shuhui

A semitransparent photovoltaic (ST‐PV) with a tandem architecture and selective absorption in invisible regions is designed. By developing highly efficient active layers that selective absorb in the UV and near‐infrared regions and designing an appropriate interconnecting layer and transparent electrode, the resulting tandem ST‐PV device exhibits light utilization efficiency of 5.7% with averaged visible transmittance (AVT) of 52.9% and power conversion efficiency up to 10.7%.

Abstract

Semitransparent (ST) photovoltaics (PVs) with selective absorption in the UV or/and near‐infrared (NIR) range(s) and reduced energy losses, are critical for high‐efficiency solar‐window applications. Here, a high‐performance tandem ST‐PV with selected absorption in the desirable regions of the solar spectrum is demonstrated. An ultralarge‐bandgap perovskite film (FAPbBr_2.43Cl_0.57, E _g ≈ 2.36 eV) is first developed to fulfil efficient selective absorption in the UV region. After optimization, the corresponding ST single junction (SJ) PV exhibits an averaged transmittance (AVT) of ≈68% and an efficiency of ≈7.5%. By sequentially reducing the visible absorbing component in a low‐bandgap organic bulk‐heterojunction layer, an ST‐PV with selective absorption in the NIR is achieved with a power conversion efficiency (PCE) of 5.9% and a high AVT of 62%. The energy loss associated with the SJ ST‐PVs is further reduced with a tandem architecture, which affords a high PCE of 10.7%, an AVT of 52.91%, and a light utilization efficiency up to 5.66%. These results represent the best balance of AVT and PCE among all ST‐PVs reported so far, and this design should pave the road for solar windows of high performance.

A semitransparent photovoltaic (ST‐PV) with a tandem architecture and selective absorption in invisible regions is designed. By developing highly efficient active layers that selective absorb in the UV and near‐infrared regions and designing an appropriate interconnecting layer and transparent electrode, the resulting tandem ST‐PV device exhibits light utilization efficiency of 5.7% with averaged visible transmittance (AVT) of 52.9% and power conversion efficiency up to 10.7%.

Abstract

Semitransparent (ST) photovoltaics (PVs) with selective absorption in the UV or/and near‐infrared (NIR) range(s) and reduced energy losses, are critical for high‐efficiency solar‐window applications. Here, a high‐performance tandem ST‐PV with selected absorption in the desirable regions of the solar spectrum is demonstrated. An ultralarge‐bandgap perovskite film (FAPbBr_2.43Cl_0.57, E _g ≈ 2.36 eV) is first developed to fulfil efficient selective absorption in the UV region. After optimization, the corresponding ST single junction (SJ) PV exhibits an averaged transmittance (AVT) of ≈68% and an efficiency of ≈7.5%. By sequentially reducing the visible absorbing component in a low‐bandgap organic bulk‐heterojunction layer, an ST‐PV with selective absorption in the NIR is achieved with a power conversion efficiency (PCE) of 5.9% and a high AVT of 62%. The energy loss associated with the SJ ST‐PVs is further reduced with a tandem architecture, which affords a high PCE of 10.7%, an AVT of 52.91%, and a light utilization efficiency up to 5.66%. These results represent the best balance of AVT and PCE among all ST‐PVs reported so far, and this design should pave the road for solar windows of high performance.

A poly(3,4‐ethylenedioxythiophene)‐free and indium tin oxide (ITO)‐free junction‐free AgNN electrode with high optoelectrical properties is proposed for flexible organic solar cells (FOSCs). The electrical sheet resistance and optical transmittance can be controlled by both initial metal thickness and NN density; even a very thin Ag layer with appropriate NN density can show high transmittance and low sheet resistance, yielding a highly efficient FOSC.

Abstract

A novel approach to fabricate flexible organic solar cells is proposed without indium tin oxide (ITO) and poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) using junction‐free metal nanonetworks (NNs) as transparent electrodes. The metal NNs are monolithically etched using nanoscale shadow masks, and they exhibit excellent optoelectronic performance. Furthermore, the optoelectrical properties of the NNs can be controlled by both the initial metal layer thickness and NN density. Hence, with an extremely thin silver layer, the appropriate density control of the networks can lead to high transmittance and low sheet resistance. Such NNs can be utilized for thin‐film devices without planarization by conductive materials such as PEDOT:PSS. A highly efficient flexible organic solar cell with a power conversion efficiency (PCE) of 10.6% and high device yield (93.8%) is fabricated on PEDOT‐free and ITO‐free transparent electrodes. Furthermore, the flexible solar cell retains 94.3% of the initial PCE even after 3000 bending stress tests (strain: 3.13%).

The factors affecting the V _OC in 2D perovskite cells with different [PbI₆]⁴⁻ layer sheets (n = 2–4) are elucidated. Nonradiative recombination at the perovskite/C₆₀ interface is found to dominate except for the n = 2 system where the bulk recombination determines the properties of the cell. Substantial V _OC gains through suppression of interfacial recombination at the top interface are expected.

Abstract

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)₃NH₃)₂(CH₃NH₃) _{n −1}Pb _n I_{3 n +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/C₆₀ 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.

Steric hindrance of side chains is purposely introduced in the design of planar nonfullerene acceptors. Compared with IDTT2F bearing bare thiophene bridge unit, IDTCN‐C, IDTCN‐O, and IDTCN‐S with alkyl, alkoxyl, and alkylthio substituted thiophene bridge units, all display favorable face‐on orientation and strong crystallinity. An excellent power conversion efficiency of 13.28% based on PBDB‐T:IDTCN‐O is achieved without any additives or annealing treatments.

Abstract

A series of alkyl, alkoxyl, and alkylthio substituted A–π–D–π–A type nonfullerene acceptors (NFAs) IDTCN‐C, IDTCN‐O, and IDTCN‐S are designed and synthesized. The introduction of a lateral side chain at the outer position of the π bridge unit can endow the terminal moiety with a confined planar conformation due to the steric hindrance. Thus, compared with nonsubstituted NFA (IDTT2F), these acceptors tend to form favorable face‐on orientation and exhibit strong crystallinity as verified with grazing‐incidence wide‐angle X‐ray scattering measurement. Moreover, the variation of side chain can significantly change the lowest unoccupied molecular orbital (LUMO) energy level of acceptors. As state‐of‐the‐art NFAs, a power conversion efficiency of 13.28% (V _oc = 0.91 V, J _sc = 19.96 mA cm⁻², and FF = 73.2%) is obtained for the as‐cast devices based on IDTCN‐O, which is among the highest value reported in literature. The excellent photovoltaic performance for IDTCN‐O can be attributed to its slightly up‐shifted LUMO level and more balanced charge transport. This research demonstrates side chain engineering is an effective way to achieve high efficiency organic solar cells.

Novel CsPbI₃ perovskite quantum dots (QDs) are prepared by ligand exchange with 2‐aminoethanethiol (AET), which shows excellent carrier mobility and stability against moisture and ultraviolet light. Photodetectors based on the AET‐CsPbI₃ QD films exhibit remarkable performance and excellent storage as well as thermal and photo stability without any encapsulation.

Abstract

A surface engineering strategy aimed at improving the stability of CsPbI₃ perovskite quantum dots (QDs) both in solution and as films is demonstrated, by performing partial ligand exchange with a short chain ligand, 2‐aminoethanethiol (AET), in place of the original long chain ligands, oleic acid (OA) and oleylamine (OAm), used in synthesis. This results in the formation of a compact ligand barrier around the particles, which prevents penetration of water molecules and thus degradation of the films and, in addition, at the same time improves carrier mobility. Moreover, the AET ligand can passivate surface traps of the QDs, leading to an enhanced photoluminescence (PL) efficiency. As a result, AET‐CsPbI₃ QDs maintain their optical performance both in solution and as films, retaining more than 95% of the initial PL intensity in water after 1 h, and under ultraviolet irradiation for 2 h. Photodetectors based on the AET‐CsPbI₃ QD films exhibit remarkable performance, such as high photoresponsivity (105 mA W⁻¹) and detectivity (5 × 10¹³ Jones at 450 nm and 3 × 10¹³ Jones at 700 nm) without an external bias. The photodetectors also show excellent stability, retaining more than 95% of the initial responsivity in ambient air for 40 h without any encapsulation.

The thermal degradation in solar‐grade silicon can be delayed by utilizing a prefabrication annealing step. Based on this, a high‐efficiency solar cell process is modified by selecting a single‐boron diffusion step and applying phosphorus‐doped polycrystalline films as electron‐selective contacts with excellent impurity‐gettering properties which result in a solar cell with a conversion efficiency of 22.6%.

Czochralski (Cz)‐grown upgraded metallurgical‐grade (UMG) silicon wafers degrade significantly during high‐temperature processes, eroding their appeal as a low‐cost alternative to conventional electronic‐grade silicon wafers. However, the thermal degradation in UMG wafers can be delayed by utilizing a prefabrication annealing step. Based on this, a high‐efficiency solar‐cell process is modified by selecting a single‐boron diffusion step and applying phosphorus‐doped polycrystalline films as electron‐selective contacts with excellent impurity‐gettering properties to minimize the thermal budget. The application of this modified high‐efficiency solar‐cell process to n‐type UMG‐Cz wafers results in a solar cell with a conversion efficiency of 22.6% on a cell area of 2 × 2 cm².

Self‐assembled monolayers (SAMs) in perovskite solar cells are summarized comprehensively herein. SAMs play significant roles such as boosting the optoelectronic properties and improving perovskite stability. An overview of SAM modification in perovskite solar cells and state‐of‐the‐art applications is provided. Finally, the remaining challenges and outlooks for future research are presented.

Perovskite solar cells (PSCs) are considered as potential candidates for next‐generation energy harvesting due to their advantages. A classic PSC has two charge transport layers (CTLs) above and below a perovskite layer, and these CTLs largely influence charge extraction and transport. Thus, an interface inevitably forms between the CTL and perovskite layer, and if the CTL and perovskite do not form a compact contact, these interfaces can become a nonradiative recombination center, which can degrade device efficiency and stability. Accordingly, interface engineering is considered an effective way to alleviate this issue. Herein, an overview of interface engineering methods on PSCs is provided, particularly with regard to types of self‐assembled monolayers and their roles in device energy level alignment and passivation effects.

Planar perovskite solar cells (PSCs) are promising photovoltaic devices accompanied with the obvious advantages of easy fabrication and scalability. Herein, a method toward obtaining high‐quality FA_1–x MA _x PbI₃ film‐based planar PSCs by sequential deposition of chlorobenzene and methylammonium chloride is proposed. A champion power conversion efficiency (PCE) of 18.57% is achieved and 91% of the initial PCE is maintained after 500 h.

Planar perovskite solar cells (PSCs) are promising photovoltaic devices accompanied with the obvious advantages of easy fabrication and scalability. To achieve highly efficient and stable PSCs, the morphology control of perovskite crystallization is crucial. Herein, a novel method toward obtaining high‐quality FA_1–x MA _x PbI₃ films by spin coating methylammonium chloride (MACl) and chlorobenzene (CB) in different sequential processes on the top of substrates is proposed. Controlling the nucleation process is beneficial for the formation of a homogeneous nucleus at the nucleation stage, leading to highly ordered seed crystals and an ultrasmooth perovskite film. As determined by photoluminescence and time‐resolved photoluminescence spectroscopy, the defects and the associated charge recombination are notably reduced by the high crystalline quality of perovskite film. Finally, a champion power conversion efficiency (PCE) of 18.57% is achieved and 91% of the initial PCE is retained after 500 h. The devices are stored in an ambient condition with 20% relative humidity (RH) at 30 °C in the dark.

Forming CH₃NH₃PbI₃/SnO₂ interfaces not only weakens the gap states induced by CH₃NH₃PbI₃ surfaces but also enhances the band offset compared to CH₃NH₃PbI₃/TiO₂ interfaces. Moreover, the interfacial properties are dependent on the interface atomic configurations. CH₃NH₃PbI₃/SnO₂ interface with PbI and SnO terminations is the most stable model, while that with PbI and O terminations exhibits the best interfacial charge transport efficiency.

Abstract

Understanding the interfacial properties of perovskite/SnO₂ interface is important for perovskite solar cell design and optimization. Here, interfacial structure and transport properties of CH₃NH₃PbI₃/SnO₂ interfaces are investigated comprehensively by density functional theory and experiment. Forming CH₃NH₃PbI₃/SnO₂ interfaces weakens the gap states induced by CH₃NH₃PbI₃ surfaces. The interfacial transport properties are strongly dependent on the interface atomic configurations. The CH₃NH₃PbI₃/SnO₂ interface with PbI and O terminations is more beneficial for hole blocking and electron transporting due to the largest valence band offset compared to the CH₃NH₃PbI₃/SnO₂ interface with other terminations. Moreover, it exhibits a larger electrostatic potential difference compared with CH₃NH₃PbI₃/TiO₂ interface, leading to the higher electron transfer efficiency. Hence, higher power conversion efficiency is achieved based on CH₃NH₃PbI₃/SnO₂ compared to CH₃NH₃PbI₃/TiO₂ structure in experiments. In addition, CH₃NH₃PbI₃/SnO₂ interfaces with PbI terminations are more stable than those with CH₃NH₃I terminations, suggesting PbI₂ layer may be preferentially formed on SnO₂ substrate during CH₃NH₃PbI₃ fabrication process. Such results could provide a useful understanding on CH₃NH₃PbI₃/SnO₂ interface and contribute to new strategies for the interface optimization.

Spiro‐OMeTAD(TFSI)₂ is successfully employed in the fabrication of highly efficient n–i–p perovskite solar cells as a p‐dopant in the absence of lithium bis(trifluoromethane)sulfonimide (LiTFSI) and air exposure. With this approach, the proportion of [spiro‐OMeTAD]⁺ is precisely controlled, and the spiro‐OMeTAD(TFSI)₂‐doped devices show a remarkably improved long‐term stability and well‐retained hole‐transporting material (HTM) morphology after aging for 300 h.

Abstract

To date, the most efficient perovskite solar cells (PSCs) employ an n–i–p device architecture that uses a 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenyl‐amine)‐9,9′‐spirobifluorene (spiro‐OMeTAD) hole‐transporting material (HTM), which achieves optimum conductivity with the addition of lithium bis(trifluoromethane)sulfonimide (LiTFSI) and air exposure. However, this additive along with its oxidation process leads to poor reproducibility and is detrimental to stability. Herein, a dicationic salt spiro‐OMeTAD(TFSI)₂, is employed as an effective p‐dopant to achieve power conversion efficiencies of 19.3% and 18.3% (apertures of 0.16 and 1.00 cm²) with excellent reproducibility in the absence of LiTFSI and air exposure. As far as it is known, these are the highest‐performing n–i–p PSCs without LiTFSI or air exposure. Comprehensive analysis demonstrates that precise control of the proportion of [spiro‐OMeTAD]⁺ directly provides high conductivity in HTM films with low series resistance, fast hole extraction, and lower interfacial charge recombination. Moreover, the spiro‐OMeTAD(TFSI)₂‐doped devices show improved stability, benefitting from well‐retained HTM morphology without forming aggregates or voids when tested under an ambient atmosphere. A facile approach is presented to fabricate highly efficient PSCs by replacing LiTFSI with spiro‐OMeTAD(TFSI)₂. Furthermore, this study provides an insight into the relationship between device performance and the HTM doping level.

Hysteresis in the dark, attributable to bias induced degradation of the p‐type interface, is investigated and eliminated in NiO‐based inverted perovskite solar cells. Enhanced stability to forward bias is obtained with the introduction of a low‐temperature hybrid magnesium‐based interlayer.

Abstract

In perovskite solar cells (PSCs), the interfaces are a weak link with respect to degradation. Electrochemical reactivity of the perovskite's halides has been reported for both molecular and polymeric hole selective layers (HSLs), and here it is shown that also NiO brings about this decomposition mechanism. Employing NiO as an HSL in p–i–n PSCs with power conversion efficiency (PCE) of 16.8%, noncapacitive hysteresis is found in the dark, which is attributable to the bias‐induced degradation of perovskite/NiO interface. The possibility of electrochemically decoupling NiO from the perovskite via the introduction of a buffer layer is explored. Employing a hybrid magnesium‐organic interlayer, the noncapacitive hysteresis is entirely suppressed and the device's electrical stability is improved. At the same time, the PCE is improved up to 18% thanks to reduced interfacial charge recombination, which enables more efficient hole collection resulting in higher V _oc and FF.

Imaging and mapping characterization techniques are used to understand the fundamental properties that allow lead halide perovskites to have excellent performance metrics. In this work, commonly‐used and specialized tools that are used characterize halide perovskite materials and solar cells, including electron microscopy, atomic force microscopy, synchrotron‐based X‐ray mapping, and ultrafast and photoluminescence mapping are reviewed.

Abstract

Perovskite solar cells (PSCs) have attracted much attention as efficiencies have gone beyond 24%. To achieve these impressive numbers, the PSC scientific community is working to improve the perovskite optoelectronic properties. Imaging and mapping characterization techniques have been widely used to understand the fundamental properties that allow lead halide perovskites to achieve high performance. In this review, these techniques are evaluated, from simple tools, such as electron microscopy, to more complex systems that include atomic force microscopy, synchrotron‐based X‐ray mapping, and ultrafast and photoluminescence mapping. These tools have helped understand lead halide perovskites and their impressive optoelectronic properties, which make them outstanding materials for solar cell applications.

A meta‐alkoxylphenylated dithieno[3,2‐b:2′,3′‐d]pyrrol‐fused nonfullerene acceptor, featuring predominant face‐on orientation in films, enables high‐efficiency as‐cast thick organic solar cells (OSCs). Binary blends with PBDB‐T contributes to a 12.1% power conversion efficiency. Addition of 15 wt% PC₇₁BM renders an efficiency of 14%, among the records for as‐cast single‐junction OSCs. All devices exhibit thickness insensitivity in an active layer thickness window of 82–202 nm.

Abstract

Molecular orientation and π–π stacking of nonfullerene acceptors (NFAs) determine its domain size and purity in bulk‐heterojunction blends with a polymer donor. Two novel NFAs featuring an indacenobis(dithieno[3,2‐b:2ʹ,3ʹ‐d]pyrrol) core with meta‐ or para‐alkoxyphenyl sidechains are designed and denoted as m‐INPOIC or p‐INPOIC, respectively. The impact of the alkoxyl group positioning on molecular orientation and photovoltaic performance of NFAs is revealed through a comparison study with the counterpart (INPIC‐4F) bearing para‐alkylphenyl sidechains. With inward constriction toward the conjugated backbone, m‐INPOIC presents predominant face‐on orientation to promote charge transport. The as‐cast organic solar cells (OSCs) by blending m‐INPOIC and PBDB‐T as active layers exhibit a power conversion efficiency (PCE) of 12.1%. By introducing PC₇₁BM as the solid processing‐aid, the ternary OSCs are further optimized to deliver an impressive PCE of 14.0%, which is among the highest PCEs for as‐cast single‐junction OSCs reported in literature to date. More attractively, PBDB‐T: m‐INPOIC:PC₇₁BM based OSCs exhibit over 11% PCEs even with an active layer thickness over 300 nm. And the devices can retain over 95% of PCE after storage for 20 days. The outstanding tolerance to film thickness and outstanding stability of the as‐cast devices make m‐INPOIC a promising candidate NFA for large‐scale solution‐processable OSCs.

The sp²‐nitrogen positions in the n‐type (D–A₁–D–A₂) conjugated polymers have a significant impact on the photovoltaic properties of p–i–n perovskite solar cells when they are used as an electron transporting layer. pBTTz with the HOMO and LUMO levels well‐matched with the valence and conduction bands of the perovskite layer, respectively, shows excellent power conversion efficiency and high stability.

Abstract

It is highly desirable to employ n‐type polymers as electron transporting layers (ETLs) in inverted perovskite solar cells (PSCs) due to their good electron mobility, high hydrophobicity, and simplicity of film forming. In this research, the capability of three n‐type donor–acceptor₁–donor–acceptor₂ (D–A₁–D–A₂) conjugated polymers (pBTT, pBTTz, and pSNT) is first explored as ETLs because these polymers possess electron mobilities as high as 0.92, 0.46, and 4.87 cm² (Vs)⁻¹ in n‐channel organic transistors, respectively. The main structural difference among pBTT, pBTTz, and pSNT is the position of sp²‐nitrogen atoms (sp²‐N) in the polymer main chains. Therefore, the effect of different substitution positions on the PSC performances is comprehensively studied. The as‐fabricated p–i–n PSCs with pBTT, pBTTz, and pSNT as ETLs show the maximum photoconversion efficiencies of 12.8%, 14.4%, and 12.0%, respectively. To be highlighted, pBTTz‐based device can maintain 80% of its stability after ten days due to its good hydrophobicity, which is further confirmed by a contact angle technique. More importantly, the pBTTz‐based device shows a neglected hysteresis. This study reveals that the n‐type polymers can be promising candidates as ETLs to approach solution‐processed highly‐efficient inverted PSCs.

Carbon‐electrode based perovskite solar cells (CPSCs) are well known for their low cost and sound stability. However, the highest power conversion efficiency of these devices is only about 70% of that demonstrated by metal electrode‐based PSCs, leaving a gap of about 30%. Bulk engineering and interface engineering is helpful in narrowing the gap. Herein, these two strategies are summarized for CPSCs.

Carbon electrodes have been adopted widely in perovskite solar cells (PSCs). Due to its suitable work function (though not high enough), the carbon electrode itself could extract photogenerated holes and has helped to achieve a power conversion efficiency of ≈16% in the absence of hole‐transporting material. Meanwhile, due to the inert chemical nature and the micrometer‐sized film thickness (≈10 μm), carbon electrodes can prolong the stability of PSCs. These merits are appealing for the commercialization of PSCs. However, the efficiency of carbon‐electrode PSCs is relatively low. A gap of ≈30% remains when comparing with PSCs using evaporated metal films as the electrode. Herein, the progresses in the efficiency of the four kinds of carbon‐electrode based PSCs (mesoscopic, embedment, planar, and quasi‐planar) are reviewed and compared to metal‐electrode based PSCs. Then, the role of bulk engineering and interface engineering in the progress of efficiency is discussed. Finally, outlooks are described in accordance with the discussions.

Here, studies on regulation of the interfacial charge balance in SnO₂‐based planar perovskite solar cells are reported. SnO₂ with optimum thickness exhibits enhanced charge balance. Moreover, trap‐assisted carrier recombination is significantly suppressed by using diethylenetriaminepentaacetic acid as a passivator. As a result, the champion device demonstrates a promising efficiency of 21.28% with negligible hysteresis and much improved environmental stability.

Control of dynamics at the electron transport layer–perovskite interface, such as charge transfer and recombination, is essential in achieving high‐efficiency planar perovskite solar cells (PSCs). Herein, it was observed that the trade‐off between unfavorable electron transport of a thick SnO₂ film and serious electron recombination at thin SnO₂ film/perovskite interfaces is essential for the performance of SnO₂‐based planar PSCs. The optimized efficiency of devices beyond 20% is obtained by using a two‐step deposition of SnO₂. Moreover, trap‐assisted carrier recombination is significantly suppressed by using the diethylenetriaminepentaacetic acid passivator via the formation of coordination with undercoordinated Sn and Pb²⁺ ions. As a result, the champion device demonstrates a promising efficiency of 21.28% with negligible hysteresis and much improved environmental stability, i.e., retaining 98% of the initial efficiency under ambient atmosphere over 1000 h.

A meta‐alkoxylphenylated dithieno[3,2‐b:2′,3′‐d]pyrrol‐fused nonfullerene acceptor, featuring predominant face‐on orientation in films, enables high‐efficiency as‐cast thick organic solar cells (OSCs). Binary blends with PBDB‐T contributes to a 12.1% power conversion efficiency. Addition of 15 wt% PC₇₁BM renders an efficiency of 14%, among the records for as‐cast single‐junction OSCs. All devices exhibit thickness insensitivity in an active layer thickness window of 82–202 nm.

Abstract

Molecular orientation and π–π stacking of nonfullerene acceptors (NFAs) determine its domain size and purity in bulk‐heterojunction blends with a polymer donor. Two novel NFAs featuring an indacenobis(dithieno[3,2‐b:2ʹ,3ʹ‐d]pyrrol) core with meta‐ or para‐alkoxyphenyl sidechains are designed and denoted as m‐INPOIC or p‐INPOIC, respectively. The impact of the alkoxyl group positioning on molecular orientation and photovoltaic performance of NFAs is revealed through a comparison study with the counterpart (INPIC‐4F) bearing para‐alkylphenyl sidechains. With inward constriction toward the conjugated backbone, m‐INPOIC presents predominant face‐on orientation to promote charge transport. The as‐cast organic solar cells (OSCs) by blending m‐INPOIC and PBDB‐T as active layers exhibit a power conversion efficiency (PCE) of 12.1%. By introducing PC₇₁BM as the solid processing‐aid, the ternary OSCs are further optimized to deliver an impressive PCE of 14.0%, which is among the highest PCEs for as‐cast single‐junction OSCs reported in literature to date. More attractively, PBDB‐T: m‐INPOIC:PC₇₁BM based OSCs exhibit over 11% PCEs even with an active layer thickness over 300 nm. And the devices can retain over 95% of PCE after storage for 20 days. The outstanding tolerance to film thickness and outstanding stability of the as‐cast devices make m‐INPOIC a promising candidate NFA for large‐scale solution‐processable OSCs.

The sp²‐nitrogen positions in the n‐type (D–A₁–D–A₂) conjugated polymers have a significant impact on the photovoltaic properties of p–i–n perovskite solar cells when they are used as an electron transporting layer. pBTTz with the HOMO and LUMO levels well‐matched with the valence and conduction bands of the perovskite layer, respectively, shows excellent power conversion efficiency and high stability.

Abstract

It is highly desirable to employ n‐type polymers as electron transporting layers (ETLs) in inverted perovskite solar cells (PSCs) due to their good electron mobility, high hydrophobicity, and simplicity of film forming. In this research, the capability of three n‐type donor–acceptor₁–donor–acceptor₂ (D–A₁–D–A₂) conjugated polymers (pBTT, pBTTz, and pSNT) is first explored as ETLs because these polymers possess electron mobilities as high as 0.92, 0.46, and 4.87 cm² (Vs)⁻¹ in n‐channel organic transistors, respectively. The main structural difference among pBTT, pBTTz, and pSNT is the position of sp²‐nitrogen atoms (sp²‐N) in the polymer main chains. Therefore, the effect of different substitution positions on the PSC performances is comprehensively studied. The as‐fabricated p–i–n PSCs with pBTT, pBTTz, and pSNT as ETLs show the maximum photoconversion efficiencies of 12.8%, 14.4%, and 12.0%, respectively. To be highlighted, pBTTz‐based device can maintain 80% of its stability after ten days due to its good hydrophobicity, which is further confirmed by a contact angle technique. More importantly, the pBTTz‐based device shows a neglected hysteresis. This study reveals that the n‐type polymers can be promising candidates as ETLs to approach solution‐processed highly‐efficient inverted PSCs.

Nature Communications, Published online: 17 July 2019; doi:10.1038/s41467-019-11087-y