Self-assembled donor-acceptor hole contacts for inverted perovskite solar cells with an efficiency approaching 22%: The impact of anchoring groups

Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing. Herein, we design and synthesize a series of donor-acceptor(D-A) type SAMs(MPA-BTCA, MPA-BT-BA, and MPA-BT-RA, where MPA is 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline;BT is benzo[c][1,2,5]-thiadiazole;CA is 2-cyanoacrylic acid, BA is benzoic acid, RA is rhodanine-3-propionic acid) with distinct anchoring groups, which show dramatically different properties. MPA-BTCA with CA anchoring groups exhibited stronger dipole moments and formed a homogeneous monolayer on the indium tin oxide(ITO) surface by adopting an upstanding self-assembling mode. However, the MPA-BT-RA molecules tend to aggregate severely in solid state due to the sp~3 hybridization of the carbon atom on the RA group, which is not favorable for achieving a long-range ordered self-assembled layer.Consequently, benefiting from high dipole moment, as well as dense and uniform self-assembled film,the device based on MPA-BT-CA yielded a remarkable power conversion efficiency(PCE) of 21.81%.Encouragingly, an impressive PCE approaching 20% can still be obtained for the MPA-BT-CA-based PSCs as the device area is increased to 0.80 cm^(2). Our work sheds light on the design principles for developing hole selecting SAMs, which will pave a way for realizing highly efficient, flexible, and large-area PSCs.

Optimization of solvent swelling for efficient organic solar cells via sequential deposition

Compared to bulk heterojunction(BHJ)organic solar cells(OSCs)prepared by the blend casting in“one step process”,sequential deposition(SD)processed OSCs can realize an ideal profile of vertical component distribution due to the swelling of polymer films.Herein,we did trials on several kinds of second solvents for swelling the polymer layer,and investigated the packing structure and morphology of the swollen films and the performance of the resulting devices.We found that an optimized morphology can be achieved by solvent swelling while using orthodichlorobenzene(o-DCB)as the second layer processing-solvent,with polymer donor PffBT-3 as bottom layer,PC71BM as top layer and bicontinuous networks in the middle.Such solvent swelling process also makes the SD method exempt from thermal annealing treatment.The device based on SD yields a power conversion effi-ciency(PCE)up to 8.7%without any post-treatment,outperforming those from the devices based on SD using other solvents and that(7.06%)from BHJ device,respectively.We also extended the use of this approach to allpolymer blend system,and successfully improved the efficiency from 4.72%(chloroform)to 9.35%(o-DCB),which is among the highest PCEs in all-polymer-based OSCs fabricated with SD method.The results demonstrate that the swelling of the polymer by the second layer solvent is a necessity for SD,paving the way towards additivefree high-performance OSCs.

Over 16% efficiency all-polymer solar cells by sequential deposition

All-polymer solar cells(all-PSCs) have received extensive attention due to their excellent mechanical robustness and performance stability. However, the power conversion efficiency(PCE) of all-PSCs still lags behind those of organic solar cells(OSCs)based on non-fullerene small molecule acceptors. Herein, we report highly efficient all-PSCs via sequential deposition(SD) with donor and acceptor layers coated sequentially to optimize the film microstructure. Compared with the bulk heterojunction(BHJ)all-PSCs, an optimized morphology with vertical component distribution was achieved for the SD-processed all-PSCs due to the synergistic effect of swelling of polymer films and using additive. Such strategy involves using chlorobenzene as the first layer processing-solvent for polymer donor, chloroform as the second processing-solvent for polymer acceptor with trace 1-chloronaphthalene, efficiently promoting exciton dissociation and charge extraction and reducing trap-assisted recombination.Consequently, over 16% all-PSCs fabricated via SD method was realized for the first time, which is much higher than that(15.2%) of its BHJ counterpart and also among the highest PCEs in all-PSCs. We have further demonstrated the generality of this approach in various all-polymer systems. This work indicates that the SD method can yield excellent all-PSCs and provides a facile approach to fabricating high-performance all-PSCs.

26 mA cm-2 JSC achieved in the integrated solar cells

Organometal halide perovskite has drawn much attention due to their high light-absorption coefficient,outstanding carrier mobility,and long-range charge-transport lengths.The most remarkable progress made by this type of perovskite materials is in the field of photovoltaics[1–4].The power conversion efficiency(PCE)of perovskite solar cells(PSCs)has exceeded 25%since they were first used as the active layer in solar cells in 2009[5].

A Cost-Effective D-A-D Type Hole-Transport Material Enabling 20% Efficiency Inverted Perovskite Solar Celis

High-performance,cost-effective hole-transport materials(HTMs)are greatly desired for the commercialization of perovskite solar cells(PVSCs).Herein,two new HTMs,TPA-FO and TPA-PDO,are devised and synthesized,which have a donor-acceptor-donor(D-A-D)type molecule design featuring carbonyl group-functionalized arenes as the acceptor(A)units.The carbonyl group at the central core of HTMs can not only tune frontier molecular orbital(FMO)energy levels and surface wettability,but also can enable efficient surface passivation effects,resulting in reduced recombination loss.When employed as HTMs in inverted PVSCs without using dopant,TPA-FO with one carbonyl group yields a high power conversion efficiency(PCE)of 20.24%,which is among the highest values reported in the inverted PVSCs with dopant-free HTMs.More importantly,the facile one-step synthetic process enables a low cost of 30 USD g^(-1) for TPA-FO,much cheaper than the most studied HTMs used for high-efficiency dopant-free PVSCs.These results demonstrate the potential of D-A-D type molecules with carbonyl group-functionalized arene core in developing the low-cost dopant-free HTMs toward highly efficient PVSCs.