Stefanie Herbst

Aqueous Solution Processed Photoconductive Cathode Interlayer for High Performance Polymer Solar Cells with Thick Interlayer and Thick Active Layer

An aqueous-solution-processed photoconductive cathode interlayer is developed, in which the photoinduced charge transfer brings multiple advantages such as increased conductivity and electron mobility, as well as reduced work function. Average power conversion efficiency over 10% is achieved even when the thickness of the cathode interlayer and active layer is up to 100 and 300 nm, respectively.

A Columnar Liquid-Crystal Phase Formed by Hydrogen-Bonded Perylene Bisimide J-Aggregates

A new perylene bisimide (PBI) dye self-assembles through hydrogen bonds and π-π interactions into J-aggregates that in turn self-organize into liquid-crystalline (LC) columnar hexagonal domains. The PBI cores are organized with the transition dipole moments parallel to the columnar axis, which is an unprecedented structural organization in π-conjugated columnar liquid crystals. Middle and wide-angle X-ray analyses reveal a helical structure consisting of three self-assembled hydrogen-bonded PBI strands that constitute a single column of the columnar hexagonal phase. This remarkable assembly mode for columnar liquid crystals may afford new anisotropic LC materials for applications in photonics.

Influence of optical material properties on strong coupling in organic semiconductor based microcavities

The optical properties of organic semiconductors are generally characterised by a number of material specific parameters, including absorbance, photoluminescence quantum yield, Stokes shift, and molecular orientation. Here, we study four different organic semiconductors and compare their optical properties to the characteristics of the exciton-polaritons that are formed when these materials are introduced into metal-clad microcavities. We find that the strength of coupling between cavity photons and excitons is clearly correlated with the absorptivity of the material. In addition, we show that anisotropy strongly affects the characteristics of the formed exciton-polaritons.

Self-assembly of multi-stranded perylene dye J-aggregates in columnar liquid-crystalline phases

Many discoid dyes self-assemble into columnar liquid-crystalline (LC) phases with packing arrangements that are undesired for photonic applications due to H-type exciton coupling. Here, we report a series of crystalline and LC perylene bisimides (PBIs) self-assembling into single or multi-stranded (two, three, and four strands) aggregates with predominant J-type exciton coupling. These differences in the supramolecular packing and optical properties are achieved by molecular design variations of tetra-bay phenoxy-dendronized PBIs with two N–H groups at the imide positions. The self-assembly is driven by hydrogen bonding, slipped π–π stacking, nanosegregation, and steric requirements of the peripheral building blocks. We could determine the impact of the packing motifs on the spectroscopic properties and demonstrate different J- and H-type coupling contributions between the chromophores. Our findings on structure–property relationships and strong J-couplings in bulk LC materials open a new avenue in the molecular engineering of PBI J-aggregates with prospective applications in photonics.Perylene bisimides (PBI) exhibit interesting photophysical and self-assembly properties but detailed understanding of the correlation between packing motif and spectroscopic properties is lacking. Here the authors report on self-assembling of PBIs in liquid crystalline phases to give aggregates with J- and H-type coupling contribution between the chromophores.

Direct observation of exciton–exciton interactions

Natural light harvesting as well as optoelectronic and photovoltaic devices depend on efficient transport of energy following photoexcitation. Using common spectroscopic methods, however, it is challenging to discriminate one-exciton dynamics from multi-exciton interactions that arise when more than one excitation is present in the system. Here we introduce a coherent two-dimensional spectroscopic method that provides a signal only in case that the presence of one exciton influences the behavior of another one. Exemplarily, we monitor exciton diffusion by annihilation in a perylene bisimide-based J-aggregate. We determine quantitatively the exciton diffusion constant from exciton–exciton-interaction 2D spectra and reconstruct the annihilation-free dynamics for large pump powers. The latter enables for ultrafast spectroscopy at much higher intensities than conventionally possible and thus improves signal-to-noise ratios for multichromophore systems; the former recovers spatio–temporal dynamics for a broad range of phenomena in which exciton interactions are present.Some photo-physical processes in multichromophore systems might get triggered only if two excitations are present. Here, the authors introduce exciton–exciton-interaction 2D spectroscopy, which is a non-linear optical method that can selectively track the time evolution of such effects.

Three-dimensional photonic confinement in imprinted liquid crystalline pillar microcavities

We demonstrate the feasibility of a thermal imprint technology capable of structuring organic thin films with liquid crystalline properties forming feature sizes on a several micrometer scale. The imprint technique can directly be applied onto a variety of substrates including dielectric mirrors. The so fabricated three-dimensional microcavities have lateral extensions up to 20 μm and heights between 1 and 5 μm. Exemplarily, pillar microcavities were produced wherein three-dimensional photonic confinement is observed by the formation of 0D cavity mode patterns. The imprint technique further favors the formation of hemispherical pillar geometries rather than cylindrical pillars, resulting in equidistant mode spacings of transversal cavity modes.