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The rare-earth tritellurides (RTe 3 ) are a distinct class of 2D layered materials that recently gained significant attention due to hosting such quantum collective phenomena as superconductivity or charge density waves (CDWs). Many members of this van der Waals (vdW) family crystals exhibit CDW behavior at room temperature, i.e. , RTe 3 compound where R = La, Ce, Pr, Nd, Sm, Gd, and Tb. Here, our systematic studies establish the CDW properties of RTe 3 when the vdW spacing/interaction strength between adjacent RTe 3 layers is engineered under extreme hydrostatic pressures. Using a non-destructive spectroscopy technique, pressure-dependent Raman studies first establish the pressure coefficients of phonon and CDW amplitude modes for a variety of RTe 3 materials, including LaTe 3 , CeTe 3 , PrTe 3 , NdTe 3 , SmTe 3 , GdTe 3 , and TbTe 3 . Results further show that the CDW phase is eventually suppressed at high pressures when the interlayer spacing is reduced and interaction strength is increased. Comparison between different RTe 3 materials shows that LaTe 3 with the largest thermodynamic equilibrium interlayer spacing (smallest chemical pressure) exhibits the most stable CDW phases at high pressures. In contrast, CDW phases in late RTe 3 systems with the largest internal chemical pressures are suppressed easily with applied pressure. Overall results provide comprehensive insights into the CDW response of the entire RTe 3 series under extreme pressures, offering an understanding of CDW formation/engineering in a unique class of vdW RTe 3 material systems.
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Two-dimensional charge order stabilized in clean polytype heterostructures
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.
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- PAR ID:
- 10324028
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 13
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Van der Waals bilayers assembled by mechanical stacking of 2D layers have been shown to realize symmetry‐breaking mechanisms, such as sliding‐ or moiré ferroelectricity, which are without equivalent in 3D ferroelectrics. Here, we discuss emergent, highly unconventional behavior in thicker semiconducting few‐layer SnS(e) van der Waals ferroelectrics crystallizing in a distorted polar structure, obtained by bottom‐up synthesis. Electron diffraction at variable temperature demonstrates a gradual displacive transformation between the polar low‐temperature and symmetric high‐temperature phase, with significant variability in both the lattice constants and the Curie temperature (TC) where the transition is completed. Strikingly, such variations are even found among stripe domains in individual crystals, where lattice constants and distortion angles change periodically between adjacent domains. The resulting spontaneously formed homo‐materials superlattices imply that such ferroelectrics adopt domain‐specific Curie temperatures, in sharp contrast with the long‐held notion of TC as a global materials parameter for a given ferroelectric.more » « less
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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 A charge density wave (CDW) represents an exotic state in which electrons are arranged in a long‐range ordered pattern in low‐dimensional materials. Although the understanding of the fundamental character of CDW is enriched after extensive studies, its practical application remains limited. Here, an unprecedented demonstration of a tunable charge‐spin interconversion (CSI) in graphene/1T‐TaS2van der Waals heterostructures is shown by manipulating the distinct CDW phases in 1T‐TaS2. Whereas CSI from spins polarized in all three directions is observed in the heterostructure when the CDW phase does not show commensurability, the output of one of the components disappears, and the other two are enhanced when the CDW phase becomes commensurate. The experimental observation is supported by first‐principles calculations, which evidence that chiral CDW multidomains in the heterostructure are at the origin of the switching of CSI. The results uncover a new approach for on‐demand CSI in low‐dimensional systems, paving the way for advanced spin‐orbitronic devices.more » « less
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1038/s41467-021-27947-5
