4.3 Article

Design Strategy of Highly Efficient Nonlinear Optical Orange-Colored Crystals with Two Electron-Withdrawing Groups

Journal

ADVANCED PHOTONICS RESEARCH
Volume 3, Issue 7, Pages -

Publisher

WILEY
DOI: 10.1002/adpr.202100350

Keywords

chromophores; nonlinear optics; photonic materials

Funding

  1. National Research Foundation of Korea (NRF) - Ministry of Science, ICT & Future Planning, Korea [2021R1A2C1005012, 2021R1A5A6002853, 2019K1A3A1A14057973]
  2. Swiss National Science Foundation (SNSF), Switzerland [IZKSZ2_188194]
  3. National Research Foundation of Korea [2021R1A2C1005012] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
  4. Swiss National Science Foundation (SNF) [IZKSZ2_188194] Funding Source: Swiss National Science Foundation (SNF)

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A new class of highly efficient nonlinear optical organic salt crystals, based on two electron-withdrawing groups (EWGs), has been reported. The crystals exhibit enhanced microscopic and macroscopic optical nonlinearity, making them promising materials for various nonlinear optical applications.
A new class of highly efficient nonlinear optical organic salt crystals is reported. In nonlinear optics based on organic materials, it is well known that using two electron-withdrawing groups (EWGs) onto cationic electron acceptors instead of conventional one EWG remarkably enhances microscopic optical nonlinearity for chromophores. However, the corresponding organic crystals possessing enhanced large macroscopic optical nonlinearity have not been reported yet. Herein, a design strategy is proposed for obtaining highly efficient nonlinear optical crystals based on two EWGs in cationic electron acceptors. Introducing a phenolic electron donor, promoting a head-to-tail interionic assembly, along with a two-EWG N-pyrimidinyl pyridinium electron acceptor in cationic chromophores results in a preferred non-centrosymmetric, perfectly parallel alignment of chromophores in crystal. Newly designed OPR (4-(4-hydroxystyryl)-1-(pyrimidin2-yl)pyridinium) crystals exhibit approximately two times larger effective first hyperpolarizability than that of analogous N-alkyl OHP (4-(4-hydroxystyryl)-1methylpyridinium) crystals based on only one EWG. OPR crystals exhibit comparable second-order optical nonlinearity to benchmark red-colored DAST (4-(4-(dimethylamino)styryl)-1-methylpyridinium 4-methylbenzenesulfonate) crystals, but a significant blue-shifted absorption resulting in orange-color crystals. Therefore, phenolic organic salt crystals using two EWGs are highly promising materials for various nonlinear optical applications.

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