A procedure is disclosed for assembly of novel two-sided monolayer or multilayer device architectures out of self-assembly or self-organizing amphiphilic compounds derived from molecules that undergo a type of valence tautomerization known as asymmetric narcissistic reactions. The two-sided monolayer architectures are constructed by Langmuir-Blodgett (LB) transfer or self-assembly (SA) techniques while the multilayer architectures are formed by Y-type LB depositions, where the two layers or bilayers of the assemblies are alternate depositions of mirror-image forms of the amphiphiles. The resulting three-dimensional supramolecular assemblies described herein are uniquely capable of commutation between two non-centrosymmetric states which have, on a macroscopic scale, an optically antipodal relationship and a third central symmetric state which is, accordingly, optically racemic. The inventive architectures are expected to be useful for constructing a variety of opto-electronic devices for application as chemical sensors or for the transmission, modulation, storage, or processing of information.