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Unusual two-step sequential reversible phase transitions with coexisting switchable nonlinear optical and dielectric behaviors in [(CH3)3NCH2Cl]2[ZnCl4]

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Abstract

A novel material with coexisting switchable nonlinear optical (NLO) and dielectric properties, [trimethylchloromethyl ammonium]2[ZnCl4] [(TMCM)2-ZnCl4], which undergoes two reversible solid state phase transitions at 337 K (Tc1) and 258 K (Tc2), respectively, has been successfully synthesized and grown as block crystals. Exceptionally, variable-temperature X-ray single crystal structural analyses of (TMCM)2-ZnCl4 reveal that the unusual space group changes from P212121 at 223 K to P21/c between Tc2 and Tc1 to Pmcn above Tc1. As expected, the dielectric value of (TMCM)2-ZnCl4 exhibits two remarkable step-like enlargements around Tc1 and Tc2, indicating that it exhibits a low dielectric state, an intermediate dielectric state and a high dielectric state. In particular, the second harmonic generation (SHG) efficiency shows a sharp step-like increase from almost zero to 0.47, and its SHG activities in a high-NLO state can be recovered after several cycles without any attenuation. The transitions of (TMCM)2-ZnCl4 could be intrinsically ascribed to the sequential order–disorder transformations of both the cations and anions. All these results demonstrate its potential application as a switchable and tunable molecular dielectric and NLO material.

Graphical abstract: Unusual two-step sequential reversible phase transitions with coexisting switchable nonlinear optical and dielectric behaviors in [(CH3)3NCH2Cl]2[ZnCl4]

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Publication details

The article was received on 07 Sep 2017, accepted on 01 Nov 2017 and first published on 01 Nov 2017


Article type: Paper
DOI: 10.1039/C7TC04095D
Citation: J. Mater. Chem. C, 2017, Advance Article
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    Unusual two-step sequential reversible phase transitions with coexisting switchable nonlinear optical and dielectric behaviors in [(CH3)3NCH2Cl]2[ZnCl4]

    W. Liao, J. Gao, X. Hua, X. Chen and Y. Lu, J. Mater. Chem. C, 2017, Advance Article , DOI: 10.1039/C7TC04095D

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