Solution-processed Organic Solar Cells Research Articles

Utilizing Metal Oxide Thin Films for Device Engineering of Solution-Processed Organic Multi-Junction Solar Cells

Electron and hole transporting layers play a major role in high-performance and stable organic-based optoelectronic devices. This paper demonstrates detailed device engineering of multi-junction organic photovoltaics built on two different metal oxide-based electron and hole transport (buffer) layers prepared by thermal or solution-processed methods. The main focus is on the device processing parameters as well as practical details of preparation of buffer layers to give the research community a clear, step-by-step recipe to successfully replicate and build series and parallel connected multi-junction solution-based organic solar cells for their needs. Here, the recipes and deposition conditions of two metal oxide buffer layers are presented in detail, based on basic commercially available materials and tools, to achieve well-engineered tandem (multi-junction) solution-processed organic solar cells. The buffer layers have appropriate energy levels for electrical selectivity of anode and cathode electrodes, and they are highly stable and chemically compatible with processing of solution-based polymer solar cells. To demonstrate the engineering steps of multi-junction devices, the PCE10:PC70BM blend is used as the active layer for all subcells. Then, to improve the power conversion efficiency of the single-junction photovoltaic device, PCE10:PC70BM blend is used in combination with DPPx:PC70BM with different absorption spectra for bottom and top subcell active layers. An optimized series tandem device with 10.6% power conversion efficiency is demonstrated. Generally, the device structures reported here can also be used for other types of optoelectronic devices, such as light emitting diodes and photodetectors.

Synergistic strategies to unveil the dual influence of additive and annealing treatment on the morphology of isatin-derived low bandgap small molecule donor in solution-processed organic solar cells

A novel organic small molecule, 5-(4-(diphenylamino)phenyl)-1-octylindoline-2,3-dione (TPI) containing an alkyl chain substituted electron accepting isatin (indoline-2,3-dione) and strong electron withdrawing N, N-diphenylaniline units have been synthesized through Suzuki coupling reaction. The molecular structure of TPI is confirmed by NMR, FT-IR, and Mass spectroscopy techniques. The TPI molecule exhibits a low band gap of approximately ∼ 2.03 eV which is also supported by the DFT results. The influence of additive and heat treatment on the electronic, morphological, and photovoltaic performance of organic solar cells was investigated meticulously. The TPI donor exhibits complementary light absorption with fullerene acceptor in combination with DIO and TA which efficiently absorb the photon in the 300–730 nm range. The TPI was later used as an electron donor material for the fabrication of organic solar cells. Remarkably, the morphology-dependent optimized TPI:PC71BM (1:3.0) exposed excellent power conversion efficiency (PCE) of about ∼ 5.56 % with enhanced VOC of ∼ 0.811 V, JSC of 11.81 mA cm−2 and FF of 55.3 % fabricated in addition with DIO and thermal annealing treatment. Most importantly, the unencapsulated devices maintained > 96 % of the initial PCE value after 240 h under ambient temperature. Our findings indicate that isatin-derived small molecules with simple architecture propose great potential for promising BHJ-OSCs material.

Critical role of the end-group acceptor in enhancing the efficiency of indacenodithiophene-benzothiadiazole-linked nonfullerene organic solar cells through morphology optimization

Solution-processed organic solar cells (OSCs) have great promise for next-generation solar energy conversion technologies. Innovative acceptors are constantly being designed to improve device efficiency. In this work, we designed and synthesized a series of A–π–D–π–A type non-fullerene acceptor (NFA) molecules, named IB-TOT, IB-TOM, IB-IOO, and IB-IOM for their applications in OSCs. All molecules showed high thermal stability, broad photoabsorption, and relatively lower highest occupied molecular orbital (HOMO) energy levels from −5.48 eV to −5.58 eV. The optimized OSCs based on these NFAs and PTB7-Th donor deliver power conversion efficiencies (PCEs) of 8.19%, 5.50%, 2.42%, and 3.10% for IB-TOT, IB-TOM, IB-IOO, and IB-IOM molecules, respectively. The higher PCE of IB-TOT-based OSCs is attributed to their excellent miscibility and superior interpenetrating network morphology compared to the other three compounds. These results demonstrate that using the 3-ethylrhodanine acceptor unit to construct the NFA molecule is a successful approach for outstanding achievement in OSCs.

Recent Progress in Semitransparent Organic Solar Cells: Photoabsorbent Materials and Design Strategies.

The increasing energy demands of the global community can be met with solar energy. Solution-processed organic solar cells have seen great progress in power conversion efficiencies (PCEs). Semitransparent organic solar cells (ST-OSCs) have made enormous progress in recent years and have been considered one of the most promising solar cell technologies for applications in building-integrated windows, agricultural greenhouses, and wearable energy resources. Therefore, through the synergistic efforts of transparent electrodes, engineering in near-infrared photoabsorbent materials, and device engineering, high-performance ST-OSCs have developed, and PCE and average visible transmittance reach over 10% and 40%, respectively. In this review, we present the recent progress in photoabsorbent material engineering and strategies for enhancing the performance of ST-OSCs to help researchers gain a better understanding of structure-property-performance relationships. To conclude, new design concepts in material engineering and outlook are proposed to facilitate the further development of high-performance ST-OSCs.

The critical role of temperature-dependent mobilities in determining the open-circuit voltage of bulk-heterojunction organic solar cells

While solution-processed bulk-heterojunction organic solar cells (OSCs) continue to attract attention as their efficiencies approach 20%, the physical origin of the non-radiative energy loss in OSCs remains under debate. Understanding the temperature dependence of open-circuit voltage (VOC) is thus important because it provides unique insights into the origin of energy loss. Herein, we simulate the VOC vs T relation of PTB7-Th:PC71BM bulk-heterojunction OSCs within the range of 160–295 K by incorporating experimentally measured temperature-dependent mobilities into the drift-diffusion model, assuming bimolecular recombination as the primary recombination mechanism. Significantly, we find that the temperature dependence of VOC can only be correctly reproduced by the model when the temperature dependence of the carrier mobilities is taken into account. The effect of the Langevin reduction coefficient on the temperature dependence of VOC is also investigated.

Solution Processed Semi-Transparent Organic Solar Cells Over 50% Visible Transmittance Enabled by Silver Nanowire Electrode with Sandwich Structure.

Photovoltaic windows with easy installation for the power supply of household appliances have long been a desire of energy researchers. However, due to the lack of top electrodes that offer both high transparency and low sheet resistance, the development of high-transparency photovoltaic windows for indoor lighting scenarios has lagged significantly behind photovoltaic windows where privacy issues are involved. Addressing this issue, this work develops a solution-processable transparent top electrode using sandwich structure silver nanowires, realizing high transparency in semi-transparent organic solar cells. The wettability and conducting properties of the electrode are improved by a modified hole-transport layer named HP. The semi-transparent solar cell exhibits good see-through properties at a high average visible transmittance of 50.8%, with power conversion efficiency of 7.34%, and light utilization efficiency of 3.73%, which is the highest without optical modulations. Moreover, flexible devices based on the above-mentioned architecture also show excellent mechanical tolerance compared with Ag electrode counterparts, which retains 94.5% of their original efficiency after 1500 bending cycles. This work provides a valuable approach for fabricating solution-processed high transparency organic solar cells, which is essential in future applications in building integrated photovoltaics.

Vacuum deposited organic solar cells with BTIC-H as A–D–A non-fullerene acceptor

The record power conversion efficiency of solution-processed organic solar cells (OSCs) has almost doubled since non-fullerene acceptors (NFAs) replaced fullerene derivatives as the best-performing acceptor molecules. The successful transition from C60 to NFAs is still pending for vacuum-thermal evaporated (VTE) OSCs, not least because most NFAs are too large to be evaporated without breaking. Due to VTE’s relevance in terms of industrial manufacturing, discovering high-performing VTE NFAs is a major opportunity for OSCs. Here, we fabricate evaporated OSCs based on the NFA BTIC-H known from solution processing. This A–D–A molecule has an unfused bithiophene core, 1,1-dicyanomethylene-3-indanone end groups, and hexyl side chains, making it small enough to be evaporated well. We pair BTIC-H with four commonly used evaporated donors—DCV5T-Me(3,3), DTDCPB, HB194, and SubNc—in planar heterojunctions. We observe appreciable photocurrents and a voltage loss of ∼0.8 V, matching that of corresponding C60 devices. Donor:BTIC-H bulk heterojunctions likely face charge collection issues due to unfavorable microstructure. Our work demonstrates one of few NFA based evaporated OSCs with encouraging performance results and gives one potential starting point for molecule design of further NFAs suitable for VTE.

Design of novel organoboron small-molecule dyes based on dipolar nitrogen-boron-nitrogen unit for solution-processed photovoltaic devices

The nitrogen-boron-nitrogen (N–B–N) structure combined with strong polar B–N and B←N bonds simultaneously, opens a new window for the development of organoboron photovoltaic materials with narrow band gap and low highest occupied molecular orbital (HOMO) energy level. In this paper, two N–B–N-embedded blocks including boron dipyrromethane (BODIPY) and double B–N bridged bipyridyl (BNBP), are exploited to rationally regulate the band gap and energy level of the resulting material by virtue of their strong electron affinities. Thus, the thiophene as a weak electron-donating part is directly attached to strong electron-withdrawing BODIPY and BNBP respectively, giving much improved photoelectric properties for such simple push-pull architectures. To further improve photoelectric and thermal properties of the material, two novel extended D-π-A-π-D-type organoboron molecules namely BDPTPA and BNBPTPA, in which BODIPY and BNBP as strong electron-deficient core (A) connect strong electron-rich triphenylamine (D) via thiophene π-spacer, are synthesized by Stille reaction between BODIPY/BNBP and “π-D” segment. Therefore, BDPTPA exhibits a preferable electrochemical band gap as small as 1.36 eV close to near-infrared (NIR) region, which is one of the lowest values among the BODIPY-based small-molecule donors (SMDs). Furthermore, BNBPTPA shows stronger light absorption of up to 1.16 × 105 M−1 cm−1, deeper HOMO energy level of −5.28 eV and very excellent thermal stability (Td = 428 °C). It is mentioning that, BNBPTPA is first used as SMD material, blending with [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) for solution-processed organic solar cell. Consequently, a reasonable power conversion efficiency (PCE) of 6.78% has been achieved with a satisfactory short-circuit density (Jsc) of 17.27 mA cm−2 and open-circuit voltage (Voc) of 0.87 V, which is the highest efficiency for BNBP-based SMDs so far. Our work demonstrates that a proposed molecular design and synthesis with dipolar N–B–N-containing unit and “π-D” fragment, can greatly broaden the types of new photovoltaic donor materials.

Improving the Performance of Layer-by-Layer Processed Organic Solar Cells via Introducing a Wide-Bandgap Dopant into the Upper Acceptor Layer.

The layer-by-layer (LbL) solution-processed organic solar cells (OSCs) are conductive to achieve vertical phase separation, tunable donor-acceptor (D/A) interfaces, and favorable charge-transport pathways. In this work, a wide-bandgap component poly(9-vinylcarbazole) (PVK) is added to the upper electron acceptor layer to improve the performance of LbL-processed OSCs. Results show that the PVK component can adjust the film morphology, dope the electron acceptor, increase the electron concentration, and improve charge transport. Such n-type doping is verified by Seebeck coefficient measurement, ultraviolet photoelectron spectroscopy, and electron paramagnetic resonance characterization. In addition, the fluorescence intensity and exciton lifetime of the PVK-doped acceptor film are increased, thus being beneficial for exciton diffusion to the D/A interface. Therefore, the power conversion efficiency (PCE) of LbL OSCs increases when 2.50 wt.% PVK is employed in the electron acceptor layer of commonly-used high-efficiency system and a maximum value of 19.05% can be achieved. The role of PVK played in the active layer is different from those of additives and ternary components reported previously, so the results provide an alternative way to enhance the device performance of LbL-processed OSCs.

A 3-Fluoropyridine Manipulating the Aggregation and Fibril Network of Donor Polymers for Eco-Friendly Solution-Processed Versatile Organic Solar Cells.

The development of eco-friendly solvent-processed organic solar cells (OSCs) suitable for industrial-scale production should be now considered the imperative research. Herein, asymmetric 3-fluoropyridine (FPy) unit is used to control the aggregation and fibril network of polymer blends. Notably, terpolymer PM6(FPy = 0.2) incorporating 20% FPy in a well-known donor polymer poly[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione)] (PM6) can reduce the regioregularity of the polymer backbone and endow them with much-enhanced solubility in eco-friendly solvents. Accordingly, the excellent adaptability for fabricating versatile devices based on PM6(FPy = 0.2) by toluene processing is demonstrated. The resulting OSCs exhibit a high power conversion efficiency (PCE) of 16.1% (17.0% by processed with chloroform) and low batch-to-batch variation. Moreover, by controlling the donor-to-acceptor weight ratio at 0.5:1.0 and 0.25:1.0, semi-transparent OSCs (ST-OSCs) yield significant light utilization efficiencies of 3.61% and 3.67%, respectively. For large-area (1.0cm2 ) indoor OSC (I-OSC), a high PCE of 20.6% is achieved with an appropriate energy loss of 0.61eV under a warm white light-emitting diode (3,000K) with the illumination of 958lux. Finally, the long-term stability of the devices is evaluated by investigating their structure-performance-stability relationship. This work provides an effective approach to realizing eco-friendly, efficient, and stable OSCs/ST-OSCs/I-OSCs.

Suppressing Bimolecular Charge Recombination and Energetic Disorder with Planar Heterojunction Active Layer Enables 18.1% Efficiency Binary Organic Solar Cells

The performance of organic solar cells has been dramatically enhanced due to the use of bulk heterojunction active layer structure. However, blending donor and acceptor in the bulk volume results in a large extent of bimolecular charge recombination and increasing energetic disorder. Herein, we fabricated organic solar cells with polymer donor PM6 and nonfullerene acceptor N3 in bilayer structure to investigate the impact of planar heterojunction configurations on charge recombination and energetic landscapes. We find superior crystallinity features in the bilayer composed of pure donor and acceptor layers. The bimolecular charge recombination and energetic disorder are effectively suppressed compared with the bulk heterojunction counterparts. Thus, a power conversion efficiency as high as 18.1% (17.8% averaged) is achieved, which stands among the top values of planar heterojunction organic solar cells. In addition, improved device shelf stability is observed because of the fewer donor–acceptor interfaces in the active layer. Our results suggest that a planar heterojunction structure could efficiently suppress the bimolecular charge recombination and energetic disorder, providing an alternative pathway for developing solution-processed organic solar cells.

A bottom-up understanding of the ligand-dominated formation of metallic nanoparticle electrodes with high broadband reflectance for enabling fully solution-processed large-area organic solar cells

Understanding the ligand-dominant impact on silver nanoparticles aids in the realization of compact-packed silver nanoparticle electrodes with high broadband reflectance, resulting in an evaporation-free large-area organic solar cell.

S,N-Heteropentacene-based molecular donor–acceptor dyads: structure–property relationships and application in single-material organic solar cells

Molecular donor–acceptor dyads D11–D18 using S,N-heteropentacenes SN5′ and fullerenic acceptors were synthesized and applied in solution-processed single-material organic solar cells reaching power conversion efficiencies of up to 2.8%.

Molecular engineering of new electron acceptor for highly efficient solution processable organic solar cells using state-of-the-art polymer donor PffBT4T-2OD

Two molecularly engineered fullerene-based electron acceptors, coded as BITh-C60 and BITh-C70, were designed, synthesized and fully characterized. The molecules have LUMO energy levels at −3.62 and-3.65 eV; and HOMO energy levels at −5.62 and −5.60 eV, respectively as confirmed by cyclic voltammetry. The acceptor BITh-C70 shows comparatively broader and stronger absorption with respect to BITh-C60. A narrow band gap polymer poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3′′′-di(2-octyldodecyl) 2,2′;5′,2″;5″,2′′′-quaterthiophen-5,5′′′-diyl)] (PffBT4T-2OD) was used to construct the solution processed bulk-heterojunction solar cells. Under optimized fabrication and evaluation conditions, BITh-C60 and BITh-C70 showed a highest power conversion efficiency (PCE) of 8.1 % and 8.8 %, respectively, which are comparatively higher than the PCEs obtained from the respective reference solar cells. The PffBT4T-2OD:BITh-C70 based BHJ solar cell shows a nearly flat EQE spectra of 75 % between 380 and 700 nm.

Fully solution-processed, light-weight, and ultraflexible organic solar cells

Organic photovoltaic (OPV) devices have the potential to be superior to other PV technologies for the use in applications that require very high flexibility or maximum specific power (power-per-weight ratio), such as textile integration, wearable electronics, or outer space applications. However, OPV devices also require encapsulation by barrier films to reduce the degradation driven by extrinsic factors, which in turn limits their flexibility and leads to lower specific power values. In this work, fully solution-processed (including both electrodes) semitransparent organic solar cells (OSCs) with performance comparable with conventional indium tin oxide-based devices are processed directly onto different barrier films of varying thicknesses. Direct cell fabrication onto barrier films leads to the elimination of the additional polyethylene terephthalate substrate and one of the two adhesive layers in the final stack of an encapsulated OPV device by replacing the industrial state-of-the-art sandwich encapsulation with a top-only encapsulation process, which yields significantly thinner and lighter ‘product-relevant’ PV devices. In addition to the increase of the specific power to 0.38 W g−1, which is more than four times higher than sandwich-encapsulated devices, these novel OSCs exhibit better flexibility and survive 5000 bending cycles with 4.5 mm bending radius. Moreover, the devices show comparable stability as conventionally encapsulated devices under constant illumination (1 sun) in ambient air for 1000 h. Finally, degradation under damp heat conditions (65 °C, 85% rh) was investigated and found to be determined by a combination of different factors, namely (UV) light soaking, intrinsic barrier properties, and potential damaging of the barriers during (laser) processing.

Novel A-π-D-π-A-type BODIPY dyads as small-molecule donors for solution-processed organic solar cells

Two novel narrow-bandgap A-π-D-π-A-type BODIPY dyes were synthesizedviaa one-step Stille reaction with “D-π” segment at the β-site of BODIPY unit, where CTBDP-based device gave an impressive PCE of 5.85% with an excellentJscof 17.70 mA cm−2.

Nanoscale heterogeneous distribution of surface energy at interlayers in organic bulk-heterojunction solar cells

<h2>Summary</h2> Surface energy of the underneath interlayer plays a crucial role in determining the morphology of bulk-heterojunction (BHJ) film in solution-processed organic solar cells (OSCs). However, little attention has been paid to this perspective at the microscopic level. In this study, we demonstrate an effective strategy to tune the nanoscale heterogeneous distribution of surface energy (HeD-SE) at interlayers through incorporating two-dimensional (2D) MoS₂ nanosheets, which modulate the component distribution, molecular orientation, and phase separation in the upper BHJ layers, leading to suppressed charge recombination and increased charge extraction in devices with enhanced power conversion efficiency (PCE) and device stability. Furthermore, we explore the relationship among the different surface energies of BHJs between the donor and the acceptor, the nanoscale HeD-SE at interlayers, and the PCEs of the resultant devices. This work reveals the impact of nanoscale heterogeneity in the distribution of surface energy in the underneath interlayers on the BHJ morphology and device performance in OSCs.

Utilizing the unique charge extraction properties of antimony tin oxide nanoparticles for efficient and stable organic photovoltaics

Simultaneously enhancing device performance and longevity, as well as balancing the requirements on cost, scalability, and simplification of processing, is the goal of interface engineering of organic solar cells (OSCs). In our work, we strategically introduce antimony (Sb 3+ ) cations into an efficient and generic n-type SnO 2 nanoparticles (NPs) host during the scalable flame spray pyrolysis synthesis. Accordingly, a significant switch of conduction property from an n-type character to a p-type character is observed, with a corresponding shift in the work function (WF) from 4.01 ± 0.02 eV for pristine SnO 2 NPs to 5.28 ± 0.02 eV for SnO 2 NPs with 20 mol. % Sb content (ATO). Both pristine SnO 2 and ATO NPs with fine-tuned optoelectronic properties exhibit remarkable charge carrier extraction properties, excellent UV resistance and photo-stability being compatible with various state-of-the-art OSCs systems. The reliable and scalable pristine SnO 2 and ATO NPs processed by doctor-blading in air demand no complex post-treatment. Our work offers a simple but unique approach to accelerate the development of advanced interfacial materials, which could circumvent the major existing interfacial problems in solution-processed OSCs. • Introducing antimony cations to effectively dope the n-type SnO 2 nanoparticles. • In-depth characterization of the cation doping effect and mechanisms. • Validation of the generic applicability of the p-type doped nanoparticles for organic photovoltaic applications. • Demonstrating efficient and stable organic solar cells based on state-of-the-art organic photovoltaic materials.

Fully vacuum-free large-area organic solar cell fabrication from polymer top electrode

Fully vacuum-free and solution-processed large-area organic solar cells (OSCs) were fabricated using a poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) polymer top electrode. In addition, to evaluate the scalability of this polymer electrode toward large-scale modules, OSCs with various sized areas were fabricated, and their performance was compared with that of a metal top electrode. As a result, when we increased the area of the OSC from 0.4 to 1.6 cm2, the fill factor (FF) decreased from 40.5 % to 30.3 % and the corresponding photoconversion efficiency (PCE) decreased from 2.0 % to 1.4 % for an OSC with a polymer electrode. The FF decreased from 54.8 % to 44.1 % and essentially had no PCE degradation for the OSC with a metal electrode. Numerical calculations were also conducted to account for the FF and PCE degradation for both electrodes and to match the experimental data. Therefore, the lower FF and PCE of the OSC with a polymer electrode directly resulted from the higher sheet resistance of the polymer electrode and the corresponding higher series resistance.

Enhanced interfacial characteristics of perovskite solar cell with multi-functional organic hole-selective interlayer

In solution-processed organic and inorganic halide perovskite solar cells (PSCs), managing the interfacial characteristics between multi-layers has been a crucial factor in determining their performance and stability. Here, we newly design an indolocarbazole-based organic molecule that can enhance the interfacial properties between a solution-processed NiOx hole transport layer and perovskite in p-i-n planar PSC. Especially, to be beneficial to this architecture, its visible transparency and energy level are optimized, and its chemical structure is crosslinked for better solution processability as a hole-selective interlayer. More importantly, it can passivate the defects in the perovskite film, consequently enhancing the quality of the film and suppressing non-radiative recombination in the devices. With this interface modification, we confirm that the performance and stability of PSC devices are largely enhanced.