Water is characterized by large molecular electric dipole moments and strong interactions between molecules; however, hydrogen bonds screen the dipole-dipole coupling and suppress the ferroelectric ...order. The situation changes drastically when water is confined: in this case ordering of the molecular dipoles has been predicted, but never unambiguously detected experimentally. In the present study we place separate H
O molecules in the structural channels of a beryl single crystal so that they are located far enough to prevent hydrogen bonding, but close enough to keep the dipole-dipole interaction, resulting in incipient ferroelectricity in the water molecular subsystem. We observe a ferroelectric soft mode that causes Curie-Weiss behaviour of the static permittivity, which saturates below 10 K due to quantum fluctuations. The ferroelectricity of water molecules may play a key role in the functioning of biological systems and find applications in fuel and memory cells, light emitters and other nanoscale electronic devices.
Intermolecular hydrogen bonds impede long-range (anti-)ferroelectric order of water. We confine H
O 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 T
≈ 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.
We describe the first-principles design and subsequent synthesis of a new material with the specific functionalities required for a solid-state-based search for the permanent electric dipole moment ...of the electron. We show computationally that perovskite-structure europium barium titanate should exhibit the required large and pressure-dependent ferroelectric polarization, local magnetic moments and absence of magnetic ordering at liquid-helium temperature. Subsequent synthesis and characterization of Eu(0.5)Ba(0.5)TiO(3) ceramics confirm the predicted desirable properties.
•EuRu2P2 is a ferromagnet with a small anisotropy with a as an easy magnetization axis.•The magnetocrystalline anisotropy was confirmed by ab-initio calculations.•Full saturated magnetic moment ...confirms the Eu2 + state over all pressures.•Sudden drop of Tc at 1.5 GPa is ascribed to the lattice compressibility change.
The EuRu2P2 single crystal was investigated by means of magnetic, transport and thermodynamic studies at ambient and hydrostatic pressures. A small magnetocrystalline anisotropy with crystallographic 100 direction as an easy magnetization direction was found by experimental measurements and confirmed by first-principles calculations. We connect a previously reported change in the compressibility observed at room temperature to a rapid change of ordering temperature under applied hydrostatic pressure.
We report on single crystal growth and crystallographic parameters results of Ce2PdIn8, Ce3PdIn11, Ce2PtIn8 and Ce3PtIn11. The Pt-systems Ce2PtIn8 and Ce3PtIn11 are synthesized for the first time. ...All these compounds are member of CenTmIn3n+2m (n=1, 2,..; m=1, 2,.. and T= transition metal) to which the extensively studied heavy fermion superconductor CeCoIn5 belongs. Single crystals have been grown by an In self-flux method. Differential scanning calorimetry studies were used to derive optimal growth conditions. Evidently, the maximum growth conditions for these materials should not exceed 750°C. Single crystal x-ray data show that Ce2TIn8 compounds crystallize in the tetragonal Ho2CoGa8 phase (space group P4/mmm) with lattice parameters a=4.6898(3)Å and c=12.1490(8)Å for Pt-based one (Pd: a=4.6881(4)Å and c=12.2031(8)Å). Ce3TIn11 compounds adopt Ce3PdIn11 structure with a=4.6874(4)Å and c=16.8422(12)Å for Pt-based one (Pd: a=4.6896Å and c=16.891Å). Specific heat experiments on Ce3PtIn11 and Ce3PdIn11 have revealed that both compounds undergo two successive magnetic transitions at T1 ~2.2K followed by TN ~2.0K and T1 ~1.7K and TN ~1.5K, respectively. In addition, both compounds exhibit enhanced Sommerfeld coefficients yielding γPt=0.300J/molK2 Ce (γPd=0.29J/molK2 Ce), hence qualifying them as heavy fermion materials.
•We have prepared single crystals of Ce2PdIn8, Ce3PdIn11, Ce2PtIn8 and Ce3PtIn11.•According to thermal analysis the maximum growth temperature should not exceed 750°C.•Complete structural parameters were obtained from single crystal diffraction studies.•Ce3TIn11 compounds order magnetically and reveal enhanced Sommerfeld coefficients.
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 H
2
O 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 H
2
O 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
T
0
3 K in the network of H
2
O 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.
Dielectric spectroscopy along with MD and MC simulations was used to study the excitations of nanoconfined water molecules in cordierite nanocages.
Many current research efforts in strongly correlated systems focus on the interplay between magnetism and superconductivity. Here we report on coexistence of both cooperative ordered states in ...recently discovered stoichiometric and fully inversion symmetric heavy fermion compound Ce3PdIn11 at ambient pressure. Thermodynamic and transport measurements reveal two successive magnetic transitions at T1 = 1.67 K and TN = 1.53 K into antiferromagnetic type of ordered states. Below Tc = 0.42 K the compound enters a superconducting state. The large initial slope of dBc2/dT ≈ - 8.6 T/K indicates that heavy quasiparticles form the Cooper pairs. The origin of the two magnetic transitions and the coexistence of magnetism and superconductivity is briefly discussed in the context of the coexistence of the two inequivalent Ce-sublattices in the unit cell of Ce3PdIn11 with different Kondo couplings to the conduction electrons.
There is an ongoing dispute in the community about the absence of a magnetic quantum critical point (QCP) in the noncentrosymmetric heavy fermion compound CeRhSi3. In order to explore this question ...we prepared single crystals of CeRh(Si1−xGex)3 with x = 0.05 and 0.15 and determined the temperature-pressure (T-p) phase diagram by means of measurements of the electrical resistivity. The substitution of isoelectronic but large Ge enforces a lattice volume increase resulting in a weakening of the Kondo interaction. As a result, the x = 0.05 and x = 0.15 compound exhibit a transition into the antiferromagnetic (AFM) at higher temperatures being TN = 4.7 K and TN1 = 19.7 K, respectively. Application of pressure suppresses TN (TN1) monotonically and pressure induced superconductivity is observed in both Ge-substituted compounds above p ⩾ 2.16 GPa (x = 0.05) and p ⩾ 2.93 GPa (x = 0.15). Extrapolation of TN(p) → 0 of CeRh(Si0.95Ge0.05)3 yields a critical pressure of pc ≈ 3.4 GPa (in CeRh(Si0.85Ge0.15)3 pc ≈ 3.5 GPa) pointing to the presence of an AFM QCP located deep inside the superconducting state.
A comprehensive study of magnetocrystalline anisotropy of a layered van der Waals ferromagnet VI3 was performed. We measured angular dependences of the torque and magnetization with respect to the ...direction of the applied magnetic field within the basal ab plane and a general orthogonal plane to ab, respectively. A twofold butterflylike signal was detected by magnetization in the orthogonal plane. This signal symmetry remains conserved throughout all magnetic regimes as well as through the known structural transition down to the lowest temperatures. The maximum of the magnetization signal and the resulting magnetization easy axis is significantly tilted from the normal to the basal ab plane by ∼40°. The close relation of the magnetocrystalline anisotropy to the crystal structure was documented. In contrast, a two-fold-like angular signal was detected in the paramagnetic region within the ab plane in the monoclinic phase, which transforms into a six-fold-like signal below the Curie temperature TC. With further cooling, another six-fold-like signal with an angular shift of ∼30° grows approaching TFM. Below TFM, in the triclinic phase, the original six-fold-like signal vanishes, being replaced by a secondary six-fold-like signal with an angular shift of ∼30°.
In this paper, we report the results of a high pressure study of the itinerant 5f-electron ferromagnet UCoGa. The work is focused on probing the expected ferromagnet-to-paramagnet quantum phase ...transition induced by high pressure and on the general features of the P-T(-H) phase diagram. Diamond anvil cells were employed to measure the magnetization and electrical resistivity under pressures up to ∼ 10 GPa. At ambient pressure, UCoGa exhibits collinear ferromagnetic ordering of uranium magnetic moments
μ
U
∼
0.74
μ
B
(at 2 K) aligned along the c-axis of the hexagonal crystal structure below Curie temperature TC = 48K. With the application of pressure, gradual decrease of both, TC and the saturated magnetic moment, has been observed up to pressures ∼ 6 GPa. This is followed by a sharp drop of magnetic moment and a sudden disappearance of the magnetic order at the pressure of 6.5 GPa, suggesting a first-order phase transition, as expected for a clean system. The low temperature power law dependence of the electrical resistivity shows distinct anomalies around the ∼ 6 GPa, consistent with the pressure evolution of the magnetic moment and the ordering temperature. The tricritical point of the UCoGa phase diagram is located at approximately ∼ 30K and ∼ 6GPa.
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