@article{NikolisBenduhnHolzmuelleretal.2017, author = {Nikolis, Vasileios C. and Benduhn, Johannes and Holzmueller, Felix and Piersimoni, Fortunato and Lau, Matthias and Zeika, Olaf and Neher, Dieter and Koerner, Christian and Spoltore, Donato and Vandewal, Koen}, title = {Reducing Voltage Losses in Cascade Organic Solar Cells while Maintaining High External Quantum Efficiencies}, series = {dvanced energy materials}, volume = {7}, journal = {dvanced energy materials}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.201700855}, pages = {122 -- 136}, year = {2017}, abstract = {High photon energy losses limit the open-circuit voltage (V-OC) and power conversion efficiency of organic solar cells (OSCs). In this work, an optimization route is presented which increases the V-OC 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 (alpha-6T) (D) and chloroboron subnaphthalocyanine (SubNc) (A) increases the V-OC of an alpha-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 (E-opt) and the energy of the charge-transfer state (E-CT) of the studied OSC, a detailed analysis of the overall voltage losses is performed. E-opt - qV(OC) losses of 0.58 eV, which are among the lowest observed for OSCs, are obtained. Most importantly, for the V-OC-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.}, language = {en} } @article{BenduhnTvingstedtPiersimonietal.2017, author = {Benduhn, Johannes and Tvingstedt, Kristofer and Piersimoni, Fortunato and Ullbrich, Sascha and Fan, Yeli and Tropiano, Manuel and McGarry, Kathryn A. and Zeika, Olaf and Riede, Moritz K. and Douglas, Christopher J. and Barlow, Stephen and Marder, Seth R. and Neher, Dieter and Spoltore, Donato and Vandewal, Koen}, title = {Intrinsic non-radiative voltage losses in fullerene-based organic solar cells}, series = {Nature Energy}, volume = {2}, journal = {Nature Energy}, publisher = {Nature Publ. Group}, address = {London}, issn = {2058-7546}, doi = {10.1038/nenergy.2017.53}, pages = {6}, year = {2017}, abstract = {Organic solar cells demonstrate external quantum efficiencies and fill factors approaching those of conventional photovoltaic technologies. However, as compared with the optical gap of the absorber materials, their open-circuit voltage is much lower, largely due to the presence of significant non-radiative recombination. Here, 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, that is, (0.2-0.3) eV higher than for technologies with minimized non-radiative voltage losses.}, language = {en} } @article{FangHolzmuellerMatulaitisetal.2016, author = {Fang, Lijia and Holzmueller, Felix and Matulaitis, Tomas and Baasner, Anne and Hauenstein, Christoph and Benduhn, Johannes and Schwarze, Martin and Petrich, Annett and Piersimoni, Fortunato and Scholz, Reinhard and Zeika, Olaf and Koerner, Christian and Neher, Dieter and Vandewal, Koen and Leo, Karl}, title = {Fluorine-containing low-energy-gap organic dyes with low voltage losses for organic solar cells}, series = {Synthetic metals : the journal of electronic polymers and electronic molecular materials}, volume = {222}, journal = {Synthetic metals : the journal of electronic polymers and electronic molecular materials}, publisher = {Elsevier}, address = {Lausanne}, issn = {0379-6779}, doi = {10.1016/j.synthmet.2016.10.025}, pages = {232 -- 239}, year = {2016}, abstract = {Fluorine-containing donor molecules TFTF, CNTF and PRTF are designed and isomer selectively synthesized for application in vacuum-deposited organic solar cells. These molecules comprise a donor acceptor molecular architecture incorporating thiophene and benzothiadiazole derivatives as the electron-donating and electron-withdrawing moieties, respectively. As opposed to previously reported materials from this class, PRTF can be purified by vacuum sublimation at moderate to high yields because of its higher volatility and better stabilization due to a stronger intramolecular hydrogen bond, as compared to TFTF and CNTF. The UV-vis absorption spectra of the three donors show an intense broadband absorption between 500 nm and 800 nm with, similar positions of their frontier energy levels. The photophysical properties of the three donor molecules are thoroughly tested and optimized in bulk heterojunction solar cells with C-60 as acceptor. PRTF shows the best performance, yielding power conversion efficiencies of up to 3.8\%. Moreover, the voltage loss for the PRTF device due to the non radiative recombination of free charge carriers is exceptionally low (0.26 V) as compared to typical values for organic solar cells (>0.34V). (C) 2016 Published by Elsevier B.V.}, language = {en} } @article{LiBenduhnQiaoetal.2019, author = {Li, Tian-yi and Benduhn, Johannes and Qiao, Zhi and Liu, Yuan and Li, Yue and Shivhare, Rishi and Jaiser, Frank and Wang, Pei and Ma, Jie and Zeika, Olaf and Neher, Dieter and Mannsfeld, Stefan C. B. and Ma, Zaifei and Vandewal, Koen and Leo, Karl}, title = {Effect of H- and J-Aggregation on the Photophysical and Voltage Loss of Boron Dipyrromethene Small Molecules in Vacuum-Deposited Organic Solar Cells}, series = {The journal of physical chemistry letters}, volume = {10}, journal = {The journal of physical chemistry letters}, number = {11}, publisher = {American Chemical Society}, address = {Washington}, issn = {1948-7185}, doi = {10.1021/acs.jpclett.9b01222}, pages = {2684 -- 2691}, year = {2019}, abstract = {An understanding of the factors limiting the open-circuit voltage (V-oc) and related photon energy loss mechanisms is critical to increase the power conversion efficiency (PCE) of small-molecule organic solar cells (OSCs), especially those with near-infrared (NIR) absorbers. In this work, two NIR boron dipyrromethene (BODIPY) molecules are characterized for application in planar (PHJ) and bulk (BHJ) heterojunction OSCs. When two H atoms are substituted by F atoms on the peripheral phenyl rings of the molecules, the molecular aggregation type in the thin film changes from the H-type to J-type. For PHJ devices, the nonradiative voltage loss of 0.35 V in the J-aggregated BODIPY is lower than that of 0.49 V in the H-aggregated device. In BHJ devices with a nonradiative voltage loss of 0.35 V, a PCE of 5.5\% is achieved with an external quantum efficiency (EQE) maximum of 68\% at 700 nm.}, language = {en} } @article{LiBenduhnLietal.2018, author = {Li, Tian-yi and Benduhn, Johannes and Li, Yue and Jaiser, Frank and Spoltore, Donato and Zeika, Olaf and Ma, Zaifei and Neher, Dieter and Vandewal, Koen and Leo, Karl}, title = {Boron dipyrromethene (BODIPY) with meso-perfluorinated alkyl substituents as near infrared donors in organic solar cells}, series = {Journal of materials chemistry : A, Materials for energy and sustainability}, volume = {6}, journal = {Journal of materials chemistry : A, Materials for energy and sustainability}, number = {38}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2050-7488}, doi = {10.1039/c8ta06261g}, pages = {18583 -- 18591}, year = {2018}, abstract = {Three furan-fused BODIPYs were synthesized with perfluorinated methyl, ethyl and n-propyl groups on the meso-carbon. They were obtained with high yields by reacting the furan-fused 2-carboxylpyrrole in corresponding perfluorinated acid and anhydride. With the increase in perfluorinated alkyl chain length, the molecular packing in the single crystal is influenced, showing increasing stacking distance and decreasing slope angle. All the BODIPYs were characterized as intense absorbers in near infrared region in solid state, peaking at similar to 800 nm with absorption coefficient of over 280 000 cm(-1). Facilitated by high thermal stability, the furan-fused BODIPYs were employed in vacuum-deposited organic solar cells as electron donors. All devices exhibit PCE over 6.0\% with the EQE maximum reaching 70\% at similar to 790 nm. The chemical modification of the BODIPY donors have certain influence on the active layer morphology, and the highest PCE of 6.4\% was obtained with a notably high jsc of 13.6 mA cm(-2). Sensitive EQE and electroluminance studies indicated that the energy losses generated by the formation of a charge transfer state and the radiative recombination at the donor-acceptor interface were comparable in the range of 0.14-0.19 V, while non-radiative recombination energy loss of 0.38 V was the main energy loss route resulting in the moderate V-oc of 0.76 V.}, language = {en} } @article{VandewalBenduhnSchellhammeretal.2017, author = {Vandewal, Koen and Benduhn, Johannes and Schellhammer, Karl Sebastian and Vangerven, Tim and R{\"u}ckert, Janna E. and Piersimoni, Fortunato and Scholz, Reinhard and Zeika, Olaf and Fan, Yeli and Barlow, Stephen and Neher, Dieter and Marder, Seth R. and Manca, Jean and Spoltore, Donato and Cuniberti, Gianaurelio and Ortmann, Frank}, title = {Absorption Tails of Donor}, series = {Journal of the American Chemical Society}, volume = {139}, journal = {Journal of the American Chemical Society}, number = {4}, publisher = {American Chemical Society}, address = {Washington}, issn = {0002-7863}, doi = {10.1021/jacs.6b12857}, pages = {1699 -- 1704}, year = {2017}, abstract = {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-60 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-60 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.}, language = {en} }