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.

Single-junction solar cells are principally limited in performance by two factors (Figure 1a). Electrons excited by photons with energy higher than the bandgap relax to the band edges, releasing surplus energy as heat (thermalization loss). Photons with energy lower than the bandgap are not absorbed (transmission loss). These losses can be alleviated with two or more absorber layers. The first layer should feature a wide bandgap material to reduce the thermalization loss for high-energy photons. The second layer should have a lower bandgap to absorb the low-energy photons that pass the first layer. In such configuration a tandem cell provides less thermalization and less transmission losses than each of the corresponding single-junction cells. In the detailed-balance limit, a double-junction (tandem) cell can reach an efficiency of 42% and a triple-junction cell 49%. [6] To construct a tandem cell, the two complementary absorber layers must be stacked optically and electrically ( Figure 1b). The interconnecting layer (ICL) between the two subcells must pass light and sustain the photocurrent by providing an optically transparent electrical contact for recombination of electrons and holes from the adjacent photoactive layers. The Fermi level of the hole-transporting layer (HTL) and the electron-transporting layer (ETL) that jointly form the ICL must match the relevant highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels in the adjacent photoactive layers (Figure 1b). The ICL should not cause voltage losses and have low resistance. The open-circuit voltage (V OC ) of the tandem solar cell is ideally the sum of the V OC s of the subcells and the photocurrent is limited by the subcell generating less current. To overcome the intrinsic performance limits of single-junction cells, the subcells should absorb complementary regions of the solar spectrum and generate equal photocurrent.In the first organic tandem solar cells, materials were thermally evaporated. Initially only metal clusters were used to interconnect the subcells, [7][8][9] later complemented by p-and n-doped organic transport layers. [10,11] In 2007, the first fully solution-processed tandem polymer solar cells were reported by Gilot et al. [12] and Kim et al. [13] In both examples the ICL featured a layer of poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) as HTL, stacked on top of either a zinc oxide or a titanium oxide layer as ETL. Kim et al. achieved a PCE of 6.5%. Since then PCEs have steadily increased. Major improvements involved the use of more efficient photoactive blends that afford a high V OC relative to their optical bandgap The efficiency of organic solar cells can benefit from multijunction device architectures, in which energy losses are substantially reduced. Herein, recent developments in the field of solution-processed multijunction organic solar cells are described. Recently, various strategies have been investigated and implemented to improve the performance of these device...

In very recent years, growing efforts have been devoted to the development of all‐polymer solar cells (all‐PSCs). One of the advantages of all‐PSCs over the fullerene‐based PSCs is the versatile design of both donor and acceptor polymers which allows the optimization of energy levels to maximize the open‐circuit voltage (Voc). However, there is no successful example of all‐PSCs with both high Voc over 1 V and high power conversion efficiency (PCE) up to 8% reported so far. In this work, a combination of a donor polymer poly[4,8‐bis(5‐(2‐octylthio)thiophen‐2‐yl)benzo[1,2‐b:4,5‐b′]dithiophene‐2,6‐diyl‐alt‐(5‐(2‐ethylhexyl)‐4H‐thieno[3,4‐c]pyrrole‐4,6(5H)‐dione)‐1,3‐diyl] (PBDTS‐TPD) with a low‐lying highest occupied molecular orbital level and an acceptor polymer poly[[N,N′‐bis(2‐octyldodecyl)‐naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐thiophene‐2,5‐diyl] (PNDI‐T) with a high‐lying lowest unoccupied molecular orbital level is used, realizing high‐performance all‐PSCs with simultaneously high Voc of 1.1 V and high PCE of 8.0%, and surpassing the performance of the corresponding PC71BM‐based PSCs. The PBDTS‐TPD:PNDI‐T all‐PSCs achieve a maximum internal quantum efficiency of 95% at 450 nm, which reveals that almost all the absorbed photons can be converted into free charges and collected by electrodes. This work demonstrates the advantages of all‐PSCs by incorporating proper donor and acceptor polymers to boost both Voc and PCEs.

Photovoltaic retinal prostheses show great potential to restore sight in patients suffering from degenerative eye diseases by electrical stimulation of the surviving neurons in the retinal network. Herein, organic photodiodes (OPDs) sensitive to near‐infrared (NIR) light are evaluated as photovoltaic pixels for future application in retinal prostheses. Single‐junction and tandem OPDs are compared. In the latter, two nominally identical single‐junction cells are processed on top of each other, effectively doubling the open‐circuit voltage (V OC). Both single‐junction and tandem OPD micropixels can deliver the required charge to stimulate neurons under pulsed NIR light at physiologically safe intensities when connected to stimulating microelectrodes in a physiological saline solution. However, only tandem OPD pixels can cover the entire charge per pulse neural stimulation window due to their higher V OC (≈1.4 V). This demonstrates the viability of high‐resolution retinal prostheses based on flexible OPD arrays.

Diketopyrrolopyrrole (DPP)‐conjugated polymers are a versatile class of semiconductors for application in organic solar cells because of their tunable optoelectronic properties. A record power conversion efficiency (PCE) of 9.4% was recently achieved for DPP polymers, but further improvements are required to reach true efficiency limits. Using five DPP polymers with different chemical structures and molecular weights, the device performance of polymer:fullerene solar cells is systematically optimized by considering device polarity, morphology, and light absorption. The polymer solubility is found to have a significant effect on the optimal device polarity. Soluble polymers show a 10–25% increase in PCE in inverted device configurations, while the device performance is independent of device polarity for less soluble DPP derivatives. The difference seems related to the polymer to fullerene weight ratio at the ZnO interface in inverted devices, which is higher for more soluble DPP polymers. Optimization of the nature of the cosolvent to narrow the fibril width of polymers in the blends toward the exciton diffusion length enhances charge generation. Additionally, the use of a retroreflective foil increases absorption of light. Combined, the effects afford a PCE of 9.6%, among the highest for DPP‐based polymer solar cells.