Sign flips, crossovers, and spatial inversions in surface plasmon resonance across a chiral-metal interface.

We consider the surface plasmon resonance established along an interface between a metal and a chiral medium (chiral case). Resulting solutions are compared with those obtained for a metal-dielectric interface (achiral case). We found that the chiral case exhibits either larger or smaller phase speeds than the achiral case due to the energy redistribution between translation and rotation. For a loss-free system, we found crossovers among the dispersion curves and spatial inversions in field profiles. These features are associated with anti-symmetric spin flips with respect to medium chirality. The short-wavelength limit leads to an upper bound on the medium chirality.

Impact of molecular quadrupole moments on the energy levels at organic heterojunctions.

The functionality of organic semiconductor devices crucially depends on molecular energies, namely the ionisation energy and the electron affinity. Ionisation energy and electron affinity values of thin films are, however, sensitive to film morphology and composition, making their prediction challenging. In a combined experimental and simulation study on zinc-phthalocyanine and its fluorinated derivatives, we show that changes in ionisation energy as a function of molecular orientation in neat films or mixing ratio in blends are proportional to the molecular quadrupole component along the π-π-stacking direction. We apply these findings to organic solar cells and demonstrate how the electrostatic interactions can be tuned to optimise the energy of the charge-transfer state at the donor-acceptor interface and the dissociation barrier for free charge carrier generation. The confirmation of the correlation between interfacial energies and quadrupole moments for other materials indicates its relevance for small molecules and polymers.

Molecular parameters responsible for thermally activated transport in doped organic semiconductors.

Doped organic semiconductors typically exhibit a thermal activation of their electrical conductivity, whose physical origin is still under scientific debate. In this study, we disclose relationships between molecular parameters and the thermal activation energy (EA) of the conductivity, revealing that charge transport is controlled by the properties of host-dopant integer charge transfer complexes (ICTCs) in efficiently doped organic semiconductors. At low doping concentrations, charge transport is limited by the Coulomb binding energy of ICTCs, which can be minimized by systematic modification of the charge distribution on the individual ions. The investigation of a wide variety of material systems reveals that static energetic disorder induced by ICTC dipole moments sets a general lower limit for EA at large doping concentrations. The impact of disorder can be reduced by adjusting the ICTC density and the intramolecular relaxation energy of host ions, allowing an increase of conductivity by many orders of magnitude.

Insight into doping efficiency of organic semiconductors from the analysis of the density of states in n-doped C60 and ZnPc.

Doping plays a crucial role in semiconductor physics, with n-doping being controlled by the ionization energy of the impurity relative to the conduction band edge. In organic semiconductors, efficient doping is dominated by various effects that are currently not well understood. Here, we simulate and experimentally measure, with direct and inverse photoemission spectroscopy, the density of states and the Fermi level position of the prototypical materials C60 and zinc phthalocyanine n-doped with highly efficient benzimidazoline radicals (2-Cyc-DMBI). We study the role of doping-induced gap states, and, in particular, of the difference Δ1 between the electron affinity of the undoped material and the ionization potential of its doped counterpart. We show that this parameter is critical for the generation of free carriers and influences the conductivity of the doped films. Tuning of Δ1 may provide alternative strategies to optimize the electronic properties of organic semiconductors.

Quantum mechanical heat transport in disordered harmonic chains.

We investigate the mechanism of heat conduction in ordered and disordered harmonic one-dimensional chains within the quantum mechanical Langevin method. In the case of disordered chains we find indications for normal heat conduction, which means that there is a finite temperature gradient, but we cannot clearly decide whether the heat resistance increases linearly with the chain length. Furthermore, we observe characteristic quantum mechanical features like the Bose-Einstein statistics of the occupation numbers of the normal modes, freezing of the heat conductivity, and influence of the entanglement within the chain on the current. For the ordered chain we recover some classical results like a vanishing temperature gradient and a heat flux independent of the length of the chain.