TY  - JOUR
A1  - Nikolis, Vasileios C.
A1  - Mischok, Andreas
A1  - Siegmund, Bernhard
A1  - Kublitski, Jonas
A1  - Jia, Xiangkun
A1  - Benduhn, Johannes
A1  - Hörmann, Ulrich
A1  - Neher, Dieter
A1  - Gather, Malte C.
A1  - Spoltore, Donato
A1  - Vandewal, Koen
T1  - Strong light-matter coupling for reduced photon energy losses in organic photovoltaics
JF  - Nature Communications
N2  - Strong light-matter coupling can re-arrange the exciton energies in organic semiconductors. Here, we exploit strong coupling by embedding a fullerene-free organic solar cell (OSC) photo-active layer into an optical microcavity, leading to the formation of polariton peaks and a red-shift of the optical gap. At the same time, the open-circuit voltage of the device remains unaffected. This leads to reduced photon energy losses for the low-energy polaritons and a steepening of the absorption edge. While strong coupling reduces the optical gap, the energy of the charge-transfer state is not affected for large driving force donor-acceptor systems. Interestingly, this implies that strong coupling can be exploited in OSCs to reduce the driving force for electron transfer, without chemical or microstructural modifications of the photoactive layer. Our work demonstrates that the processes determining voltage losses in OSCs can now be tuned, and reduced to unprecedented values, simply by manipulating the device architecture.
Y1  - 2019
U6  - https://doi.org/10.1038/s41467-019-11717-5
SN  - 2041-1723
VL  - 10
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Deschler, Felix
A1  - Neher, Dieter
A1  - Schmidt-Mende, Lukas
T1  - Perovskite semiconductors for next generation optoelectronic applications
JF  - APL Materials
Y1  - 2019
U6  - https://doi.org/10.1063/1.5119744
SN  - 2166-532X
VL  - 7
IS  - 8
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Kniepert, Juliane
A1  - Paulke, Andreas
A1  - Perdigon-Toro, Lorena
A1  - Kurpiers, Jona
A1  - Zhang, Huotian
A1  - Gao, Feng
A1  - Yuan, Jun
A1  - Zou, Yingping
A1  - Le Corre, Vincent M.
A1  - Koster, Lambert Jan Anton
A1  - Neher, Dieter
T1  - Reliability of charge carrier recombination data determined with charge extraction methods
JF  - Journal of applied physics
N2  - Charge extraction methods are popular for measuring the charge carrier density in thin film organic solar cells and to draw conclusions about the order and coefficient of nongeminate charge recombination. However, results from such studies may be falsified by inhomogeneous steady state carrier profiles or surface recombination. Here, we present a detailed drift-diffusion study of two charge extraction methods, bias-assisted charge extraction (BACE) and time-delayed collection field (TDCF). Simulations are performed over a wide range of the relevant parameters. Our simulations reveal that both charge extraction methods provide reliable information about the recombination order and coefficient if the measurements are performed under appropriate conditions. However, results from BACE measurements may be easily affected by surface recombination, in particular for small active layer thicknesses and low illumination densities. TDCF, on the other hand, is more robust against surface recombination due to its transient nature but also because it allows for a homogeneous high carrier density to be inserted into the active layer. Therefore, TDCF is capable to provide meaningful information on the order and coefficient of recombination even if the model conditions are not exactly fulfilled. We demonstrate this for an only 100 nm thick layer of a highly efficient nonfullerene acceptor (NFA) blend, comprising the donor polymer PM6 and the NFA Y6. TDCF measurements were performed as a function of delay time for different laser fluences and bias conditions. The full set of data could be consistently fitted by a strict second order recombination process, with a bias- and fluence-independent bimolecular recombination coefficient k(2) = 1.7 x 10(-17)m(3) s(-1). BACE measurements performed on the very same layer yielded the identical result, despite the very different excitation conditions. This proves that recombination in this blend is mostly through processes in the bulk and that surface recombination is of minor importance despite the small active layer thickness. Published under license by AIP Publishing.
Y1  - 2019
U6  - https://doi.org/10.1063/1.5129037
SN  - 0021-8979
SN  - 1089-7550
VL  - 126
IS  - 20
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Wang, Qiong
A1  - Mosconi, Edoardo
A1  - Wolff, Christian Michael
A1  - Li, Junming
A1  - Neher, Dieter
A1  - De Angelis, Filippo
A1  - Suranna, Gian Paolo
A1  - Grisorio, Roberto
A1  - Abate, Antonio
T1  - Rationalizing the molecular design of hole-selective contacts to improve charge extraction in Perovskite solar cells
JF  - dvanced energy materials
N2  - Two new hole selective materials (HSMs) based on dangling methylsulfanyl groups connected to the C-9 position of the fluorene core are synthesized and applied in perovskite solar cells. Being structurally similar to a half of Spiro-OMeTAD molecule, these HSMs (referred as FS and DFS) share similar redox potentials but are endowed with slightly higher hole mobility, due to the planarity and large extension of their structure. Competitive power conversion efficiency (up to 18.6%) is achieved by using the new HSMs in suitable perovskite solar cells. Time-resolved photoluminescence decay measurements and electrochemical impedance spectroscopy show more efficient charge extraction at the HSM/perovskite interface with respect to Spiro-OMeTAD, which is reflected in higher photocurrents exhibited by DFS/FS-integrated perovskite solar cells. Density functional theory simulations reveal that the interactions of methylammonium with methylsulfanyl groups in DFS/FS strengthen their electrostatic attraction with the perovskite surface, providing an additional path for hole extraction compared to the sole presence of methoxy groups in Spiro-OMeTAD. Importantly, the low-cost synthesis of FS makes it significantly attractive for the future commercialization of perovskite solar cells.
KW  - hole extraction
KW  - hole selective materials
KW  - perovskite solar cells
KW  - sulfur
KW  - triple-cation perovskite
Y1  - 2019
U6  - https://doi.org/10.1002/aenm.201900990
SN  - 1614-6832
SN  - 1614-6840
VL  - 9
IS  - 28
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Schwarze, Martin
A1  - Schellhammer, Karl Sebastian
A1  - Ortstein, Katrin
A1  - Benduhn, Johannes
A1  - Gaul, Christopher
A1  - Hinderhofer, Alexander
A1  - Toro, Lorena Perdigon
A1  - Scholz, Reinhard
A1  - Kublitski, Jonas
A1  - Roland, Steffen
A1  - Lau, Matthias
A1  - Poelking, Carl
A1  - Andrienko, Denis
A1  - Cuniberti, Gianaurelio
A1  - Schreiber, Frank
A1  - Neher, Dieter
A1  - Vandewal, Koen
A1  - Ortmann, Frank
A1  - Leo, Karl
T1  - Impact of molecular quadrupole moments on the energy levels at organic heterojunctions
JF  - Nature Communications
N2  - The functionality of organic semiconductor devices crucially depends on molecular energies, namely the ionisation energy and the electron affinity. Ionisation energy and electron affinity values of thin films are, however, sensitive to film morphology and composition, making their prediction challenging. In a combined experimental and simulation study on zinc-phthalocyanine and its fluorinated derivatives, we show that changes in ionisation energy as a function of molecular orientation in neat films or mixing ratio in blends are proportional to the molecular quadrupole component along the p-p-stacking direction. We apply these findings to organic solar cells and demonstrate how the electrostatic interactions can be tuned to optimise the energy of the charge-transfer state at the donor-acceptor interface and the dissociation barrier for free charge carrier generation. The confirmation of the correlation between interfacial energies and quadrupole moments for other materials indicates its relevance for small molecules and polymers.
Y1  - 2019
U6  - https://doi.org/10.1038/s41467-019-10435-2
SN  - 2041-1723
VL  - 10
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Ullbrich, Sascha
A1  - Benduhn, Johannes
A1  - Jia, Xiangkun
A1  - Nikolis, Vasileios C.
A1  - Tvingstedt, Kristofer
A1  - Piersimoni, Fortunato
A1  - Roland, Steffen
A1  - Liu, Yuan
A1  - Wu, Jinhan
A1  - Fischer, Axel
A1  - Neher, Dieter
A1  - Reineke, Sebastian
A1  - Spoltore, Donato
A1  - Vandewal, Koen
T1  - Emissive and charge-generating donor-acceptor interfaces for organic optoelectronics with low voltage losses
JF  - Nature materials
N2  - Intermolecular charge-transfer states at the interface between electron donating (D) and accepting (A) materials are crucial for the operation of organic solar cells but can also be exploited for organic light-emitting diodes(1,2). Non-radiative charge-transfer state decay is dominant in state-of-the-art D-A-based organic solar cells and is responsible for large voltage losses and relatively low power-conversion efficiencies as well as electroluminescence external quantum yields in the 0.01-0.0001% range(3,4). In contrast, the electroluminescence external quantum yield reaches up to 16% in D-A-based organic light-emitting diodes(5-7). Here, we show that proper control of charge-transfer state properties allows simultaneous occurrence of a high photovoltaic and emission quantum yield within a single, visible-light-emitting D-A system. This leads to ultralow-emission turn-on voltages as well as significantly reduced voltage losses upon solar illumination. These results unify the description of the electro-optical properties of charge-transfer states in organic optoelectronic devices and foster the use of organic D-A blends in energy conversion applications involving visible and ultraviolet photons(8-11).
KW  - Electronics, photonics and device physics
KW  - Optoelectronic devices and components
KW  - Photonic devices
KW  - Solar energy and photovoltaic technology
Y1  - 2019
U6  - https://doi.org/10.1038/s41563-019-0324-5
SN  - 1476-1122
SN  - 1476-4660
VL  - 18
IS  - 5
SP  - 459
EP  - 464
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Li, Tian-yi
A1  - Benduhn, Johannes
A1  - Qiao, Zhi
A1  - Liu, Yuan
A1  - Li, Yue
A1  - Shivhare, Rishi
A1  - Jaiser, Frank
A1  - Wang, Pei
A1  - Ma, Jie
A1  - Zeika, Olaf
A1  - Neher, Dieter
A1  - Mannsfeld, Stefan C. B.
A1  - Ma, Zaifei
A1  - Vandewal, Koen
A1  - Leo, Karl
T1  - Effect of H- and J-Aggregation on the Photophysical and Voltage Loss of Boron Dipyrromethene Small Molecules in Vacuum-Deposited Organic Solar Cells
JF  - The journal of physical chemistry letters
N2  - 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.
Y1  - 2019
U6  - https://doi.org/10.1021/acs.jpclett.9b01222
SN  - 1948-7185
VL  - 10
IS  - 11
SP  - 2684
EP  - 2691
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Zu, Fengshuo
A1  - Wolff, Christian Michael
A1  - Ralaiarisoa, Maryline
A1  - Amsalem, Patrick
A1  - Neher, Dieter
A1  - Koch, Norbert
T1  - Unraveling the Electronic Properties of Lead Halide Perovskites with Surface Photovoltage in Photoemission Studies
JF  - ACS applied materials & interfaces
N2  - The tremendous success of metal-halide perovskites, especially in the field of photovoltaics, has triggered a substantial number of studies in understanding their optoelectronic properties. However, consensus regarding the electronic properties of these perovskites is lacking due to a huge scatter in the reported key parameters, such as work function (Φ) and valence band maximum (VBM) values. Here, we demonstrate that the surface photovoltage (SPV) is a key phenomenon occurring at the perovskite surfaces that feature a non-negligible density of surface states, which is more the rule than an exception for most materials under study. With ultraviolet photoelectron spectroscopy (UPS) and Kelvin probe, we evidence that even minute UV photon fluxes (500 times lower than that used in typical UPS experiments) are sufficient to induce SPV and shift the perovskite Φ and VBM by several 100 meV compared to dark. By combining UV and visible light, we establish flat band conditions (i.e., compensate the surface-state-induced surface band bending) at the surface of four important perovskites, and find that all are p-type in the bulk, despite a pronounced n-type surface character in the dark. The present findings highlight that SPV effects must be considered in all surface studies to fully understand perovskites’ photophysical properties.
KW  - lead halide perovskite films
KW  - ultraviolet photoelectron spectroscopy
KW  - Kelvin probe
KW  - surface band bending
KW  - surface photovoltage
KW  - surface states
Y1  - 2019
U6  - https://doi.org/10.1021/acsami.9b05293
SN  - 1944-8244
SN  - 1944-8252
VL  - 11
IS  - 24
SP  - 21578
EP  - 21583
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Kegelmann, Lukas
A1  - Tockhorn, Philipp
A1  - Wolff, Christian Michael
A1  - Márquez, José A.
A1  - Caicedo Dávila, Sebastián
A1  - Korte, Lars
A1  - Unold, Thomas
A1  - Loevenich, Wilfried
A1  - Neher, Dieter
A1  - Rech, Bernd
A1  - Albrecht, Steve
T1  - Mixtures of Dopant-Free Spiro-OMeTAD and Water-Free PEDOT as a Passivating Hole Contact in Perovskite Solar Cells
JF  - ACS applied materials & interfaces
N2  - 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.
KW  - perovskite solar cell
KW  - selective contact
KW  - spiro-OMeTAD
KW  - PEDOT
KW  - recombination
KW  - passivation
KW  - quasi-Fermi level splitting
Y1  - 2019
U6  - https://doi.org/10.1021/acsami.9b01332
SN  - 1944-8244
SN  - 1944-8252
VL  - 11
IS  - 9
SP  - 9172
EP  - 9181
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Collado-Fregoso, Elisa
A1  - Pugliese, Silvina N.
A1  - Wojcik, Mariusz
A1  - Benduhn, Johannes
A1  - Bar-Or, Eyal
A1  - Toro, Lorena Perdigon
A1  - Hörmann, Ulrich
A1  - Spoltore, Donato
A1  - Vandewal, Koen
A1  - Hodgkiss, Justin M.
A1  - Neher, Dieter
T1  - Energy-gap law for photocurrent generation in fullerene-based organic solar cells
BT  - the case of low-donor-content blends
JF  - Journal of the American Chemical Society
N2  - The involvement of charge-transfer (CT) states in the photogeneration and recombination of charge carriers has been an important focus of study within the organic photovoltaic community. In this work, we investigate the molecular factors determining the mechanism of photocurrent generation in low-donor-content organic solar cells, where the active layer is composed of vacuum-deposited C-60 and small amounts of organic donor molecules. We find a pronounced decline of all photovoltaic parameters with decreasing CT state energy. Using a combination of steady-state photocurrent measurements and time-delayed collection field experiments, we demonstrate that the power conversion efficiency, and more specifically, the fill factor of these devices, is mainly determined by the bias dependence of photocurrent generation. By combining these findings with the results from ultrafast transient absorption spectroscopy, we show that blends with small CT energies perform poorly because of an increased nonradiative CT state decay rate and that this decay obeys an energy-gap law. Our work challenges the common view that a large energy offset at the heterojunction and/or the presence of fullerene clusters guarantee efficient CT dissociation and rather indicates that charge generation benefits from high CT state energies through a slower decay to the ground state.
Y1  - 2019
U6  - https://doi.org/10.1021/jacs.8b09820
SN  - 0002-7863
VL  - 141
IS  - 6
SP  - 2329
EP  - 2341
PB  - American Chemical Society
CY  - Washington
ER  -