AbstractSurface active diacetylene monolayers were polymerized at the gas–water interface and bilayers formed from these layers were deposited onto lock‐and‐key devices. Samples exhibited intial conductivities on the order of 10−7Ω−1cm−1, which decayed at varying rates depending on sample composition to 10−11Ω−1cm−1. This initial space charge current was found to be strongly dependent on the presence of small amounts of water. A current increase was observed of over three orders of magnitude in some samples upon doping with iodine. Current flow decreased, however, back to original values after removal of the iodine. Polydiacetylene bilayers were also found to exhibit photo conductive current increases of over an
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