Single-particle and collective excitations of polar water molecules confined in nano-pores within a cordierite crystal lattice

M. A. Belyanchikov; Z. V. Bedran; M. Savinov; P. Bednyakov; P. Proschek; J. Prokleska; V. A. Abalmasov; E. S. Zhukova; V. G. Thomas; A. Dudka; A. Zhugayevych; J. Petzelt; A. S. Prokhorov; V. B. Anzin; R. K. Kremer; J. K. H. Fischer; P. Lunkenheimer; A. Loidl; E. Uykur; M. Dressel; B. Gorshunov

doi:10.1039/D1CP05338H

Single-particle and collective excitations of polar water molecules confined in nano-pores within a cordierite crystal lattice†

M. A. Belyanchikov,

^a Z. V. Bedran,^a M. Savinov,^b P. Bednyakov,^b P. Proschek,^c J. Prokleska,^c V. A. Abalmasov,^d E. S. Zhukova,^a V. G. Thomas,

^ef A. Dudka,^g A. Zhugayevych,

^h J. Petzelt,^b A. S. Prokhorov,^ai V. B. Anzin,^ai R. K. Kremer,^j J. K. H. Fischer,

‡^k P. Lunkenheimer,

^k A. Loidl,

^k E. Uykur,^l M. Dressel

^al and B. Gorshunov*^a

Author affiliations

* Corresponding authors

^a Moscow Institute of Physics and Technology, 141700 Dolgoprudny, Moscow Region, Russia

^b Institute of Physics, Czech Academy of Sciences, 18221 Praha 8, Czech Republic

^c Department of Condensed Matter Physics, Faculty of Mathematics and Physics, Charles University, 12116 Prague 2, Czech Republic

^d Institute of Automation and Electrometry SB RAS, 630090 Novosibirsk, Russia

^e Sobolev Institute of Geology and Mineralogy, RAS, 630090 Novosibirsk, Russia

^f Novosibirsk State University, 630090 Novosibirsk, Russia

^g Shubnikov Institute of Crystallography, “Crystallography and Photonics”, Russian Academy of Sciences, 119333 Moscow, Russia

^h Skolkovo Institute of Science and Technology, 143026 Moscow, Russia

ⁱ Prokhorov General Physics Institute of the Russian Academy of Sciences, Moscow, Russia

^j Max-Planck-Institut für Festkörperforschung, 70569 Stuttgart, Germany

^k Experimental Physics V, University of Augsburg, 86135 Augsburg, Germany

^l 1. Physikalisches Institut, Universität Stuttgart, 70569 Stuttgart, Germany

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.

Physical Chemistry Chemical Physics

Single-particle and collective excitations of polar water molecules confined in nano-pores within a cordierite crystal lattice†

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Single-particle and collective excitations of polar water molecules confined in nano-pores within a cordierite crystal lattice

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