Suchergebnisse

We develop a temperature-dependent theory for singlet exciton hopping transport in disordered semiconductors. It draws on the transport level concept within a Förster transfer model and bridges the gap in describing the transition from equilibrium to nonequilibrium time-dependent spectral diffusion.We test the validity range of the developed model using kinetic Monte Carlo simulations and find agreement over a broad range of temperatures. It reproduces the scaling of the diffusion length and spectral shift with the dimensionless disorder parameter and describes in a unified manner the transition from equilibrium to nonequilibrium transport regime. We find that the diffusion length in the nonequilibrium regime does not scale with the the third power of the Förster radius. The developed theory provides a powerful tool for interpreting time-resolved and steady state spectroscopy experiments in a variety of disordered materials, including organic semiconductors and colloidal quantum dots. ; This project has received funding from the Universidad Carlos III de Madrid, the European Union's Seventh Frame- work Programme for research, technological development, and demonstration under Grant Agreement No. 600371, el Ministerio de Economía, Industria y Competitividad (COFUND2014-51509), el Ministerio de Educación, cultura y Deporte (CEI-15-17), and Banco Santander.

We demonstrate that efficient and nearly field-independent charge separation of electron hole pairs in organic planar heterojunction solar cells can be described by an incoherent hopping mechanism. Using kinetic Monte Carlo simulations that include the effect of on-chain delocalization as well as entropic contributions, we simulate the dissociation of the charge-transfer state in polymer fullerene bilayer solar cells. The model further explains experimental results of almost field independent charge separation in bilayers of molecular systems with fullerenes and provides important guidelines at the molecular level for maximizing the efficiencies of organic solar cells. Thus, utilizing coherent phenomena is not necessarily required for highly efficient charge separation in organic solar cells. ; This project has received funding from the Universidad Carlos III de Madrid, the European Union's Seventh Framework Programme for research, technological development, and demonstration under Grant Agreement No. 600371, el Ministerio de Economı́a, Industria y Competitividad (COFUND2014-51509), el Ministerio de Educación, cultura y Deporte (CEI-15-17), and Banco Santander. We also acknowledge additional funding from the German Research Foundation DFG (GRK1640) and the Bavarian University Centre for Latin America (BAYLAT).

Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S-2 -> S-1 internal conversion process, revealing an efficient unidirectional donor acceptor energy-transfer process. Detailed analysis of the excited state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S-2-S-1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition. ; This project has received funding from the Universidad Carlos III de Madrid, the European Union's Seventh Framework Programme for research, technological development and demonstration under grant agreement n° 600371, el Ministerio de Economia y Competitividad (COFUND2014-51509), el Ministerio de Educación, cultura y Deporte (CEI-15-17) and Banco Santander. This work was partially supported by CONICET, UNQ, ANPCyT (PICT-2014-2662). We also acknowledge support of the Center for Integrated Nano-technology (CINT), a U.S. Department of Energy, Office of Basic Energy Sciences user facility, as well as additional funding from the Bavarian University Centre for Latin America (BAYLAT). The work in Mons is supported by BELSPO through the PAI P6/27 Functional Supramolecular Systems project and by the Belgian National Fund for Scientific Research FNRS/F.R.S. DB is a Research Director of FNRS.

A symmetrical cyanine dye chromophore is modified with different counteranions to study the effect on crystal packing, polarizability, thermal stability, optical properties, light absorbing layer morphology, and organic photovoltaic (OPV) device parameters. Four sulfonate-based anions and the bulky bistriflylimide anion are introduced to the 2-[5-(1,3-dihydro-1,3,3-trimethyl-2H-indol-2-ylidene)-1,3-pentadien-1-yl]-1,3,3-trimethyl-3H-indolium chromophore using an Amberlyst A26 (OH− form) anion exchanger. Anionic charge distribution clearly correlates with device performance, whereby an average efficiency of 2% was reached in a standard bilayer organic solar. Evidence is given that the negative charge of the anion distributed over a large number of atoms is significantly more important than the size of the organic moieties of the sulfonate charge carrying group. This provides a clear strategy for future design of more efficient cyanine dyes for OPV applications. ; The authors thank Dr. Matthias Nagel (Empa) for suggestions and Dr. Mohammed Makha (Empa) for his help with the thermal evaporation techniques. The use of the Scanning Probe Microscopy User Laboratory at Empa is gratefully acknowledged. The authors thank the Swiss National Science Foundation for financial support under grant number 160116. This project has also received funding from the Universidad Carlos III de Madrid, the European Union's Seventh Framework Program for research, technological development and demonstration under grant agreement No. 600371, el Ministerio de Economía, Industria y Competitividad (COFUND2014-51509), el Ministerio de Educación, cultura y Deporte (CEI-15-17), and Banco Santander.

This work has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 838009 (TSFP) and No 812872 (TADFlife). D.S. acknowledges support from the Marie Skłodowska-Curie Individual Fellowship, the National Postdoctoral Program for Innovative Talents (BX201700164), the Jiangsu Planned Projects for Postdoctoral Research Funds (2018K011A). E.Z.-C. is a Royal Society Leverhulme Trust Senior Research fellow (SRF∖R1∖201089). The St Andrews team would also like to thank the Leverhulme Trust (RPG-2016047) and EPSRC (EP/P010482/1) for financial support. This work was also supported by Comunidad de Madrid (Spain) – multiannual agreement with UC3M ("Excelencia para el Profesorado Universitario" – EPUC3M14) – Fifth regional research plan 2016-2020 and by the Spanish Ministry of Science, Innovation and Universities (MICINN) through project RTI2018-101020-B-100. X.Z. would like to thank the support from the National Key Research & Development Program of China (Grant No. 2020YFA0714601, 2020YFA0714604), the National Natural Science Foundation of China (Grant No. 52130304, 51821002), Suzhou Key Laboratory of Functional Nano & Soft Materials, Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), the 111 Project, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices. ; The potential of dendrimers exhibiting thermally activated delayed fluorescence (TADF) as emitters in solution-processed organic light-emitting diodes (OLEDs) has to date not yet been realized. This in part is due to a poor understanding of the structure–property relationship in dendrimers where reports of detailed photophysical characterization and mechanism studies are lacking. In this report, using absorption and solvatochromic photoluminescence studies in solution, the origin and character of the lowest excited electronic ...

While it has been argued that field-dependent geminate pair recombination (GR) is important, this process is often disregarded when analyzing the recombination kinetics in bulk heterojunction organic solar cells (OSCs). To differentiate between the contributions of GR and nongeminate recombination (NGR) the authors study bilayer OSCs using either a PCDTBTtype polymer layer with a thickness from 14 to 66 nm or a 60 nm thick p-DTS(FBTTh2)(2) layer as donor material and C-60 as acceptor. The authors measure JV-characteristics as a function of intensity and charge-extraction-by-linearly-increasing-voltage-type hole mobilities. The experiments have been complemented by Monte Carlo simulations. The authors find that fill factor (FF) decreases with increasing donor layer thickness (L-p) even at the lowest light intensities where geminate recombination dominates. The authors interpret this in terms of thickness dependent back diffusion of holes toward their siblings at the donor-acceptor interface that are already beyond the Langevin capture sphere rather than to charge accumulation at the donor-acceptor interface. This effect is absent in the p-DTS(FBTTh2)(2) diode in which the hole mobility is by two orders of magnitude higher. At higher light intensities, NGR occurs as evidenced by the evolution of s-shape of the JV-curves and the concomitant additional decrease of the FF with increasing layer thickness. ; The authors acknowledge financial support by the Bavarian State Ministry of Science, Research, and the Arts through the Collaborative Research Network "Solar Technologies go Hybrid", by the Volkswagen foundation and by the German Science Foundation DFG through the doctoral training center "GRK 1640." This project further received funding from the Universidad Carlos III de Madrid, the European Union's Seventh Framework Programme for research, technological development and demonstration under grant agreement no. 600371, el Ministerio de Economía y Competitividad (COFUND2014-51509), el Ministerio de Educación, cultura y Deporte (CEI-15-17), and Banco Santander. M.R. additionally acknowledges support from the Hanns Seidel Foundation for a stipend through funds from the German Ministry of Education and Research (BMBF). T.-Q.N. thanks the Office of Naval Research (#N000141410076) for the support. Furthermore, the authors would like to thank the anonymous referees for helpful suggestions.