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1.
Phys Rev Lett ; 132(26): 266505, 2024 Jun 28.
Article in English | MEDLINE | ID: mdl-38996298

ABSTRACT

The properties of kagome metals are governed by the interdependence of band topology and electronic correlations resulting in remarkably rich phase diagrams. Here, we study the temperature evolution of the bulk electronic structure of the antiferromagnetic kagome metal FeGe using infrared spectroscopy. We uncover drastic changes in the low-energy interband absorption at the 100 K structural phase transition that has been linked to a charge-density-wave (CDW) instability. We explain this effect by the minuscule Fe displacement in the kagome plane, which results in parallel bands in the vicinity of the Fermi level. In contrast to conventional CDW materials, however, the spectral weight shifts to low energies, ruling out the opening of a CDW gap in FeGe.

2.
Nat Commun ; 15(1): 5389, 2024 Jun 25.
Article in English | MEDLINE | ID: mdl-38918440

ABSTRACT

Plasmon polaritons, or plasmons, are coupled oscillations of electrons and electromagnetic fields that can confine the latter into deeply subwavelength scales, enabling novel polaritonic devices. While plasmons have been extensively studied in normal metals or semimetals, they remain largely unexplored in correlated materials. In this paper, we report infrared (IR) nano-imaging of thin flakes of CsV3Sb5, a prototypical layered Kagome metal. We observe propagating plasmon waves in real-space with wavelengths tunable by the flake thickness. From their frequency-momentum dispersion, we infer the out-of-plane dielectric function ϵ c that is generally difficult to obtain in conventional far-field optics, and elucidate signatures of electronic correlations when compared to density functional theory (DFT). We propose correlation effects might have switched the real part of ϵ c from negative to positive values over a wide range of middle-IR frequencies, transforming the surface plasmons into hyperbolic bulk plasmons, and have dramatically suppressed their dissipation.

3.
Phys Chem Chem Phys ; 24(11): 6890-6904, 2022 Mar 16.
Article in English | MEDLINE | ID: mdl-35253024

ABSTRACT

Recently, the low-temperature phase of water molecules confined within nanocages formed by the crystalline lattice of water-containing cordierite crystals has been reported to comprise domains with ferroelectrically ordered dipoles within the a, b-planes which are antiferroelectrically alternating along the c-axis. In the present work, comprehensive broad-band dielectric spectroscopy is combined with specific heat studies and molecular dynamics and Monte Carlo simulations in order to investigate in more detail the collective modes and single-particle excitations of nanoconfined water molecules. From DFT-MD simulations we reconstruct the potential-energy landscape experienced by the H2O molecules. A rich set of anisotropic temperature-dependent excitations is observed in the terahertz frequency range. Their origin is associated with the complex rotational/translational vibrations of confined H2O molecules. A strongly temperature dependent relaxational excitation, observed at radio-microwave frequencies for the electric field parallel to the crystallographic a-axis, E||a is analyzed in detail. The temperature dependences of loss-peak frequency and dielectric strength of the excitation together with specific heat data confirm a ferroelectric order-disorder phase transition at T0 ≈ 3 K in the network of H2O dipoles. Additional dielectric data are also provided for polarization E||b, too. Overall, these combined experimental investigations enable detailed conclusions concerning the dynamics of the confined water molecules that develop within their microscopic energy landscapes.

4.
Phys Rev Lett ; 127(7): 076402, 2021 Aug 13.
Article in English | MEDLINE | ID: mdl-34459638

ABSTRACT

The anisotropic optical response of the layered, nodal-line semimetal ZrSiS at ambient and high pressure is investigated by frequency-dependent reflectivity measurements for the polarization along and perpendicular to the layers. The highly anisotropic optical conductivity is in very good agreement with results from density-functional theory calculations and confirms the anisotropic character of ZrSiS. Whereas the in-plane optical conductivity shows only modest pressure-induced changes, we found strong effects on the out-of-plane optical conductivity spectrum of ZrSiS, with the appearance of two prominent excitations. These pronounced pressure-induced effects can neither be attributed to a structural phase transition according to our single-crystal x-ray diffraction measurements, nor can they be explained by electronic correlation and electron-hole pairing effects, as revealed by theoretical calculations. Our findings are discussed in the context of the recently proposed excitonic insulator phase in ZrSiS.

5.
Nat Commun ; 11(1): 3927, 2020 08 06.
Article in English | MEDLINE | ID: mdl-32764722

ABSTRACT

Intermolecular hydrogen bonds impede long-range (anti-)ferroelectric order of water. We confine H2O molecules in nanosized cages formed by ions of a dielectric crystal. Arranging them in channels at a distance of ~5 Å with an interchannel separation of ~10 Å prevents the formation of hydrogen networks while electric dipole-dipole interactions remain effective. Here, we present measurements of the temperature-dependent dielectric permittivity, pyrocurrent, electric polarization and specific heat that indicate an order-disorder ferroelectric phase transition at T0 ≈ 3 K in the water dipolar lattice. Ab initio molecular dynamics and classical Monte Carlo simulations reveal that at low temperatures the water molecules form ferroelectric domains in the ab-plane that order antiferroelectrically along the channel direction. This way we achieve the long-standing goal of arranging water molecules in polar order. This is not only of high relevance in various natural systems but might open an avenue towards future applications in biocompatible nanoelectronics.

6.
Phys Rev Lett ; 125(7): 076403, 2020 Aug 14.
Article in English | MEDLINE | ID: mdl-32857538

ABSTRACT

Temperature- and frequency-dependent infrared spectroscopy identifies two contributions to the electronic properties of the magnetic kagome metal Fe_{3}Sn_{2}: two-dimensional Dirac fermions and strongly correlated flat bands. The interband transitions within the linearly dispersing Dirac bands appear as a two-step feature along with a very narrow Drude component due to intraband contribution. Low-lying absorption features indicate flat bands with multiple van Hove singularities. Localized charge carriers are seen as a Drude peak shifted to finite frequencies. The spectral weight is redistributed when the spins are reoriented at low temperatures; a sharp mode appears suggesting the opening of a gap due to the spin reorientation as the sign of additional Weyl nodes in the system.

7.
J Phys Chem Lett ; 11(9): 3623-3628, 2020 May 07.
Article in English | MEDLINE | ID: mdl-32329348

ABSTRACT

Water at the solid-liquid interface exhibits an anomalous ionic conductivity and dielectric constant compared to bulk water. Both phenomena still lack a detailed understanding. Here, we report radio-frequency measurements and analyses of the electrodynamic properties of interfacial water confined in nanoporous matrices formed by diamond grains of various sizes, ranging from 5 nm to 0.5 µm in diameter. Contrary to bulk water, the charge-carrying protons/holes in interfacial water are not mutually screened, allowing for higher mobility in the external electric field. Thus, the protonic conductivity reaches a maximum value, which can be 5 orders of magnitude higher than that of bulk water. Our results aid in the understanding of physical and chemical properties of water confined in porous materials and pave the way to the development of new type of highly efficient proton-conductive materials for applications in electrochemical energy systems, membrane separations science, and nanofluidics.

8.
Rev Sci Instrum ; 89(5): 054708, 2018 May.
Article in English | MEDLINE | ID: mdl-29864800

ABSTRACT

We present the design, test, and performance of a piston type pressure cell for low-temperature dielectric measurements up to 10 kbar with particular emphasis on the electrical feedthrough for four coaxial cables and four conventional copper wires. The coaxial cables provide proper shielding of the applied test signal; a commercial continuous flow cryostat allows us to minimize the total cable length enabling temperature and pressure-dependent dielectric spectroscopy measurements down to 8 K and up to 5 MHz. We performed open compensation measurements, i.e., background measurements of the response originating from the pressure setup without a sample, to obtain its high frequency characteristics. The stray capacitance of the pressure setup is determined as Cstray = 40 fF, making it possible to measure small single crystals with a weak dielectric response. The proper operation is verified by comparing measurements of a test sample in the pressure setup at ambient pressure and in a standard dielectric spectroscopy setup.

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