TY  - JOUR
A1  - Vandewal, Koen
A1  - Benduhn, Johannes
A1  - Schellhammer, Karl Sebastian
A1  - Vangerven, Tim
A1  - Rückert, Janna E.
A1  - Piersimoni, Fortunato
A1  - Scholz, Reinhard
A1  - Zeika, Olaf
A1  - Fan, Yeli
A1  - Barlow, Stephen
A1  - Neher, Dieter
A1  - Marder, Seth R.
A1  - Manca, Jean
A1  - Spoltore, Donato
A1  - Cuniberti, Gianaurelio
A1  - Ortmann, Frank
T1  - Absorption Tails of Donor
BT  - C-60 Blends Provide Insight into Thermally Activated Charge-Transfer Processes and Polaron Relaxation
JF  - Journal of the American Chemical Society
N2  - 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.
Y1  - 2017
U6  - https://doi.org/10.1021/jacs.6b12857
SN  - 0002-7863
VL  - 139
IS  - 4
SP  - 1699
EP  - 1704
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Benduhn, Johannes
A1  - Tvingstedt, Kristofer
A1  - Piersimoni, Fortunato
A1  - Ullbrich, Sascha
A1  - Fan, Yeli
A1  - Tropiano, Manuel
A1  - McGarry, Kathryn A.
A1  - Zeika, Olaf
A1  - Riede, Moritz K.
A1  - Douglas, Christopher J.
A1  - Barlow, Stephen
A1  - Marder, Seth R.
A1  - Neher, Dieter
A1  - Spoltore, Donato
A1  - Vandewal, Koen
T1  - Intrinsic non-radiative voltage losses in fullerene-based organic solar cells
JF  - Nature Energy
N2  - 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.
Y1  - 2017
U6  - https://doi.org/10.1038/nenergy.2017.53
SN  - 2058-7546
VL  - 2
PB  - Nature Publ. Group
CY  - London
ER  -