In the past decade, the field of optics has been stimulated by new concepts such as plasmonics and extraordinary optical transmission, which are paving the way for next-generation photonic components. In this context, hybrid materials that combine the properties of structured metals with semiconductor or molecular materials to create novel functionalities offer much potential. While studying molecule– metal interactions, we have found a new phenomenon whereby molecules can induce transparency in optically thick metal films perforated with subwavelength holes. Nonintuitively, transparent windows are opened up at wavelengths at which the molecules absorb strongly, that is, where one would normally expect no transmission. Here we report a detailed study of this phenomenon showing, among other things, that the molecular material must be within the dipole coupling distance (less than ca. 20 nm) from the metal surface, and that the mechanism involves surface plasmons but is independent of the arrangement of the holes. The phenomenon thus provides new flexibility for tailoring extraordinary optical transmission through subwavelength holes and points to new directions for preparing plasmonic hybrid materials for photonics and energy-conversion applications. Absorption-induced transparency (AIT) is best illustrated by the schematic and spectra in Figure 1. Figure 1a shows the transmission spectrum of a square array of 100 nm-diameter holes milled by focused ion beam (FIB) in a 200 nm-thick Ag film with a period of 250 nm (black curve). Only the transmission peak associated with the (1,0) surface plasmon (SP) resonance on the glass/metal interface of the hole array is visible at 518 nm. When an approximately 30 nm layer of a J-aggregate of a cyanine compound (2,2’-dimethyl-8-phenyl5,6,5’,6’-dibenzothiacarbocyanine chloride) is adsorbed on the hole array, its transmission spectrum shows an intense new transmission with a sharp onset at 685 nm (red curve). Figure 1b shows the absorption spectrum of the cyanine Jaggregate layer (measured as 1 reflection) taken on a
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