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. 2019 Dec 17;9(71):41832-41836.
doi: 10.1039/c9ra09224b. eCollection 2019 Dec 13.

A breakthrough in the intrinsic multiferroic temperature region in Prussian blue analogues

Qingrong Kong  1 , Ruixuan Qin  1 , Dong Li  1 , Haixia Zhao  1 , Yanping Ren  1 , Lasheng Long  1 , Lansun Zheng  1
Affiliations

A breakthrough in the intrinsic multiferroic temperature region in Prussian blue analogues

Qingrong Kong et al. RSC Adv. .

Abstract

Thin films of [(FeII x CrII 1-x )]1.5[CrIII(CN)6]·yH2O (x ≈ 0.30-0.35, y ≈ 1.77) (1) on FTO substrates (namely film 1) were synthesized with an electrochemical method. Investigation of the ferroelectricity of film 1 at different temperatures reveals that it exhibits ferroelectric behaviour in the temperature range from 10 K to 310 K. Study of the X-ray absorption (XAS) of the crushed film 1 and simulation of the structure of film 1 and crushed film 1 by using the Materials Studio software indicate that the vacancy defects and interactions between the film and FTO substrate make a key contribution to the ferroelectricity of film 1. Owing to the magnetic phase transition point being up to 210 K, film 1 is a multiferroic material and its magneto/electric coexistence temperature can be as high as 210 K.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. Polarization versus electric field curve (P–E hysteresis loop) at different temperatures (a) 10 K, (b) 100 K, (c) 300 K, (d) 310 K of film 1.
Fig. 2
Fig. 2. PFM measurements of film 1. (a) PFM phase mapping. (b) PFM amplitude mapping image overlaid on the 3D topography (5 × 5 μm2). (c) PFM phase hysteresis loop. (d) PFM butterfly loop.
Fig. 3
Fig. 3. Fourier transform (a) Fe K-edge and (b) Cr K-edge EXAFS of 1, (NH4)Fe[Fe(CN)4]·xH2O, K3Cr(CN)6, Fe foil and Cr foil respectively.
Fig. 4
Fig. 4. Schematic illustration of the structure in the ternary metal Prussian blue 1 (the solvent water molecules in the hole were omitted for clarity). (a) The crush film structure of F23 space group with twelve symmetric elements (E, 8C3, 3C2). (b) The film structure of C2 space group with two (E, C2) symmetric elements. (c) The dipole moment of the CN–CrII/FeII–OH2 around vacancies of [CrIII(CN)6]3− in F23 space group. (d) The dipole moment of the CN–CrII/FeII–OH2 around vacancies of [CrIII(CN)6]3− in C2 space group.
Fig. 5
Fig. 5. (a) The temperature-dependent dielectric constant of the film 1 at f = 10 kHz (blue), and thermal variation of χm measured at 10 Oe (black), respectively. (b) P–E hysteresis loop near the magnetic phase transition temperature of film 1.
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