|Title:||Multi-functional supramolecular building blocks with hydroxy piperidino groups : new opportunities for developing nonlinear optical ionic crystals|
|Authors :||Lee, Kang-Hyun|
Kim, Jun Wan
|Published in :||CrystEngComm|
|Publisher / Ed. Institution :||Royal Society of Chemistry|
|License (according to publishing contract) :||Licence according to publishing contract|
|Type of review:||Peer review (Publication)|
|Subject (DDC) :||540: Chemistry|
|Abstract:||We report on multi-functional supramolecular building blocks for obtaining a non-centrosymmetric crystal structure, which is the essential requirement for achieving a macroscopic second-order nonlinear optical activity. The supramolecular building blocks PM (piperidin-4-ylmethanol) and PO (piperidin-4-ol) consist of a piperidino group acting as a strong electron-donating group and a hydroxyl group acting as a strong hydrogen-bonding group, which also may act as a ‘site-isolation’ group. The quinolinium crystals PMQ-T and POQ-T that introduce PM and PO blocks, respectively, exhibit a non-centrosymmetric crystal structure with nonlinear optical activity, while analogous quinolinium DAQ-T crystal with the widely used N,N-dimethylamino (DA) group exhibits a centrosymmetric crystal structure without nonlinear optical activity. Compared to the DAQ-T crystal, the PMQ-T and POQ-T crystals exhibit a lower tendency to form a hydrate phase in the crystalline state. The PMQ-T crystal exhibits a higher molecular optical nonlinearity in the crystalline state than the DAQ-T crystal, which is attributed to the ‘site-isolation’ effect resulting from the bulky PM block. In addition, the PMQ-T crystal exhibits large macroscopic optical nonlinearities with more than 3 times higher off-diagonal effective hyperpolarizability than that of benchmark stilbazolium crystals. Therefore, multi-functional supramolecular building blocks PM and PO can give new opportunities for developing non-centrosymmetric ionic crystals for nonlinear optical applications.|
|Departement:||School of Engineering|
|Organisational Unit:||Institute of Computational Physics (ICP)|
|Publication type:||Article in scientific Journal|
|Appears in Collections:||Publikationen School of Engineering|
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