TY  - JOUR
A1  - Alqahtani, Obaid
A1  - Babics, Maxime
A1  - Gorenflot, Julien
A1  - Savikhin, Victoria
A1  - Ferron, Thomas
A1  - Balawi, Ahmed H.
A1  - Paulke, Andreas
A1  - Kan, Zhipeng
A1  - Pope, Michael
A1  - Clulow, Andrew J.
A1  - Wolf, Jannic
A1  - Burn, Paul L.
A1  - Gentle, Ian R.
A1  - Neher, Dieter
A1  - Toney, Michael F.
A1  - Laquai, Frederic
A1  - Beaujuge, Pierre M.
A1  - Collins, Brian A.
T1  - Mixed Domains Enhance Charge Generation and Extraction in Bulk-Heterojunction Solar Cells with Small-Molecule Donors
JF  - Advanced energy materials
N2  - The interplay between nanomorphology and efficiency of polymer-fullerene bulk-heterojunction (BHJ) solar cells has been the subject of intense research, but the generality of these concepts for small-molecule (SM) BHJs remains unclear. Here, the relation between performance; charge generation, recombination, and extraction dynamics; and nanomorphology achievable with two SM donors benzo[1,2-b:4,5-b]dithiophene-pyrido[3,4-b]-pyrazine BDT(PPTh2)(2), namely SM1 and SM2, differing by their side-chains, are examined as a function of solution additive composition. The results show that the additive 1,8-diiodooctane acts as a plasticizer in the blends, increases domain size, and promotes ordering/crystallinity. Surprisingly, the system with high domain purity (SM1) exhibits both poor exciton harvesting and severe charge trapping, alleviated only slightly with increased crystallinity. In contrast, the system consisting of mixed domains and lower crystallinity (SM2) shows both excellent exciton harvesting and low charge recombination losses. Importantly, the onset of large, pure crystallites in the latter (SM2) system reduces efficiency, pointing to possible differences in the ideal morphologies for SM-based BHJ solar cells compared with polymer-fullerene devices. In polymer-based systems, tie chains between pure polymer crystals establish a continuous charge transport network, whereas SM-based active layers may in some cases require mixed domains that enable both aggregation and charge percolation to the electrodes.
KW  - charge transport
KW  - domain purity
KW  - microscopy
KW  - mixed domains
KW  - organic solar cells
KW  - photovoltaic devices
KW  - resonant X-ray scattering
KW  - small molecules
KW  - transient spectroscopy
Y1  - 2018
U6  - https://doi.org/10.1002/aenm.201702941
SN  - 1614-6832
SN  - 1614-6840
VL  - 8
IS  - 19
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Jiang, Wei
A1  - Stolterfoht, Martin
A1  - Jin, Hui
A1  - Burn, Paul L.
T1  - Hole-transporting poly(dendrimer)s as electron donors for low donor organic solar cells with efficient charge transport
JF  - Macromolecules : a publication of the American Chemical Society
N2  - Recent work on bulk-heterojunction organic solar cells has shown that photoexcitation of the electron acceptor followed by photoinduced hole transfer can play a significant role in photocurrent generation. To establish a clear understanding of the role of the donor in the photoinduced hole transfer process, we have synthesized a series of triphenylamine-based hole-transporting poly(dendrimer)s with mechanically flexible nonconjugated backbones via ring-opening metathesis polymerization and used them in low donor content solar cells. The poly(dendrimer)s were found to retain the hole transporting properties of the parent dendrimer, with hole mobilities of similar to 10(-3) cm(2)/(V s) for solution processed neat films. However, when blended with [6,6]-phenyl-C-70-butyric acid methyl ester (PC70BM), the best performing poly(dendrimer) was found to form films that had balanced and relatively high hole/electron mobilities of similar to 5 x 10(-4) cm(2) /(V s). In contrast, at the same concentration the parent dendrimer:PC70BM blend was found to have a hole mobility of 4 orders of magnitude less than the electron mobility. The balanced hole and electron mobilities for the 6 wt % poly(dendrimer):PC70BM blend led to an absence of second-order bimolecular recombination losses at the maximum power point and resulted in a fill factor of 0.65 and a PCE 2.1% for the devices, which was almost three times higher than the cells composed of the parent dendrimer:PC70BM blends.
Y1  - 2020
U6  - https://doi.org/10.1021/acs.macromol.0c00520
SN  - 0024-9297
SN  - 1520-5835
VL  - 53
IS  - 8
SP  - 2902
EP  - 2911
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Jiang, Wei
A1  - Tao, Chen
A1  - Stolterfoht, Martin
A1  - Jin, Hui
A1  - Stephen, Meera
A1  - Lin, Qianqian
A1  - Nagiri, Ravi C. R.
A1  - Burn, Paul L.
A1  - Gentle, Ian R.
T1  - Hole-transporting materials for low donor content organic solar cells
BT  - charge transport and device performance
JF  - Organic electronics : physics, materials and applications
N2  - Low donor content solar cells are an intriguing class of photovoltaic device about which there is still considerable discussion with respect to their mode of operation. We have synthesized a series of triphenylamine-based materials for use in low donor content devices with the electron accepting [6,6]-phenyl-C71-butyric acid methyl ester (PC(7)0BM). The triphenylamine-based materials absorb light in the near UV enabling the PC(7)0BM to be be the main light absorbing organic semiconducting material in the solar cell. It was found that the devices did not operate as classical Schottky junctions but rather photocurrent was generated by hole transfer from the photo-excited PC(7)0BM to the triphenylamine-based donors. We found that replacing the methoxy surface groups with methyl groups on the donor material led to a decrease in hole mobility for the neat films, which was due to the methyl substituted materials having the propensity to aggregate. The thermodynamic drive to aggregate was advantageous for the performance of the low donor content (6 wt%) films. It was found that the 6 wt% donor devices generally gave higher performance than devices containing 50 wt% of the donor.
KW  - photoexcited hole transfer
KW  - photocurrent generation
KW  - synthesis
KW  - hole
KW  - mobility
KW  - low donor content
KW  - Schottky junction
Y1  - 2020
U6  - https://doi.org/10.1016/j.orgel.2019.105480
SN  - 1566-1199
SN  - 1878-5530
VL  - 76
PB  - Elsevier
CY  - Amsterdam
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Wolff, Christian Michael
A1  - Marquez, Jose A.
A1  - Zhang, Shanshan
A1  - Hages, Charles J.
A1  - Rothhardt, Daniel
A1  - Albrecht, Steve
A1  - Burn, Paul L.
A1  - Meredith, Paul
A1  - Unold, Thomas
A1  - Neher, Dieter
T1  - Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells
JF  - Nature Energy
N2  - The performance of perovskite solar cells is predominantly limited by non-radiative recombination, either through trap-assisted recombination in the absorber layer or via minority carrier recombination at the perovskite/transport layer interfaces. Here, we use transient and absolute photoluminescence imaging to visualize all non-radiative recombination pathways in planar pintype perovskite solar cells with undoped organic charge transport layers. We find significant quasi-Fermi-level splitting losses (135 meV) in the perovskite bulk, whereas interfacial recombination results in an additional free energy loss of 80 meV at each individual interface, which limits the open-circuit voltage (V-oc) of the complete cell to similar to 1.12 V. Inserting ultrathin interlayers between the perovskite and transport layers leads to a substantial reduction of these interfacial losses at both the p and n contacts. Using this knowledge and approach, we demonstrate reproducible dopant-free 1 cm(2) perovskite solar cells surpassing 20% efficiency (19.83% certified) with stabilized power output, a high V-oc (1.17 V) and record fill factor (>81%).
KW  - Energy science and technology
KW  - Solar cells
Y1  - 2018
U6  - https://doi.org/10.1038/s41560-018-0219-8
SN  - 2058-7546
VL  - 3
IS  - 10
SP  - 847
EP  - 854
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Yazmaciyan, Aren
A1  - Stolterfoht, Martin
A1  - Burn, Paul L.
A1  - Lin, Qianqian
A1  - Meredith, Paul
A1  - Armin, Ardalan
T1  - Recombination losses above and below the transport percolation threshold in bulk heterojunction organic solar cells
JF  - Advanced energy materials
N2  - Achieving the highest power conversion efficiencies in bulk heterojunction organic solar cells requires a morphology that delivers electron and hole percolation pathways for optimized transport, plus sufficient donor:acceptor contact area for near unity charge transfer state formation. This is a significant structural challenge, particularly in semiconducting polymer:fullerene systems. This balancing act in the model high efficiency PTB7:PC70BM blend is studied by tuning the donor:acceptor ratio, with a view to understanding the recombination loss mechanisms above and below the fullerene transport percolation threshold. The internal quantum efficiency is found to be strongly correlated to the slower carrier mobility in agreement with other recent studies. Furthermore, second-order recombination losses dominate the shape of the current density-voltage curve in efficient blend combinations, where the fullerene phase is percolated. However, below the charge transport percolation threshold, there is an electric-field dependence of first-order losses, which includes electric-field-dependent photogeneration. In the intermediate regime, the fill factor appears to be limited by both first- and second-order losses. These findings provide additional basic understanding of the interplay between the bulk heterojunction morphology and the order of recombination in organic solar cells. They also shed light on the limitations of widely used transport models below the percolation threshold.
KW  - bulk heterojunctions
KW  - charge transport
KW  - organic solar cells
KW  - percolation threshold
KW  - recombination losses
Y1  - 2018
U6  - https://doi.org/10.1002/aenm.201703339
SN  - 1614-6832
SN  - 1614-6840
VL  - 8
IS  - 18
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Zhang, Shanshan
A1  - Hosseini, Seyed Mehrdad
A1  - Gunder, Rene
A1  - Petsiuk, Andrei
A1  - Caprioglio, Pietro
A1  - Wolff, Christian Michael
A1  - Shoaee, Safa
A1  - Meredith, Paul
A1  - Schorr, Susan
A1  - Unold, Thomas
A1  - Burn, Paul L.
A1  - Neher, Dieter
A1  - Stolterfoht, Martin
T1  - The Role of Bulk and Interface Recombination in High-Efficiency Low-Dimensional Perovskite Solar Cells
JF  - Advanced materials
N2  - 2D Ruddlesden-Popper perovskite (RPP) solar cells have excellent environmental stability. However, the power conversion efficiency (PCE) of RPP cells remains inferior to 3D perovskite-based cells. Herein, 2D (CH3(CH2)(3)NH3)(2)(CH3NH3)(n-1)PbnI3n+1 perovskite cells with different numbers of [PbI6](4-) sheets (n = 2-4) are analyzed. Photoluminescence quantum yield (PLQY) measurements show that nonradiative open-circuit voltage (V-OC) losses outweigh radiative losses in materials with n > 2. The n = 3 and n = 4 films exhibit a higher PLQY than the standard 3D methylammonium lead iodide perovskite although this is accompanied by increased interfacial recombination at the top perovskite/C-60 interface. This tradeoff results in a similar PLQY in all devices, including the n = 2 system where the perovskite bulk dominates the recombination properties of the cell. In most cases the quasi-Fermi level splitting matches the device V-OC within 20 meV, which indicates minimal recombination losses at the metal contacts. The results show that poor charge transport rather than exciton dissociation is the primary reason for the reduction in fill factor of the RPP devices. Optimized n = 4 RPP solar cells had PCEs of 13% with significant potential for further improvements.
KW  - 2D perovskites
KW  - interface recombination
KW  - perovskite solar cells
KW  - photoluminescence
KW  - V-OC loss
Y1  - 2019
U6  - https://doi.org/10.1002/adma.201901090
SN  - 0935-9648
SN  - 1521-4095
VL  - 31
IS  - 30
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Zhang, Shanshan
A1  - Stolterfoht, Martin
A1  - Armin, Ardalan
A1  - Lin, Qianqian
A1  - Zu, Fengshuo
A1  - Sobus, Jan
A1  - Jin, Hui
A1  - Koch, Norbert
A1  - Meredith, Paul
A1  - Burn, Paul L.
A1  - Neher, Dieter
T1  - Interface Engineering of Solution-Processed Hybrid Organohalide Perovskite Solar Cells
JF  - ACS applied materials & interfaces
N2  - Engineering the interface between the perovskite absorber and the charge-transporting layers has become an important method for improving the charge extraction and open-circuit voltage (V-OC) of hybrid perovskite solar cells. Conjugated polymers are particularly suited to form the hole-transporting layer, but their hydrophobicity renders it difficult to solution-process the perovskite absorber on top. Herein, oxygen plasma treatment is introduced as a simple means to change the surface energy and work function of hydrophobic polymer interlayers for use as p-contacts in perovskite solar cells. We find that upon oxygen plasma treatment, the hydrophobic surfaces of different prototypical p-type polymers became sufficiently hydrophilic to enable subsequent perovskite junction processing. In addition, the oxygen plasma treatment also increased the ionization potential of the polymer such that it became closer to the valance band energy of the perovskite. It was also found that the oxygen plasma treatment could increase the electrical conductivity of the p-type polymers, facilitating more efficient charge extraction. On the basis of this concept, inverted MAPbI(3) perovskite devices with different oxygen plasma-treated polymers such as P3HT, P3OT, polyTPD, or PTAA were fabricated with power conversion efficiencies of up to 19%.
KW  - organohalide lead perovskites
KW  - solar cells
KW  - surface wetting
KW  - work function
KW  - oxygen plasma
KW  - transport layer
Y1  - 2018
U6  - https://doi.org/10.1021/acsami.8b02503
SN  - 1944-8244
VL  - 10
IS  - 25
SP  - 21681
EP  - 21687
PB  - American Chemical Society
CY  - Washington
ER  -