Burn‐in Free Nonfullerene‐Based Organic Solar Cells

Organic solar cells that are free of burn‐in, the commonly observed rapid performance loss under light, are presented. The solar cells are based on poly(3‐hexylthiophene) (P3HT) with varying molecular weights and a nonfullerene acceptor (rhodanine‐benzothiadiazole‐coupled indacenodithiophene, IDTBR) and are fabricated in air. P3HT:IDTBR solar cells light‐soaked over the course of 2000 h lose about 5% of power conversion efficiency (PCE), in stark contrast to [6,6]‐Phenyl C61 butyric acid methyl ester (PCBM)‐based solar cells whose PCE shows a burn‐in that extends over several hundreds of hours and levels off at a loss of ≈34%. Replacing PCBM with IDTBR prevents short‐circuit current losses due to fullerene dimerization and inhibits disorder‐induced open‐circuit voltage losses, indicating a very robust device operation that is insensitive to defect states. Small losses in fill factor over time are proposed to originate from polymer or interface defects. Finally, the combination of enhanced efficiency and stability in P3HT:IDTBR increases the lifetime energy yield by more than a factor of 10 when compared with the same type of devices using a fullerene‐based acceptor instead.     

Additive‐Free Organic Solar Cells with Power Conversion Efficiency over 10%

Nowadays, solvent additives are widely used in organic solar cells (OSCs) to tune the nano‐morphology of the active blend film and enhance the device performance. With their help, power conversion efficiencies (PCEs) of OSCs have recently stepped over 10%. However, residual additive in the device can induce undesirable morphological change and also accelerate photo‐oxidation degradation of the active blend film. Thereby, their involvements are actually unfavorable for practical applications. Here, a donor material PThBDTP is employed, and PThBDTP:PC71BM based OSCs are fabricated. A PCE of over 10% is achieved without using any additives and film post‐treatments. The device displays a high open‐circuit voltage of 0.977 V, a large short‐circuit current density of 13.49 mA cm^‐2, and a high fill factor of 76.3%. These results represent an important step towards developing high‐efficiency additive‐free OSCs.     

Overcoming Space‐Charge Effect for Efficient Thick‐Film Non‐Fullerene Organic Solar Cells

Organic solar cells (OSCs) containing non‐fullerene acceptors have realized high power conversion efficiency (PCE) up to 14%. However, most of these high‐performance non‐fullerene OSCs have been reported with optimal active layer thickness of about 100 nm, mainly due to the low electron mobility (≈10^?4–10^?5 cm² V^?1 s^?1) of non‐fullerene acceptors, which are not suitable for roll‐to‐roll large‐scale processing. In this work, an efficient non‐fullerene OSC based on 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):EH‐IDTBR (consists of electron‐rich indaceno[1,2‐b:5,6‐b′]dithiophene as the central unit and an electron‐deficient 5,6‐benzo[c][1,2,5]thiadiazole unit flanked with rhodanine as the peripheral group) with thickness‐independent PCE (maintaining a PCE of 9.1% with an active layer thickness of 300 nm) is presented by optimizing device architectures to overcome the space‐charge effects. Optical modeling reveals that most of the incident light is absorbed near the transparent electrode side in thick‐film devices. The transport distance of electrons with lower mobility will therefore be shortened when using inverted device architecture, in which most of the excitons are generated close to the cathode side and therefore substantially reduces the accumulation of electrons in the device. As a result, an efficient thick‐film non‐fullerene OSC is realized. These results provide important guidelines for the development of more efficient thick‐film non‐fullerene OSCs.     

Development of Dopant‐Free Organic Hole Transporting Materials for Perovskite Solar Cells

There has been considerable progress over the last decade in development of the perovskite solar cells (PSCs), with reported performances now surpassing 25.2% power conversion efficiency. Both long‐term stability and component costs of PSCs remain to be addressed by the research community, using hole transporting materials (HTMs) such as 2,2′,7,7′‐tetrakis(N,N′‐di‐pmethoxyphenylamino)‐9,9′‐spirbiuorene(Spiro‐OMeTAD) and poly[bis(4‐phenyl)(2,4,6‐trimethylphenyl)amine] (PTAA). HTMs are essential for high‐performance PSC devices. Although effective, these materials require a relatively high degree of doping with additives to improve charge mobility and interlayer/substrate compatibility, introducing doping‐induced stability issues with these HTMs, and further, additional costs and experimental complexity associated with using these doped materials. This article reviews dopant‐free organic HTMs for PSCs, outlining reports of structures with promising properties toward achieving low‐cost, effective, and scalable materials for devices with long‐term stability. It summarizes recent literature reports on non‐doped, alternative, and more stable HTMs used in PSCs as essential components for high‐efficiency cells, categorizing HTMs as reported for different PSC architectures in addition to use of dopant‐free small molecular and polymeric HTMs. Finally, an outlook and critical assessment of dopant‐free organic HTMs toward commercial application and insight into the development of stable PSC devices is provided.     

Toward High‐Temperature Stability of PTB7‐Based Bulk Heterojunction Solar Cells: Impact of Fullerene Size and Solvent Additive

The use of fullerene as acceptor limits the thermal stability of organic solar cells at high temperatures as their diffusion inside the donor leads to phase separation via Ostwald ripening. Here it is reported that fullerene diffusion is fully suppressed at temperatures up to 140 °C in bulk heterojunctions based on the benzodithiophene‐based polymer (the poly[[4,8‐bis[(2‐ethylhexyl)oxy]‐benzo[1,2‐b:4,5‐b′]dithiophene‐2,6‐diyl][3‐fluoro‐2‐[(2‐ethylhexyl)carbonyl]‐thieno[3,4‐b]thiophenediyl]], (PTB7) in combination with the fullerene derivative [6,6]‐phenyl‐C71‐butyric acid methyl ester (PC₇₀BM). The blend stability is found independently of the presence of diiodooctane (DIO) used to optimize nanostructuration and in contrast to PTB7 blends using the smaller fullerene derivative PC₇₀BM. The unprecedented thermal stability of PTB7:PC₇₀BM layers is addressed to local minima in the mixing enthalpy of the blend forming stable phases that inhibit fullerene diffusion. Importantly, although the nanoscale morphology of DIO processed blends is thermally stable, corresponding devices show strong performance losses under thermal stress. Only by the use of a high temperature annealing step removing residual DIO from the device, remarkably stable high efficiency solar cells with performance losses less than 10% after a continuous annealing at 140 °C over 3 days are obtained. These results pave the way toward high temperature stable polymer solar cells using fullerene acceptors.     

ITO‐Free and Fully Solution‐Processed Semitransparent Organic Solar Cells with High Fill Factors

Organic photovoltaic (OPV) solar cells that can be simply processed from solution are in the focus of the academic and industrial community because of their enormous potential to reduce cost. One big challenge in developing a fully solution‐processed OPV technology is the design of a well‐performing electrode system, allowing the replacement of ITO. Several solution‐processed electrode systems were already discussed, but none of them could match the performance of ITO. Here, we report efficient ITO‐free and fully solution‐processed semitransparent inverted organic solar cells based on silver nanowire (AgNW) electrodes. To demonstrate the potential of these AgNW electrodes, they were employed as both the bottom and top electrodes. Record devices achieved fill factors as high as 63.0%, which is comparable to ITO based reference devices. These results provide important progress for fully printed organic solar cells and indicate that ITO‐free, transparent as well as non‐transparent organic solar cells can indeed be fully solution‐processed without losses.     

Reverse‐Graded 2D Ruddlesden–Popper Perovskites for Efficient Air‐Stable Solar Cells

2D Ruddlesden–Popper perovskites (RPPs) have emerged as a promising solar cell material. A group of novel RPPs with cyclohexane methylamine (CMA) as a spacer cation is presented. Unlike previously reported RPPs, the deposited films of (CMA)₂(MA)_n?1Pb_nI_3n+1 (MA is CH₃NH₃⁺, n = 1, 2, 3, …) exhibit multiple phases with reverse‐graded quantum well (QW) distribution; small n (n = 2) RPPs are located at the surface and large n (n ≥ 10) RPPs at the bottom. This has three advantages: (a) The outer, more moisture resistant, small n RPPs create a stable barrier that protects the vulnerable large n RPP lattice from being attacked by water molecules. (b) It forms a type‐II band alignment between different phases, which favors self‐driven charge transport. (c) The natural structure of graded QWs expands the range of photon collection. Attributed to these properties, the best efficiency of 15.05%, with high open‐circuit voltage (V_oc) of 1.10 V for a first‐generation solar cell containing (CMA)₂(MA)₈Pb₉I₂₈, is achieved. A notable enhancement in short wavelength is observed in the Incident photon‐to‐current conversion efficiency spectra. This device shows significantly improved long‐term stability, retaining ≈95% of the initial efficiency after 4600 h exposure in ambient conditions with 40–70% relative humidity.     

High‐Performance and Stable All‐Polymer Solar Cells Using Donor and Acceptor Polymers with Complementary Absorption

To explore the advantages of emerging all‐polymer solar cells (all‐PSCs), growing efforts have been devoted to developing matched donor and acceptor polymers to outperform fullerene‐based PSCs. In this work, a detailed characterization and comparison of all‐PSCs using a set of donor and acceptor polymers with both conventional and inverted device structures is performed. A simple method to quantify the actual composition and light harvesting contributions from the individual donor and acceptor is described. Detailed study on the exciton dissociation and charge recombination is carried out by a set of measurements to understand the photocurrent loss. It is unraveled that fine‐tuned crystallinity of the acceptor, matched donor and acceptor with complementary absorption and desired energy levels, and device architecture engineering can synergistically boost the performance of all‐PSCs. As expected, the PBDTTS‐FTAZ:PNDI‐T10 all‐PSC attains a high and stable power conversion efficiency of 6.9% without obvious efficiency decay in 60 d. This work demonstrates that PNDI‐T10 can be a potential alternative acceptor polymer to the widely used acceptor N2200 for high‐performance and stable all‐PSCs.     

Scaling Up ITO‐Free Solar Cells

Indium‐tin‐oxide‐free (ITO‐free) polymer solar cells with composite electrodes containing current‐collecting grids and a semitransparent poly(3,4‐ethylenedioxythiophene):polystyrenesulfonate) (PEDOT:PSS) conductor are demonstrated. The up‐scaling of the length of the solar cell from 1 to 6 cm and the effect of the grid line resistance are explored for a series of devices. Laser‐beam‐induced current (LBIC) mapping is used for quality control of the devices. A theoretical modeling study is presented that enables the identification of the most rational cell dimension for the grids with different resistances. The performance of ITO‐free organic solar cells with different dimensions and different electrode resistances are evaluated for different light intensities. The current generation and electric potential distribution are found to not be uniformly distributed in large‐area devices at simulated 1 Sun illumination. The generated current uniformity increases with decreasing light intensities.     

Tailoring Organic Cation of 2D Air‐Stable Organometal Halide Perovskites for Highly Efficient Planar Solar Cells

2D perovskites have recently been shown to exhibit significantly improved environmental stability. Derived from their 3D analogues, 2D perovskites are formed by inserting bulky alkylammonium cations in‐between the anionic layers. However, these insulating organic spacer cations also hinder charge transport. Herein, such a 2D perovskite, (iso‐BA)₂(MA)₃Pb₄I₁₃, that contains short branched‐chain spacer cations (iso‐BA⁺) and shows a remarkable increase of optical absorption and crystallinity in comparison to the conventional linear one, n‐BA⁺, is designed. After applying the hot‐casting (HC) technique, all these properties are further improved. The HC (iso‐BA)₂(MA)₃Pb₄I₁₃ sample exhibits the best ambient stability by maintaining its initial optical absorption after storage of 840 h in an environmental chamber at 20 °C with a relative humidity of 60% without encapsulation. More importantly, the out‐of‐plane crystal orientation of (iso‐BA)₂(MA)₃Pb₄I₁₃ film is notably enhanced, which increases cross‐plane charge mobility. As a result, the highest power conversion efficiencies (PCEs) measured from for current density versus voltage curves afford 8.82% and 10.63% for room‐temperature and HC‐processed 2D perovskites based planar solar cells, respectively. However, the corresponding steady‐state PCEs are remarkably lower, which is presumably due to the significant hysteresis phenomena caused by low charge extraction efficiency at interfaces of C₆₀/2D perovskites.     

Nonfullerene n‐Type Organic Semiconductors for Perovskite Solar Cells

Compared to inorganic semiconductors and/or fullerene derivatives, nonfullerene n‐type organic semiconductors present some advantages, such as low‐temperature processing, flexibility, and molecule structure diversity, and have been widely used in perovskite solar cells (PSCs). In this research news article, the recent advances in nonfullerene n‐type organic semiconductors which function as electron‐transporting, interface‐modifying, additive, and light‐harvesting materials in PSCs are summarized. The remaining challenges and promising future directions of nonfullerene‐based PSCs are also discussed.     

Constructing High‐Performance Organic Photovoltaics via Emerging Non‐Fullerene Acceptors and Tandem‐Junction Structure

In consideration of the unique advantages of new non‐fullerene acceptors and the tandem‐junction structure, organic photovoltaics (OPVs) based on them are very promising. Studies related to this emerging area began in 2016 with achieved power conversion efficiencies (PCEs) of 8–10%, which have now been boosted to 17%. In this essay, the construction of high‐performance OPVs is discussed, with a focus on combining the advantages of new non‐fullerene acceptors and the tandem‐junction structure. In order to achieve higher PCEs, methods to enable high short‐circuit current density, open‐circuit voltage, and fill factor are discussed. In addition, the stability and reproducibility of high‐efficiency OPVs are also addressed. Herein, it is forecast that the new non‐fullerene acceptors‐based tandem‐junction OPVs will become the next big wave in the field and achieve high PCEs over 20% in the near future. Some promising research directions on this emerging hot topic are proposed which may further push the field into the 25% high efficiency era and considerably advance the technology beyond laboratory research.