Abstract

Organic second-order nonlinear optical materials are of great significance in the field of integrated photonics, optical data storage and optical information processing. In this work, two iodide salts with benzo[e]indol cations as electron-withdrawing groups were designed and synthesized, which are (E)-2-(4-hydroxy-3-methoxystyryl)-1,1,3-trimethyl-1H-benzo[e]indol-3-ium iodide (1-TB) and (E)-2-(3,4-dihydroxystyryl)-1,1,3-trimethyl-1H-benzo[e]indol-3-ium iodide (2-TB). Under the irradiation of 1064 nm laser, the second harmonic generations of the 1-TB and 2-TB powders are 760 and 580 times that of urea, respectively. Among them, crystals of 1-TB are successfully grown by a slow cooling method without using seed crystals. Bulk crystal with a size of 8.0 × 3.0 × 1.0 mm3 and many submillimeter single crystals with excellent optical quality are obtained.

Highlights

  • With the development of the information age, optoelectronic technology has gradually become the main pillar of information technology in the 21st century [1,2,3,4,5,6,7,8]

  • (2-(4-hydroxy-3-methoxystyryl)-3-methylbenzo[d]thiazol-3-ium) series single crystals have the same order of magnitude of nonlinear optical susceptibilities as DAST and DSTMS [20,21,22]

  • The 1-TB and 2-TB are designed as D-π-A delocalized systems with benzo[e]indol cation as the electron-withdrawing group and pair-arranged combination to provide electrons [25]. It is well-known that a necessary requirement for the generation of second-order nonlinearity is the noncentrosymmetric arrangement of the chromophore molecules

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Summary

Introduction

With the development of the information age, optoelectronic technology has gradually become the main pillar of information technology in the 21st century [1,2,3,4,5,6,7,8]. To obtain an organic single crystal that satisfies the strong macroscopic second-order nonlinear optical characteristics of laser frequency conversion and terahertz wave generation, the preparation of a large first-order hyperpolarizabilities β of chromophore is the primary premise. The 1-TB and 2-TB are designed as D-π-A delocalized systems with benzo[e]indol cation as the electron-withdrawing group and pair-arranged (hydroxy, methoxy) combination to provide electrons [25] It is well-known that a necessary requirement for the generation of second-order nonlinearity is the noncentrosymmetric arrangement of the chromophore molecules. I hydrogen bond can reduce the energy of the whole system and keep it more stable [27,28,29] These advancements indicate that the 1-TB is an organic second-order NLO salt material with promising applications

Materials and Instruments
Synthesis of 1-TB
Synthesis of 2-TB
Environmental Stability and Solubility
Single Crystal Growth and Characterization
Macroscopic Second-Order Nonlinear Optical Properties
Conclusions
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