Abstract

Stimuli-responsive materials with coexisting nonlinear optical (NLO) and dielectric properties are technologically important, which enable simultaneous conversion of optoelectronic properties between different states under external stimuli. By rationally screening guest cations (C6H5NF2)+ in the crown-ether inclusion system, we synthesized a crown-ether supramolecular compound [(C6H5NF2)(18-crown-6)][PF6] (1). Differential scanning calorimetry (DSC) showed that 1 undergoes a reversible phase transition above room temperatures (305 K/292 K), with a thermal hysteresis of 13 K. Temperature-dependent dielectric and NLO measurements show that the compound exhibits two distinct switching response behaviors. Structural analysis indicates that the order–disorder change of the host molecule 18-crown-6 and the guest organic cation during the phase transition induces the dielectric and NLO switching behavior of the compound.

Highlights

  • IntroductionAs an important class of functional materials, compounds with switchable physical properties via optical, electrical, magnetic, or mechanical manipulation are technologically important, because they can be used in a wide range of applications, including switches and memory devices [1,2,3,4,5]

  • As an important class of functional materials, compounds with switchable physical properties via optical, electrical, magnetic, or mechanical manipulation are technologically important, because they can be used in a wide range of applications, including switches and memory devices [1,2,3,4,5].Recently, a great deal of effort in this field has been devoted to the design of molecule-based materials with multiple switching effects of physical properties for potential application in the fields of digital processing, optoelectronic devices, and sensors [6,7,8]

  • This is due to the structural characteristics of the supramolecular compounds, where the dipolar rotator molecules undergo the order–disorder change, leading to rich structural phase transitions accompanied by ferroelectric, dielectric, and nonlinear optical (NLO) switching, as exemplified by

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Summary

Introduction

As an important class of functional materials, compounds with switchable physical properties via optical, electrical, magnetic, or mechanical manipulation are technologically important, because they can be used in a wide range of applications, including switches and memory devices [1,2,3,4,5]. A few novel crown-ether-based clathrates have been synthesized recently, there is still much room for structural tailoring, because (i) the switching behaviors of most of the reported. 2)(18-crown-6)][PF6] (1) based by tetrahedral anion, which shows dielectric and NLO switching effects simultaneously [22]. This1).differs from most the crown ether inclusion complexescomplexes reported, room temperature This differs fromof most of the crown ether inclusion interesting to find (Scheme that 1 shows a high second harmonic generation (SHG). (HTP), totally different that shows a high second harmonic generation state in the low temperature phase (LTP). The high temperature phase (HTP), totally different from(HTP), that observed for the phase and a low state in the high temperature phase totally different the synthesis, structural phase transitions, dielectric, and NLO switching effects of 1.

Thermal
8.32. These features
Variable-Temperature Structures of 1
Dielectric
SHG Properties of 1
The Flexible Thin Films of 1
Experiment
Single-Crystal X-ray Crystallography
General Measurements
Conclusions
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