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Issue 15, 2018
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Switchable behaviors of quadratic nonlinear optical properties originating from bi-step phase transitions in a molecule-based crystal

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Abstract

Solid-state nonlinear optical (NLO) switches are recently emerging as a new class of promising stimuli-responsive materials for photoelectric application. Herein, we report an organic molecular crystal, N- methylcyclohexylamine picrate (1), which exhibits remarkable switching behaviors of quadratic NLO properties with a large contrast of ∼20 between its NLO-on and NLO-off states. This is almost comparable with the conventional photochromic counterparts, and suggests the great potential of 1 as a quadratic NLO-switching candidate. It is noteworthy that 1 undergoes bi-step structural phase transitions at T1 = 240 K and T2 = 285 K, which are closely associated with its NLO-switching activities. Above T1, disordering of anionic and cationic moieties leads to vanishing of the NLO effect, (i.e. NLO-off state). In contrast, below T1, stepwise frozen ordering of the structural moieties generates strong NLO activities, with the NLO response being ∼0.9 times that of KH2PO4. Such an order–disorder transformation accounts for the high-contrast NLO switching of 1. It is believed that this finding affords an effective strategy for designing new stimuli-responsive materials.

Graphical abstract: Switchable behaviors of quadratic nonlinear optical properties originating from bi-step phase transitions in a molecule-based crystal

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Publication details

The article was received on 25 Jan 2018, accepted on 07 Mar 2018 and first published on 09 Mar 2018


Article type: Paper
DOI: 10.1039/C8TC00407B
Citation: J. Mater. Chem. C, 2018,6, 4150-4155
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    Switchable behaviors of quadratic nonlinear optical properties originating from bi-step phase transitions in a molecule-based crystal

    K. Tao, Z. Wu, S. Han, J. Zhang, C. Ji, Y. Wang, W. Zhang, J. Luo and Z. Sun, J. Mater. Chem. C, 2018, 6, 4150
    DOI: 10.1039/C8TC00407B

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