@misc{ZhongCausaMooreetal.2020, author = {Zhong, Yufei and Causa, Martina and Moore, Gareth John and Krauspe, Philipp and Xiao, Bo and G{\"u}nther, Florian and Kublitski, Jonas and BarOr, Eyal and Zhou, Erjun and Banerji, Natalie}, title = {Sub-picosecond charge-transfer at near-zero driving force in polymer:non-fullerene acceptor blends and bilayers}, series = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, journal = {Zweitver{\"o}ffentlichungen der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, number = {1}, issn = {1866-8372}, doi = {10.25932/publishup-51193}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-511936}, pages = {12}, year = {2020}, abstract = {Organic photovoltaics based on non-fullerene acceptors (NFAs) show record efficiency of 16 to 17\% and increased photovoltage owing to the low driving force for interfacial charge-transfer. However, the low driving force potentially slows down charge generation, leading to a tradeoff between voltage and current. Here, we disentangle the intrinsic charge-transfer rates from morphology-dependent exciton diffusion for a series of polymer:NFA systems. Moreover, we establish the influence of the interfacial energetics on the electron and hole transfer rates separately. We demonstrate that charge-transfer timescales remain at a few hundred femtoseconds even at near-zero driving force, which is consistent with the rates predicted by Marcus theory in the normal region, at moderate electronic coupling and at low re-organization energy. Thus, in the design of highly efficient devices, the energy offset at the donor:acceptor interface can be minimized without jeopardizing the charge-transfer rate and without concerns about a current-voltage tradeoff.}, language = {en} } @article{ZhongCausaMooreetal.2020, author = {Zhong, Yufei and Causa, Martina and Moore, Gareth John and Krauspe, Philipp and Xiao, Bo and G{\"u}nther, Florian and Kublitski, Jonas and BarOr, Eyal and Zhou, Erjun and Banerji, Natalie}, title = {Sub-picosecond charge-transfer at near-zero driving force in polymer:non-fullerene acceptor blends and bilayers}, series = {Nature Communications}, volume = {11}, journal = {Nature Communications}, number = {1}, publisher = {Nature Publishing Group UK}, address = {London}, issn = {2041-1723}, doi = {10.1038/s41467-020-14549-w}, pages = {1 -- 10}, year = {2020}, abstract = {Organic photovoltaics based on non-fullerene acceptors (NFAs) show record efficiency of 16 to 17\% and increased photovoltage owing to the low driving force for interfacial charge-transfer. However, the low driving force potentially slows down charge generation, leading to a tradeoff between voltage and current. Here, we disentangle the intrinsic charge-transfer rates from morphology-dependent exciton diffusion for a series of polymer:NFA systems. Moreover, we establish the influence of the interfacial energetics on the electron and hole transfer rates separately. We demonstrate that charge-transfer timescales remain at a few hundred femtoseconds even at near-zero driving force, which is consistent with the rates predicted by Marcus theory in the normal region, at moderate electronic coupling and at low re-organization energy. Thus, in the design of highly efficient devices, the energy offset at the donor:acceptor interface can be minimized without jeopardizing the charge-transfer rate and without concerns about a current-voltage tradeoff.}, language = {en} } @article{ZamponiPenfoldNachtegaaletal.2014, author = {Zamponi, Flavio and Penfold, Thomas J. and Nachtegaal, Maarten and L{\"u}bcke, Andrea and Rittmann, Jochen and Milne, Chris J. and Chergui, Majed and van Bokhoven, Jeroen A.}, title = {Probing the dynamics of plasmon-excited hexanethiol-capped gold nanoparticles by picosecond X-ray absorption spectroscopy}, series = {physical chemistry, chemical physics : PCCP}, volume = {2014}, journal = {physical chemistry, chemical physics : PCCP}, number = {16}, issn = {1463-9076}, doi = {10.1039/c4cp03301a}, pages = {23157 -- 23163}, year = {2014}, abstract = {Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8\% expansion of the Au-Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.}, language = {en} } @misc{ZamponiPenfoldNachtegaaletal.2014, author = {Zamponi, Flavio and Penfold, Thomas J. and Nachtegaal, Maarten and L{\"u}bcke, Andrea and Rittmann, Jochen and Milne, Chris J. and Chergui, Majed and van Bokhoven, Jeroen A.}, title = {Probing the dynamics of plasmon-excited hexanethiol-capped gold nanoparticles by picosecond X-ray absorption spectroscopy}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-74492}, pages = {23157 -- 23163}, year = {2014}, abstract = {Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8\% expansion of the Au-Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.}, language = {en} }