Theoretical framework identifies key properties enhancing NLO activity in chiral crystals, suggesting new design strategies.
A simple theoretical framework is presented to identify the key molecular properties and macromolecular arrangements leading to high second-order nonlinear optical (NLO) activity of chiral crystals. In chiral materials, maximum second harmonic generation (SHG) efficiency is predicted for an antiparallel molecular arrangement of Λ-like chromophores. This prediction is in stark contrast to the majority of previous crystal engineering efforts for second-order NLO materials, which have been focused almost exclusively on the construction of crystals exhibiting high degrees of polar order. Methods for possible rational electrostatic control of crystal structure by appropriate molecular design are considered.
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Wampler et al. (2008) studied this question.
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