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Organic semiconductors have the remarkable property that their optical excitation not only generates charge-neutral electron-hole pairs (excitons) but also charge-separated polaron pairs with high yield. The microscopic mechanisms…
The separation of photogenerated polaron pairs in organic bulk heterojunction solar cells is the intermediate but crucial step between exciton dissociation and charge transport to the electrodes. In state-of-the-art devices, above 80% of…
The mechanism of electron-hole separation in organic solar cells is currently hotly debated. Recent experimental work suggests that these charges can separate on extremely short timescales (<100 fs). This can be understood in terms of…
When an excess charge carrier is added to a semiconducting polymer chain, it is well known that the carrier may self-trap into a polaronic state accompanied by a bond length adjustment pattern. A different mechanism of self-localization is…
Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials [1]. In situations where charge carriers induce a lattice distortion due to…
All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of…
We present a fully quantum-mechanical model of the electronic dynamics of primary photoexcitations in a polymeric semiconductor heterojunction, which includes both polymer stacking and phonon relaxation. By examining the phonon-induced…
We probe charge photogeneration and subsequent recombination dynamics in neat regioregular poly(3-hexylthiophene) films over six decades in time by means of time-resolved photoluminescence spectroscopy. Exciton dissociation at 10K occurs…
Charge carriers in organic semiconductors form polarons, which are self-localized states stabilized by interactions with their environment. Using a dielectric-stabilized tight-binding model parameterized from first-principles calculations,…
Charge carrier localization in extended atomic systems has been described previously as being driven by disorder, point defects or distortions of the ionic lattice. Here we show for the first time by means of first-principles computations…
Mixed-dimensional van der Waals heterojunctions comprising polymer and twodimensional (2D) semiconductors have many characteristics of an ideal charge separation interface for optoelectronic and photonic applications. However, the…
In polymer:fullerene solar cells, the origin of the losses in the field-dependent photocurrent is still controversially debated. We contribute to the ongoing discussion by performing photo-induced charge extraction measurements on…
In organic photovoltaics, the mechanism by which free electrons and holes are generated overcoming the Coulomb attraction is a currently much debated topic. To elucidate this mechanism at a molecular level, we carried out a combined…
Using long C_{N}H_{2} conjugated carbon chains with the polyynic structure as prototypical examples of one-dimensional (1D) semiconductors, we discuss self-localization of excess charge carriers into 1D large polarons in the presence of the…
Organic solar cells must separate strongly bound electron-hole pairs into free charges. This is achieved at interfaces between electron donor and acceptor organic semiconductors. The most popular electron acceptor is the fullerene…
Polarons are composite quasiparticles comprising electronic charge carriers taken together with the alterations they induce in surrounding condensed matter. Strong-coupling polarons form when electronic charge carriers become self-trapped:…
The ongoing depletion of fossil fuels has led to an intensive search for additional renewable energy sources. Solar-based technologies could provide sufficient energy to satisfy the global economic demands in the near future. Photovoltaic…
The perturbation of a semiconductor from the thermodynamic equilibrium often leads to the display of nonlinear dynamics and formation of spatiotemporal patterns due to the spontaneous generation of competing processes. Here, we describe the…
Materials containing high densities of exceptionally displaceable ions (e.g. perovskites) have extremely large ratios of their static to high-frequency dielectric constants, > 2. Large polarons form in such materials as their electronic…
We report transient electron paramagnetic resonance (trEPR) measurements with sub-microsecond time resolution performed on a P3HT:PCBM blend at low temperature. The trEPR spectrum immediately following photoexcitation reveals signatures of…