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  1. One-dimensional (1D) van der Waals (vdW) materials display electronic and magnetic transport properties that make them uniquely suited as interconnect materials and for low-dimensional optoelectronic applications. However, there are only around 700 1D vdW structures in general materials databases, making database curation approaches ineffective for 1D discovery. Here, we utilize machine-learning techniques to discover 1D vdW compositions that have not yet been synthesized. Our techniques go beyond discovery efforts involving elemental substitutions and instead start with a composition space of 4741 binary and 392,342 ternary formulas. We predict up to 3000 binary and 10,000 ternary 1D compounds and further classify them by expected magnetic and electronic properties. Our model identifies MoI3, a material we experimentally confirm to exist with wire-like subcomponents and exotic magnetic properties. More broadly, we find several chalcogen-, halogen-, and pnictogen-containing compounds expected to be synthesizable using chemical vapor deposition and chemical vapor transport. 
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    Free, publicly-accessible full text available November 9, 2024
  2. Free, publicly-accessible full text available October 1, 2024
  3. Abstract

    The development of cryogenic semiconductor electronics and superconducting quantum computing requires composite materials that can provide both thermal conduction and thermal insulation. We demonstrated that at cryogenic temperatures, the thermal conductivity of graphene composites can be both higher and lower than that of the reference pristine epoxy, depending on the graphene filler loading and temperature. There exists a well-defined cross-over temperature—above it, the thermal conductivity of composites increases with the addition of graphene; below it, the thermal conductivity decreases with the addition of graphene. The counter-intuitive trend was explained by the specificity of heat conduction at low temperatures: graphene fillers can serve as, both, the scattering centers for phonons in the matrix material and as the conduits of heat. We offer a physical model that explains the experimental trends by the increasing effect of the thermal boundary resistance at cryogenic temperatures and the anomalous thermal percolation threshold, which becomes temperature dependent. The obtained results suggest the possibility of using graphene composites for, both, removing the heat and thermally insulating components at cryogenic temperatures—a capability important for quantum computing and cryogenically cooled conventional electronics.

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  4. null (Ed.)
    Recent years have witnessed a much broader use of Brillouin inelastic light-scattering spectroscopy for the investigation of phonons and magnons in novel materials, nanostructures and devices. Driven by the developments in instrumentation and the strong need for accurate knowledge on the energies of elemental excitations, Brillouin–Mandelstam spectroscopy is rapidly becoming an essential technique that is complementary to Raman inelastic light-scattering spectroscopy. We provide an overview of recent progress in the Brillouin light-scattering technique, focusing on the use of this photonic method for the investigation of confined acoustic phonons, phononic metamaterials and magnon propagation and scattering. This Review emphasizes the emerging applications of Brillouin–Mandelstam spectroscopy for phonon-engineered structures and spintronic devices, and concludes with a perspective on future directions. 
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  5. We conducted a tip-enhanced Raman scattering spectroscopy (TERS) and photoluminescence (PL) study of quasi-1D TaSe 3− δ nanoribbons exfoliated onto gold substrates. At a selenium deficiency of δ ∼ 0.25 (Se/Ta = 2.75), the nanoribbons exhibit a strong, broad PL peak centered around ∼920 nm (1.35 eV), suggesting their semiconducting behavior. Such nanoribbons revealed a strong TERS response under 785 nm (1.58 eV) laser excitation, allowing for their nanoscale spectroscopic imaging. Nanoribbons with a smaller selenium deficiency (Se/Ta = 2.85, δ ∼ 0.15) did not show any PL or TERS response. The confocal Raman spectra of these samples agree with the previously-reported spectra of metallic TaSe 3 . The differences in the optical response of the nanoribbons examined in this study suggest that even small variations in Se content can induce changes in electronic band structure, causing samples to exhibit either metallic or semiconducting character. The temperature-dependent electrical measurements of devices fabricated with both types of materials corroborate these observations. The density-functional-theory calculations revealed that substitution of an oxygen atom in a Se vacancy can result in band gap opening and thus enable the transition from a metal to a semiconductor. However, the predicted band gap is substantially smaller than that derived from the PL data. These results indicate that the properties of van der Waals materials can vary significantly depending on stoichiometry, defect types and concentration, and possibly environmental and substrate effects. In view of this finding, local probing of nanoribbon properties with TERS becomes essential to understanding such low-dimensional systems. 
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  6. null (Ed.)
  7. Abstract

    We report the results of polarization‐dependent Raman spectroscopy of phonon states in single‐crystalline quasi‐one‐dimensional NbTe4and TaTe4van der Waals materials. The measurements were conducted in the wide temperature range from 80 to 560 K. Our results show that although both materials have identical crystal structures and symmetries, there is a drastic difference in the intensity of their Raman spectra. While TaTe4exhibits well‐defined peaks through the examined wavenumber and temperature ranges, NbTe4reveals extremely weak Raman signatures. The measured spectral positions of the phonon peaks agree with the phonon band structure calculated using the density‐functional theory. We offer possible reasons for the intensity differences between the two van der Waals materials. Our results provide insights into the phonon properties of NbTe4and TaTe4van der Waals materials and indicate the potential of Raman spectroscopy for studying charge‐density‐wave quantum condensate phases.

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