Repozytorium

Cyano-bridged perovskite [(CH3)3NOH]2[KM(CN)6], [M: Fe(III), and Co(III)] for high-temperature multi-axial ferroelectric applications with enhanced thermal and nonlinear optical performance.

Autorzy

Magdalena Rok

Agnieszka Ciżman

Bartosz Zarychta

Jan K. Zaręba

Monika Trzebiatowska

Mirosław Mączka

Alessandro Stroppa

Shurong Yuan

Anthony E. Phillips

Grażyna Bator

Rok wydania

2020

Czasopismo

Journal of Materials Chemistry C

Numer woluminu

8

Strony

17491-17501

DOI

10.1039/d0tc04527f

Kolekcja

Naukowa

Język

Angielski

Typ publikacji

Artykuł

Streszczenie

Highly stable ferroelectrics with reversible high-temperature phase transitions and switchable nonlinear optical behaviour are much coveted targets for emerging optoelectronic applications. Here, we demonstrate a cyano-bridged perovskite [(CH3)3NOH]2[KCo(CN)6] (TMAO-Co), a new analogue of the multi-axial ferroelectric [(CH3)3NOH]2[KFe(CN)6] (TMAO-Fe) with improved thermal stability and enhanced second-order nonlinear optical response. Indeed, for TMAO-Co the Curie temperature (Tc) is shifted to a higher value of ca. 416 K (improvement by ca. 10 K versus TMAO-Fe); the separation between Tc and the decomposition threshold is 46 K. TMAO-Co is a biaxial ferroelectric as revealed by P(E) hysteresis loop measurements along the a and c crystallographic directions with spontaneous polarization values of 0.9 and 0.63 μC cm−2 at 293 K, respectively. The SHG response of TMAO-Co is two times higher than that of TMAO-Fe. The improved stability of TMAO-Co to thermal and optical loads allowed for demonstration of bistable switching of nonlinear optical response between SHG-on and SHG-off states by temperature sweeping. Structurally, TMAO-Co reproduces the unusual characteristics of TMAO-Fei.e. the first-order phase transition between (polar) monoclinic to (nonpolar) cubic phases involving bond switching and is assisted by the pronounced increase of disorder of the TMAO cations above Tc. Combined temperature-resolved Raman and infrared spectroscopic measurements were employed to track the symmetry increase above Tc, which is primarily associated with changes in hydrogen-bonding. Consistent with the bond-switching character of the phase transitions, a pronounced shift to higher wavenumbers is observed for the O–H stretching modes. The DFT calculations demonstrate that the system's polarization along the a-axis mostly comes from the rotation of the [(CH3)3NOH]2 cluster, while the atomic displacement of the framework contributes largely to that along the c axis.

Adres publiczny

http://dx.doi.org/10.1039/d0tc04527f

Strona internetowa wydawcy

https://www.rsc.org/

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Phase transition tuning by Fe(III)/Co(III) substitution in switchable cyano-bridged perovskites: (C3H5N2)2[KFexCo1-x(CN)6].

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