Organic solar cells demonstrate external quantum efficiencies and fill factors approaching those of conventional photovoltaic technologies. However, as compared to the optical gap of the absorber materials, their open-circuit voltage is much lower, largely due to the presence of significant nonradiative recombination. In this work, we study a large data set of published and new material combinations and find that non-radiative voltage losses decrease with increasing charge-transfer state energies. This observation is explained by considering non-radiative charge-transfer state decay as electron transfer in the Marcus inverted regime, being facilitated by a common skeletal molecular vibrational mode. Our results suggest an intrinsic link between non-radiative voltage losses and electron-vibration coupling, indicating that these losses are unavoidable. Accordingly, the theoretical upper limit for the power conversion efficiency of single junction organic solar cells would be reduced to about 25.5% and the optimal optical gap increases to (1.45-1.65) eV, i.e. (0.2-0.3) eV higher than for technologies with minimized non-radiative voltage losses. Manuscript: "Intrinsic Non-Radiative Voltage Losses in Fullerene-Based OSCs" J. Benduhn et al.
Color‐tunable photoluminescence from continuous graphitic carbon nitride (g‐C3N4) thin films is demonstrated. The films are employed in light‐emitting diodes. A strong redshift of the electroluminescence with respect to photoluminescence is observed and a model for this uncommon behavior is provided.
In disordered organic semiconductors, the transfer of a rather localized charge carrier from one site to another triggers a deformation of the molecular structure quantified by the intramolecular relaxation energy. A similar structural relaxation occurs upon population of intermolecular charge-transfer (CT) states formed at organic electron donor (D)-acceptor (A) interfaces. Weak CT absorption bands for D-A complexes occur at photon energies below the optical gaps of both the donors and the C acceptor as a result of optical transitions from the neutral ground state to the ionic CT state. In this work, we show that temperature-activated intramolecular vibrations of the ground state play a major role in determining the line shape of such CT absorption bands. This allows us to extract values for the relaxation energy related to the geometry change from neutral to ionic CT complexes. Experimental values for the relaxation energies of 20 D:C CT complexes correlate with values calculated within density functional theory. These results provide an experimental method for determining the polaron relaxation energy in solid-state organic D-A blends and show the importance of a reduced relaxation energy, which we introduce to characterize thermally activated CT processes.
Electrical transport properties of poly (3-hexylthiophene) (P3HT) (6,6)-phenyl C61-butyric acid methyl ester (PCBM) solar cells, with and without encapsulation, have been investigated and analyzed using admittance spectroscopy and capacitance voltage measurements at different temperatures. The admittance spectroscopy clearly reveals two defect states with activation energies of 53 and 100 meV, and a concentration ten times higher in the unencapsulated sample. These defects seem to have a strong effect on the charge transport and the solar cell performance when they are present with a high concentration, since they lead to a decrease of the mobility and also the short-circuit current and the efficiency. The origin of these defects has been assigned to reaction of the blend with O2 which is also known to induce p-type doping in pure P3HT. In an attempt to understand the effect of these defects on the organic solar cell performance, modeling and simulation were carried out using the effective medium layer model and gave good agreement with the measurements results.
High photon energy losses limit the open‐circuit voltage (VOC) and power conversion efficiency of organic solar cells (OSCs). In this work, an optimization route is presented which increases the VOC by reducing the interfacial area between donor (D) and acceptor (A). This optimization route concerns a cascade device architecture in which the introduction of discontinuous interlayers between alpha‐sexithiophene (α‐6T) (D) and chloroboron subnaphthalocyanine (SubNc) (A) increases the VOC of an α‐6T/SubNc/SubPc fullerene‐free cascade OSC from 0.98 V to 1.16 V. This increase of 0.18 V is attributed solely to the suppression of nonradiative recombination at the D–A interface. By accurately measuring the optical gap (Eopt) and the energy of the charge‐transfer state (ECT) of the studied OSC, a detailed analysis of the overall voltage losses is performed. Eopt – qVOC losses of 0.58 eV, which are among the lowest observed for OSCs, are obtained. Most importantly, for the VOC‐optimized devices, the low‐energy (700 nm) external quantum efficiency (EQE) peak remains high at 79%, despite a minimal driving force for charge separation of less than 10 meV. This work shows that low‐voltage losses can be combined with a high EQE in organic photovoltaic devices.
The influence of fullerene side chain functionalization on both the morphology and electro-optical properties of bulk-heterojunction polymer:fullerene solar cells is discussed through a systematic investigation of material blends consisting of the conjugated polymer poly[2-methoxy-5-(3′,7′-dimethyloctyloxy)-1,4-phenylene vinylene] (MDMO-PPV) as donor and fullerene molecules with different side chains as the acceptor. The varying side chain of the fullerenes was found to induce morphological changes as confirmed by different analytical techniques such as Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD), and Nuclear Magnetic Resonance (NMR). The fullerene with the shorter side chain, [6,6]-phenyl-C61-butyric acid methyl ester (PCBM), forms crystalline nanophases in the blend, while this is not the case for the alternative diphenylmethanofullerene acceptor, [6,6]-1,1-bis(4,4′-dodecyloxyphenyl)methanofullerene (DPM-12). The introduction of NMR allows us to estimate the fraction of crystalline fullerene. The morphological changes have a profound effect on the characteristics of charge transfer states (CT) formed at the polymer:fullerene interfaces. Crystallization of fullerene molecules shifts the energy of the CT state. This shift in energy is directly manifested in the open-circuit voltage of solar cells based on the fullerene acceptors under investigation.
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