We show by a combination of spectrally resolved fluorescence and atomic force microscopy that individual, single crystalline, needlelike aggregates of hexaphenyl molecules with submicron cross-sectional dimensions act as optical waveguides (“nanofibers”) in the blue spectral range. The nanofibers are formed via laser-supported, dipole-assisted self-assembly on single crystalline mica substrates. This method allows us to modify the morphology of individual aggregates as well as their mutual distances and the overall orientation of needle arrays. An analytical theory describes quantitatively the waveguiding behavior. From measurements of the damping of propagating 425-nm light the imaginary part of the dielectric function of individual nanoscaled organic aggregates is determined.

We report on dipole-assisted, self-assembled formation of p-6P and p-5P needles on cleaved and heated mica (0001) surfaces. Low-energy electron diffraction (LEED) reveals that the needles are single crystalline with the (11̄1̄) face parallel to the surface, consisting of parallel stacks of laying molecules oriented along the direction of microscopic dipoles on the mica surface. They have submicrometer cross-sectional dimensions and lengths as large as millimeters. Moreover, due to the strong dipole confinement of individual molecules, the needles form large domains with parallel oriented entities. A pronounced optical dichroism agrees with the findings from LEED.

Molecular chirality and the inherently connected differential absorption of circular polarized light (CD) combined with semiconducting properties offers great potential for chiral opto-electronics. Here we discuss the temperature-controlled assembly of enantiopure prolinol functionalized squaraines with opposite handedness into intrinsically circular dichroic, molecular J-aggregates in spincasted thin films. By Mueller matrix spectroscopy we accurately probe an extraordinary high excitonic circular dichroism, which is not amplified by mesoscopic ordering effects. At maximum, CD values of 1000 mdeg/nm are reached and, after accounting for reflection losses related to the thin film nature, we obtain a film thickness independent dissymmetry factorg = 0.75. The large oscillator strength of the corresponding absorption within the deep-red spectral range translates into a negative real part of the dielectric function in the spectral vicinity of the exciton resonance. Thereby, we provide a new small molecular benchmark material for the development of organic thin film based chiroptics.

We study gain and lasing processes in individual self-assembled organic nanofibers grown on mica substrates. The gain-induced response of the nanofibers is found to depend sensitively on the fiber structure. In homogeneous fibers where no coherent optical feedback is present, high net optical gain (of up to ${10}^3{\mathrm{cm}}^{-1}$ ) results in spectral narrowing at the material gain peaks. In the case of strong optical feedback, which occurs in long nanofibers with randomly distributed scattering centers, gain is in turn responsible for low-threshold coherent random laser action.

Laser-supported, dipole-assisted self-assembly results in blue-light guiding nanostructures, namely single-crystalline nanofibers of hexaphenyl molecules. The nanofibers are up to 1 mm long, extremely well-aligned to each other and their cross sections can be tuned to span the range from nonguiding to guiding single optical modes at λ=425.5 nm. An analytical theory for such organic waveguides can reproduce quantitatively the experimentally observed behavior. From the measured damping of propagating, vibrationally dressed excitons the imaginary part of the dielectric function of isolated nanoscaled organic aggregates is determined.