Quasi-phase-matching in chiral materials

The second-order nonlinear optical coefficients associated with chirality differ in sign for the two mirror-image forms (enantiomers) of a chiral material. Structures comprised of alternating stacks of the enantiomers can therefore be used for quasi-phase-matched frequency conversion, as we demonstrate here by second-harmonic generation from Langmuir-Blodgett films of a helicenebisquinone. Such structures could lead to new types of frequency converters in which both the second-order nonlinear response and quasi-phase-matching arise from the chirality of a material rather than its polar order.