@article{BaunachChowdhuryStallforthetal.2021, author = {Baunach, Martin and Chowdhury, Somak and Stallforth, Pierre and Dittmann-Th{\"u}nemann, Elke}, title = {The landscape of recombination events that create nonribosomal peptide diversity}, series = {Molecular biology and evolution : MBE}, volume = {38}, journal = {Molecular biology and evolution : MBE}, number = {5}, publisher = {Oxford Univ. Press}, address = {Oxford}, issn = {0737-4038}, doi = {10.1093/molbev/msab015}, pages = {2116 -- 2130}, year = {2021}, abstract = {Nonribosomal peptides (NRP) are crucial molecular mediators in microbial ecology and provide indispensable drugs. Nevertheless, the evolution of the flexible biosynthetic machineries that correlates with the stunning structural diversity of NRPs is poorly understood. Here, we show that recombination is a key driver in the evolution of bacterial NRP synthetase (NRPS) genes across distant bacterial phyla, which has guided structural diversification in a plethora of NRP families by extensive mixing andmatching of biosynthesis genes. The systematic dissection of a large number of individual recombination events did not only unveil a striking plurality in the nature and origin of the exchange units but allowed the deduction of overarching principles that enable the efficient exchange of adenylation (A) domain substrates while keeping the functionality of the dynamic multienzyme complexes. In the majority of cases, recombination events have targeted variable portions of the A(core) domains, yet domain interfaces and the flexible A(sub) domain remained untapped. Our results strongly contradict the widespread assumption that adenylation and condensation (C) domains coevolve and significantly challenge the attributed role of C domains as stringent selectivity filter during NRP synthesis. Moreover, they teach valuable lessons on the choice of natural exchange units in the evolution of NRPS diversity, which may guide future engineering approaches.}, language = {en} } @article{GaoWangBlakesleyetal.2012, author = {Gao, Feng and Wang, Jianpu and Blakesley, James C. and Hwang, Inchan and Li, Zhe and Greenham, Neil C.}, title = {Quantifying loss mechanisms in polymer Fullerene photovoltaic devices}, series = {dvanced energy materials}, volume = {2}, journal = {dvanced energy materials}, number = {8}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.201200073}, pages = {956 -- 961}, year = {2012}, language = {en} } @article{KegelmannTockhornWolffetal.2019, author = {Kegelmann, Lukas and Tockhorn, Philipp and Wolff, Christian Michael and M{\´a}rquez, Jos{\´e} A. and Caicedo D{\´a}vila, Sebasti{\´a}n and Korte, Lars and Unold, Thomas and Loevenich, Wilfried and Neher, Dieter and Rech, Bernd and Albrecht, Steve}, title = {Mixtures of Dopant-Free Spiro-OMeTAD and Water-Free PEDOT as a Passivating Hole Contact in Perovskite Solar Cells}, series = {ACS applied materials \& interfaces}, volume = {11}, journal = {ACS applied materials \& interfaces}, number = {9}, publisher = {American Chemical Society}, address = {Washington}, issn = {1944-8244}, doi = {10.1021/acsami.9b01332}, pages = {9172 -- 9181}, year = {2019}, abstract = {Doped spiro-OMeTAD at present is the most commonly used hole transport material (HTM) in n-i-p-type perovskite solar cells, enabling high efficiencies around 22\%. However, the required dopants were shown to induce nonradiative recombination of charge carriers and foster degradation of the solar cell. Here, in a novel approach, highly conductive and inexpensive water-free poly(3,4-ethylenedioxythiophene) (PEDOT) is used to replace these dopants. The resulting spiro-OMeTAD/PEDOT (SpiDOT) mixed films achieve higher lateral conductivities than layers of doped spiro-OMeTAD. Furthermore, combined transient and steady-state photoluminescence studies reveal a passivating effect of PEDOT, suppressing nonradiative recombination losses at the perovskite/HTM interface. This enables excellent quasi-Fermi level splitting values of up to 1.24 eV in perovskite/SpiDOT layer stacks and high open-circuit voltages (V-OC) up to 1.19 V in complete solar cells. Increasing the amount of dopant-free spiro-OMeTAD in SpiDOT layers is shown to enhance hole extraction and thereby improves the fill factor in solar cells. As a consequence, stabilized efficiencies up to 18.7\% are realized, exceeding cells with doped spiro-OMeTAD as a HTM in this study. Moreover, to the best of our knowledge, these results mark the lowest nonradiative recombination loss in the V-OC (140 mV with respect to the Shockley-Queisser limit) and highest efficiency reported so far for perovskite solar cells using PEDOT as a HTM.}, language = {en} } @article{KrueckemeierRauStolterfohtetal.2019, author = {Kr{\"u}ckemeier, Lisa and Rau, Uwe and Stolterfoht, Martin and Kirchartz, Thomas}, title = {How to report record open-circuit voltages in lead-halide perovskite solar cells}, series = {Advanced energy materials}, volume = {10}, journal = {Advanced energy materials}, number = {1}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.201902573}, pages = {11}, year = {2019}, abstract = {Open-circuit voltages of lead-halide perovskite solar cells are improving rapidly and are approaching the thermodynamic limit. Since many different perovskite compositions with different bandgap energies are actively being investigated, it is not straightforward to compare the open-circuit voltages between these devices as long as a consistent method of referencing is missing. For the purpose of comparing open-circuit voltages and identifying outstanding values, it is imperative to use a unique, generally accepted way of calculating the thermodynamic limit, which is currently not the case. Here a meta-analysis of methods to determine the bandgap and a radiative limit for open-circuit voltage is presented. The differences between the methods are analyzed and an easily applicable approach based on the solar cell quantum efficiency as a general reference is proposed.}, language = {en} } @article{RanLoveHeiberetal.2018, author = {Ran, Niva A. and Love, John A. and Heiber, Michael C. and Jiao, Xuechen and Hughes, Michael P. and Karki, Akchheta and Wang, Ming and Brus, Viktor V. and Wang, Hengbin and Neher, Dieter and Ade, Harald and Bazan, Guillermo C. and Thuc-Quyen Nguyen,}, title = {Charge generation and recombination in an organic solar cell with low energetic offsets}, series = {dvanced energy materials}, volume = {8}, journal = {dvanced energy materials}, number = {5}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.201701073}, pages = {12}, year = {2018}, abstract = {Organic bulk heterojunction (BHJ) solar cells require energetic offsets between the donor and acceptor to obtain high short-circuit currents (J(SC)) and fill factors (FF). However, it is necessary to reduce the energetic offsets to achieve high open-circuit voltages (V-OC). Recently, reports have highlighted BHJ blends that are pushing at the accepted limits of energetic offsets necessary for high efficiency. Unfortunately, most of these BHJs have modest FF values. How the energetic offset impacts the solar cell characteristics thus remains poorly understood. Here, a comprehensive characterization of the losses in a polymer:fullerene BHJ blend, PIPCP:phenyl-C61-butyric acid methyl ester (PC61BM), that achieves a high V-OC (0.9 V) with very low energy losses (E-loss = 0.52 eV) from the energy of absorbed photons, a respectable J(SC) (13 mA cm(-2)), but a limited FF (54\%) is reported. Despite the low energetic offset, the system does not suffer from field-dependent generation and instead it is characterized by very fast nongeminate recombination and the presence of shallow traps. The charge-carrier losses are attributed to suboptimal morphology due to high miscibility between PIPCP and PC61BM. These results hold promise that given the appropriate morphology, the J(SC), V-OC, and FF can all be improved, even with very low energetic offsets.}, language = {en} }