the monolayer limit, TiSe2exhibits a sizable energy gap in the CDW phase that makes it a promising quantum material. It is shown that interfacing a single layer of TiSe2with dissimilar van der Waals materials enables control of its properties. Using angle‐resolved photoemission spectroscopy, the energy gap opening is analyzed as a function of temperature for TiSe2monolayers supported on different van der Waals substrates. A substantial increase in the CDW transition temperature of ≈45 K is observed on MoS2compared to graphite (highly oriented pyrolytic graphite) substrates. This control of the CDW in monolayer TiSe2is suggested to arise from varying charge screening of the unconventional CDW of TiSe2by the substrate. In addition, the suppression of CDW order and a complete closing of the energy gap by electron doping of monolayer TiSe2is demonstrated. Regulating the many‐body physics phenomena in monolayer TiSe2lays the foundation of modifying TiSe2in, for example, artificial van der Waals heterostructures and thus creates a new approach for utilizing the quantum states of TiSe2in device applications.
more » « less- Award ID(s):
- 1701390
- NSF-PAR ID:
- 10078133
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Quantum Technologies
- Volume:
- 1
- Issue:
- 3
- ISSN:
- 2511-9044
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract y Se2(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. -
Recently a new research field of quasi-one-dimensional (1D) van der Waals quantummaterials has emerged from earlier work on low-dimensional systems [1-2]. The quasi-1D van der Waalsmaterials have 1D motifs in their crystal structure [1]. Many of these materials reveal strongly correlatedphenomena such as charge density waves (CDW) [1-2]. The CDW phase is a periodic modulation of theelectronic charge density, accompanied by distortions in the underlying crystal lattice. Potential uses for CDWmaterials include memory storage and oscillators [3]. Raman spectroscopy can identify the CDW transitions todifferent phases via the appearance of phonon peaks due to emerging superstructure or the disappearance ofcertain peaks due to the loss of translation symmetry in the crystal lattice [3]. In this presentation, we report theresults of the angle and temperature-dependent Raman scattering spectroscopy investigation of themechanically exfoliated nanowires of the quasi-1D Nb van der Waals material. It is known that Nb forms in atetragonal crystal structure with space group 124 (P4/mcc). Recently, this material attracted attention as aCDW material with multiple phase transitions, some of them, possibly, near room temperature. Littleinformation is known on the Raman characteristics of this material. Our Raman data for different polarizationangles show strong anisotropy in the response depending on the crystal direction. The most pronouncedRaman peaks reveal strong temperature dependence. The results of the measurements will be compared withthe theoretical predictions. Our data is important for further investigation of this quasi-1D CDW material forpossible applications in phase-change memory and reconfigurable devices. A.A.B. acknowledges the support of the Vannevar Bush Faculty Fellowship (VBFF) from the Office of NavalResearch (ONR) contract N00014-21-1-2947 “One-Dimensional Quantum Materials” and the National ScienceFoundation (NSF) program Designing Materials to Revolutionize and Engineer our Future (DMREF) via aproject DMR-1921958 “Data-Driven Discovery of Synthesis Pathways and Distinguishing ElectronicPhenomena of 1D van der Waals Bonded Solids”. A. D. and S. K. acknowledge support through the MaterialGenome Initiative funding allocated to the National Institute of Standards and Technology. [1] A. A. Balandin, F. Kargar, T. T. Salguero, and R. Lake, “One-dimensional van der Waals quantummaterials", Mater. Today, 55, 74 (2022). [2] A. A. Balandin, R. K. Lake, and T. T. Salguero, "One-dimensional van der Waals materials - Advent of a newresearch field" Appl. Phys. Lett., 121, 040401 (2022). [3] A. A. Balandin, S. V. Zaitzev-Zotov, and G. Grüner, "Charge-density-wave quantum materials and devices—New developments and future prospects", Appl. Phys. Lett., 119, 170401 (2021). [4] R. Samnakay, et al., “Zone-folded phonons and the charge-density-wave transition in 1T-TaSe2 thin films, Nano Lett., 15, 2965 (2015).more » « less
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Abstract Body: Recently a new research field of quasi-one-dimensional (1D) van der Waals quantummaterials has emerged from earlier work on low-dimensional systems [1-2]. The quasi-1D van der Waalsmaterials have 1D motifs in their crystal structure [1]. Many of these materials reveal strongly correlatedphenomena such as charge density waves (CDW) [1-2]. The CDW phase is a periodic modulation of theelectronic charge density, accompanied by distortions in the underlying crystal lattice. Potential uses for CDWmaterials include memory storage and oscillators [3]. Raman spectroscopy can identify the CDW transitions todifferent phases via the appearance of phonon peaks due to emerging superstructure or the disappearance ofcertain peaks due to the loss of translation symmetry in the crystal lattice [3]. In this presentation, we report theresults of the angle and temperature-dependent Raman scattering spectroscopy investigation of themechanically exfoliated nanowires of the quasi-1D Nb van der Waals material. It is known that Nb forms in atetragonal crystal structure with space group 124 (P4/mcc). Recently, this material attracted attention as aCDW material with multiple phase transitions, some of them, possibly, near room temperature. Littleinformation is known on the Raman characteristics of this material. Our Raman data for different polarizationangles show strong anisotropy in the response depending on the crystal direction. The most pronouncedRaman peaks reveal strong temperature dependence. The results of the measurements will be compared withthe theoretical predictions. Our data is important for further investigation of this quasi-1D CDW material forpossible applications in phase-change memory and reconfigurable devices. A.A.B. acknowledges the support of the Vannevar Bush Faculty Fellowship (VBFF) from the Office of NavalResearch (ONR) contract N00014-21-1-2947 “One-Dimensional Quantum Materials” and the National ScienceFoundation (NSF) program Designing Materials to Revolutionize and Engineer our Future (DMREF) via aproject DMR-1921958 “Data-Driven Discovery of Synthesis Pathways and Distinguishing ElectronicPhenomena of 1D van der Waals Bonded Solids”. A. D. and S. K. acknowledge support through the MaterialGenome Initiative funding allocated to the National Institute of Standards and Technology. [1] A. A. Balandin, F. Kargar, T. T. Salguero, and R. Lake, “One-dimensional van der Waals quantummaterials", Mater. Today, 55, 74 (2022). [2] A. A. Balandin, R. K. Lake, and T. T. Salguero, "One-dimensional van der Waals materials - Advent of a newresearch field" Appl. Phys. Lett., 121, 040401 (2022). [3] A. A. Balandin, S. V. Zaitzev-Zotov, and G. Grüner, "Charge-density-wave quantum materials and devices—New developments and future prospects", Appl. Phys. Lett., 119, 170401 (2021). [4] R. Samnakay, et al., “Zone-folded phonons and the charge-density-wave transition in 1T-TaSe2 thin films,” Nano Lett., 15, 2965 (2015).more » « less
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Abstract Van der Waals (vdW) materials are an indispensable part of functional device technology due to their versatile physical properties and ease of exfoliating to the low‐dimensional limit. Among all the compounds investigated so far, the search for magnetic vdW materials has intensified in recent years, fueled by the realization of magnetism in 2D. However, metallic magnetic vdW systems are still uncommon. In addition, they rarely host high‐mobility charge carriers, which is an essential requirement for high‐speed electronic applications. Another shortcoming of 2D magnets is that they are highly air sensitive. Using chemical reasoning, TaCo2Te2is introduced as an air‐stable, high‐mobility, magnetic vdW material. It has a layered structure, which consists of Peierls distorted Co chains and a large vdW gap between the layers. It is found that the bulk crystals can be easily exfoliated and the obtained thin flakes are robust to ambient conditions after 4 months of monitoring using an optical microscope. Signatures of canted antiferromagntic behavior are also observed at low‐temperature. TaCo2Te2shows a metallic character and a large, nonsaturating, anisotropic magnetoresistance. Furthermore, the Hall data and quantum oscillation measurements reveal the presence of both electron‐ and hole‐type carriers and their high mobility.
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Van der Waals heterojunctions of two-dimensional transition-metal dichalcogenides are intensely investigated for multiple optoelectronics applications. Strong and adjustable interactions between layers can influence the charge and energy flow that govern material performance. We report ab initio quantum molecular dynamics investigation of the influence of the bilayer twist angle on charge transfer and recombination in MoS 2 /WS 2 heterojunctions, including high-symmetry 0° and 60° configurations, and low symmetry 9.43° and 50.57° structures with Moiré patterns. The twist angle modulates interlayer coupling, as evidenced by changes in the interlayer distance, electron-vibrational interactions, and spectral shifts in the out-of-plane vibrational frequencies. Occurring on a femtosecond timescale, the hole transfer depends weakly on the twist angle and is ultrafast due to high density of acceptor states and large nonadiabatic coupling. In contrast, the electron–hole recombination takes nanoseconds and varies by an order of magnitude depending on the twist angle. The recombination is slow because it occurs across a large energy gap. It depends on the twist angle because the nonadiabatic coupling is sensitive to the interlayer distance and overlap of electron and hole wavefunctions. The Moiré pattern systems exhibit weaker interlayer interaction, generating longer-lived charges. Both charge separation and recombination are driven by out-of-plane vibrational motions. The simulations rationalize the experimental results on the influence of the bilayer twist angle on the charge separation and recombination. The atomistic insights provide theoretical guidance for design of high-performance optoelectronic devices based on 2D van der Waals heterostructures.more » « less
