Exemplary thin-film optical devices have first and second layer groups disposed as a layer stack on a substrate. The first layer group comprises a first PPN layer, a first LCP layer, and a first barrier layer all superposed. The second layer group is superposed relative to the first layer group, and includes a second PPN layer, a second LCP layer, and a second barrier layer all superposed. The first and second layer groups cooperate to polarize multiple wavelengths of an incident light flux in a broadband and/or wide-angle manner. Each of the layer groups has an alignment layer, a respective liquid-crystal polymer layer, and a barrier layer.