Chen Weijie

Acetic acid (Ac) is used as an antisolvent for preparing perovskite films with excellent optoelectronic properties. Ac is found to not only reduce perovskite film roughness and residual PbI₂ but also generate a passivation effect from the electron‐rich carbonyl group. The best 0.159 cm² devices produce efficiencies of 22.0% for Cs_0.05FA_0.80MA_0.15Pb(I_0.85Br_0.15)₃ and 23.0% for Cs_0.05FA_0.90MA_0.05Pb(I_0.95Br_0.05)₃.

Abstract

Improving the quality of perovskite poly‐crystalline film is essential for the performance of associated solar cells approaching their theoretical limit efficiency. Pinholes, unwanted defects, and nonperovskite phase can be easily generated during film formation, hampering device performance and stability. Here, a simple method is introduced to prepare perovskite film with excellent optoelectronic property by using acetic acid (Ac) as an antisolvent to control perovskite crystallization. Results from a variety of characterizations suggest that the small amount of Ac not only reduces the perovskite film roughness and residual PbI₂ but also generates a passivation effect from the electron‐rich carbonyl group (CO) in Ac. The best devices produce a PCE of 22.0% for Cs_0.05FA_0.80MA_0.15Pb(I_0.85Br_0.15)₃ and 23.0% for Cs_0.05FA_0.90MA_0.05Pb(I_0.95Br_0.05)₃ on 0.159 cm² with negligible hysteresis. This further improves device stability producing a cell that maintained 96% of its initial efficiency after 2400 h storage in ambient environment (with controlled relative humidity (RH) <30%) without any encapsulation.

A new indacenothiophene‐based electron transporting material ITCP‐M with near‐infrared (NIR) absorption is developed and applied in inverted perovskite solar cells (PSCs). Interestingly, ITCP‐M can extend absorption to the NIR region in addition to electron extraction and electron transporting, which contributes to the enhanced photovoltaic performance of MAPbI₃‐based inverted PSCs.

Lead‐based organic–inorganic hybrid perovskite solar cells (PSCs) usually show an absorption edge around 800 nm, while the near‐infrared (NIR) wavelength beyond 800 nm cannot be utilized. Herein, a new indacenothiophene‐based electron transporting material (ETM), namely, ITCP‐M, is developed, which works to enhance electron extraction and electron transporting, and simultaneously extends photoresponses to the NIR region in MAPbI₃‐based inverted PSCs. Notably, the ITCP‐M‐based device exhibits a prominent photoresponse beyond 800 nm as observed from the external quantum efficiency (EQE) spectra, contributing to enhanced short‐circuit current density (J _sc) without sacrificing the open‐circuit voltage and fill factor. As a result, inverted PSCs using ITCP‐M ETM delivers a high efficiency of 19.15%, representing one of the highest efficiencies in inverted PSCs using nonfullerene ETMs. This work provides a new and simple strategy to extend photoresponses to the NIR absorption region for MAPbI₃‐based inverted PSCs that can significantly improve device performance.

The use of two precursor preparation methods for the deposition of phenethylammonium‐containing organic‐inorganic hybrid perovskite films for photovoltaic applications is reported. It is found that film properties, photovoltaic device performance, and stability differ depending on the precursor preparation methods. These new insights are important for optimizing precursor preparations for lower dimensional perovskite films to achieve the best device performance and stability.

For the fabrication of low‐dimensional perovskite solar cells, understanding the effect of precursor preparation on film formation is critical to achieve high‐quality perovskite film and, therefore, high efficiency in related solar devices. Herein, the two methods to prepare phenethylammonium‐based mixed perovskite precursors with the same chemical composition are reported. These methods are called 1) different phase (DP) and 2) same phase (SP) methods as the former involves the mixing of a 3D perovskite precursor with a 2D perovskite precursor, whereas the latter involves the mixing of quasi‐2D perovskite precursors. The films prepared by these methods are characterized by X‐ray diffraction, Kelvin probe force microscopy, and scanning electron microscopy, revealing different perovskite structures. The power conversion efficiency (PCE) of the champion cells by DP and SP methods reaches 19.1% and 18.9%, respectively. Results of the aging test show a dramatic improvement in the stability of SP perovskite devices maintaining 86% of its initial performance after exposure to a relative humidity (RH) 8 ± 5% for 1000 hr and over 80% of its initial PCE after continuous 1 sun illumination (including UV) at RH 70%. The new insights provided by this work are important to design perovskite precursor preparation methods for the best device performance and stability.

A comparative investigation of single‐donor component and different donor:acceptor blend ratio‐based organic solar cells (OSCs) is conducted using BTID‐0F as the donor and PC₇₁BM as the acceptor. The highest PCEs of 1.61% for single‐donor and 8.47% for BTID‐0F:PC₇₁BM‐based OSCs are obtained. Herein, the mechanism of charge generation in organic materials, thus obtaining high‐efficient single‐component OSCs, is analyzed.

Organic solar cells (OSCs) require a bulk heterojunction of a donor and an acceptor for efficient charge generation, whereas other types of solar cells normally use the p‐i‐n device structure. Herein, a comparative investigation of the p‐i‐n‐structured OSCs is conducted based on single‐donor‐component BTID‐0F and the bulkheterojuction OSCs with different donor:acceptor blend ratios using BTID‐0F as the donor and PC₇₁BM as the acceptor. The highest power conversion efficiency (PCE) of 1.61% is obtained for single‐donor‐based OSCs. The impact of PC₇₁BM weight ratio in BTID‐0F:PC₇₁BM‐based OSCs upon blend morphology, material energetics, photogenerated charge dynamic process, and photovoltaic device performance is investigated, and the highest PCE reaches 8.47%. Results indicate that even when the acceptor sites are highly diluted and the acceptor phase is discontinuous, electron transport can occur with a reasonable electron mobility. The PCE of 1.61% is the highest PCE reported for p‐i‐n structure OSCs based on a single‐donor component, which is helpful to understand the mechanism of charge generation in organic materials and thus obtainhigh‐efficient OSCs using the p‐i‐n structure.

Acetic acid (Ac) is used as an antisolvent for preparing perovskite films with excellent optoelectronic properties. Ac is found to not only reduce perovskite film roughness and residual PbI₂ but also generate a passivation effect from the electron‐rich carbonyl group. The best 0.159 cm² devices produce efficiencies of 22.0% for Cs_0.05FA_0.80MA_0.15Pb(I_0.85Br_0.15)₃ and 23.0% for Cs_0.05FA_0.90MA_0.05Pb(I_0.95Br_0.05)₃.

Abstract

Improving the quality of perovskite poly‐crystalline film is essential for the performance of associated solar cells approaching their theoretical limit efficiency. Pinholes, unwanted defects, and nonperovskite phase can be easily generated during film formation, hampering device performance and stability. Here, a simple method is introduced to prepare perovskite film with excellent optoelectronic property by using acetic acid (Ac) as an antisolvent to control perovskite crystallization. Results from a variety of characterizations suggest that the small amount of Ac not only reduces the perovskite film roughness and residual PbI₂ but also generates a passivation effect from the electron‐rich carbonyl group (CO) in Ac. The best devices produce a PCE of 22.0% for Cs_0.05FA_0.80MA_0.15Pb(I_0.85Br_0.15)₃ and 23.0% for Cs_0.05FA_0.90MA_0.05Pb(I_0.95Br_0.05)₃ on 0.159 cm² with negligible hysteresis. This further improves device stability producing a cell that maintained 96% of its initial efficiency after 2400 h storage in ambient environment (with controlled relative humidity (RH) <30%) without any encapsulation.

Pressure‐induced optical properties variation of lead‐free halide double perovskite (NH₄)₂SeBr₆ is strongly correlated with the re‐organization of Br‐Br bonds and the rotation and distortion of [SeBr₆]²⁻ octahedra. The structure–optical property relationship constructed here is a straightforward approach to optimize the optoelectronic properties of halide double perovskites (HDPs) and further stimulate the development of next‐generation clear energy based on HDPs solar cells.

Abstract

Lead‐free halide double perovskites (HDPs) are promising candidates for high‐performance solar cells because of their environmentally‐friendly property and chemical stability in air. The power conversion efficiency of HDPs‐based solar cells needs to be further improved before their commercialization in the market. It requires a thoughtful understanding of the correlation between their specific structure and property. Here, the structural and optical properties of an important HDP‐based (NH₄)₂SeBr₆ are investigated under high pressure. A dramatic piezochromism is found with the increase in pressure. Optical absorption spectra reveal the pressure‐induced red‐shift in bandgap with two distinct anomalies at 6.57 and 11.18 GPa, and the energy tunability reaches 360 meV within 20.02 GPa. Combined with structural characterizations, Raman and infrared spectra, and theoretical calculations using density functional theory, results reveal that, the first anomaly is caused by the formation of a Br‐Br bond among the [SeBr₆]²⁻ octahedra, and the latter is attributed to a cubic‐to‐tetragonal phase transition. These results provide a clear correlation between the chemical bonding and optical properties of (NH₄)₂SeBr₆. It is believed that the proposed strategy paves the way to optimize the optoelectronic properties of HDPs and further stimulate the development of next‐generation clear energy based on HDPs solar cells.

A polar nonconjugated small molecule ultrathin layer with an intrinsic dipole moment is introduced to modify the work function of indium tin oxide and to optimize the front interface energy level alignment, which contributes to suppressed energy loss and results in a 20.55% efficient electron transport layer–free perovskite solar cell with enhanced open‐circuit voltage short circuit current density and fill factor, simultaneously.

Abstract

Efficient electron transport layer–free perovskite solar cells (ETL‐free PSCs) with cost‐effective and simplified design can greatly promote the large area flexible application of PSCs. However, the absence of ETL usually leads to the mismatched indium tin oxide (ITO)/perovskite interface energy levels, which limits charge transfer and collection, and results in severe energy loss and poor device performance. To address this, a polar nonconjugated small‐molecule modifier is introduced to lower the work function of ITO and optimize interface energy level alignment by virtue of an inherent dipole, as verified by photoemission spectroscopy and Kelvin probe force microscopy measurements. The resultant barrier‐free ITO/perovskite contact favors efficient charge transfer and suppresses nonradiative recombination, endowing the device with enhanced open circuit voltage, short circuit current density, and fill factor, simultaneously. Accordingly, power conversion efficiency increases greatly from 12.81% to a record breaking 20.55%, comparable to state‐of‐the‐art PSCs with a sophisticated ETL. Also, the stability is enhanced with decreased hysteresis effect due to interface defect passivation and inhibited interface charge accumulation. This work facilitates the further development of highly efficient, flexible, and recyclable ETL‐free PSCs with simplified design and low cost by interface electronic structure engineering through facile electrode modification.

Chain gang: Regulating the alkyl‐chain length of quantum dots attached to inorganic CsPbBr₃ perovskites, maximizes charge extraction and transfer at the perovskite/carbon interface. The optimized inorganic CsPbBr₃ perovskite solar cell (PSC) with C₁₂ alkyl chain QDs yields an efficiency of up to 10.85 %.

Abstract

Improved charge extraction and wide spectral absorption promote power conversion efficiency of perovskite solar cells (PSCs). The state‐of‐the‐art carbon‐based CsPbBr₃ PSCs have an inferior power output capacity because of the large optical band gap of the perovskite film and the high energy barrier at perovskite/carbon interface. Herein, we use alkyl‐chain regulated quantum dots as hole‐conductors to reduce charge recombination. By precisely controlling alkyl‐chain length of ligands, a balance between the surface dipole induced charge coulomb repulsive force and quantum tunneling distance is achieved to maximize charge extraction. A fluorescent carbon electrode is used as a cathode to harvest the unabsorbed incident light and to emit fluorescent light at 516 nm for re‐absorption by the perovskite film. The optimized PSC free of encapsulation achieves a maximum power conversion efficiency up to 10.85 % with nearly unchanged photovoltaic performances under 80 %RH, 80 °C, or light irradiation in air.

Watching the defects: Defects play a pivotal role in the overall performance of perovskite solar cells. In this review, we focus on central questions of “what defects exist in metal halide perovskites” and “how can one reduce detrimental defects aiming high‐performance perovskite solar cells”.

Abstract

In several photovoltaic (PV) technologies, the presence of electronic defects within the semiconductor band gap limit the efficiency, reproducibility, as well as lifetime. Metal halide perovskites (MHPs) have drawn great attention because of their excellent photovoltaic properties that can be achieved even without a very strict film‐growth control processing. Much has been done theoretically in describing the different point defects in MHPs. Herein, we discuss the experimental challenges in thoroughly characterizing the defects in MHPs such as, experimental assignment of the type of defects, defects densities, and the energy positions within the band gap induced by these defects. The second topic of this Review is passivation strategies. Based on a literature survey, the different types of defects that are important to consider and need to be minimized are examined. A complete fundamental understanding of defect nature in MHPs is needed to further improve their optoelectronic functionalities.

Carbon dots synthesized using different ratios of common precursors citric acid and ethylenediamine are employed as interface modifiers able to adjust the work function of the indium tin oxide electrodes over the broad range, and to minimize the charge injection/extraction energy barriers in perovskite solar cells and quantum dot based light‐emitting diodes.

Abstract

Controlling the transport and minimizing charge carrier trapping at interfaces is crucial for the performance of various optoelectronic devices. Here, how electronic properties of stable, abundant, and easy‐to‐synthesized carbon dots (CDs) are controlled via the surface chemistry through a chosen ratio of their precursors citric acid and ethylenediamine are demonstrated. This allows to adjust the work function of indium tin oxide (ITO) films over the broad range of 1.57 eV, through deposition of thin CD layers. CD modifiers with abundant amine groups reduce the ITO work function from 4.64 to 3.42 eV, while those with abundant carboxyl groups increase it to 4.99 eV. Using CDs to modify interfaces between metal oxide (SnO₂ and ZnO) films and active layers of solar cells and light‐emitting diodes (LEDs) allows to significantly improve their performance. Power conversion efficiency of CH₃NH₃PbI₃ perovskite solar cells increases from 17.3% to 19.5%; the external quantum efficiency of CsPbI₃ perovskite quantum dot LEDs increases from 4.8% to 10.3%; and that of CdSe/ZnS quantum dot LEDs increases from 8.1% to 21.9%. As CD films are easily fabricated in air by solution processing, the approach paves the way to a simplified manufacturing of large‐area and low‐cost optoelectronic devices.

A new nonfullerene acceptor (TOBDT) with asymmetrical side chains is rationally designed and reported. Compared to the PM6:TOBDT binary devices, the as‐cast ternary devices based on PM6:IDIC:TOBDT obtain improved J _sc, V _oc, and fill factor values simultaneously, leading to a high power conversion efficiency of 14.0%, which is among the best reported for as‐cast fullerene‐free ternary devices.

Abstract

A new small‐molecule nonfullerene acceptor based on the benzo[1,2‐b:4,5‐b′]dithiophene (BDT) fused central core with asymmetrical alkoxy and thienyl side chains, namely TOBDT, is designed and synthesized. The alkoxy unit helps narrow the bandgap, and thienyl side chain helps enhance the intermolecular interaction. As a result, TOBDT is suitable to match the deep‐lying highest occupied molecular orbital (HOMO) of polymer donor PM6. Then, a strong crystalline acceptor IDIC is introduced as the third component to fabricate as‐cast nonfullerene ternary devices to achieve absorption and morphology control. Addition of IDIC not only mixes well with TOBDT but modulates the morphology of the blend film, which helps to balance the charge transport properties and reduce the photovoltage loss of ternary devices. All these contribute to synergetic improvement of J _sc, V _oc, and fill factor parameters, leading to a power conversion efficiency of 14.0% for the as‐cast fullerene‐free ternary device.

A series of novel Ruddlesden–Popper perovskite films of (PBA_{1− x} BA _x )₂MA₃Pb₄I₁₃ are successfully designed and fabricated to reveal the interplay of binary organic spacers on the precursor chemistry, film morphology, crystal orientation, trap states, and charge transport to obtain highly efficient solar cells, providing an effective design strategy to further develop stable and efficient perovskite materials and devices.

Abstract

Ruddlesden–Popper perovskite (RPP) materials have attracted great attention due to their superior stability, where the organic spacer dominantly determines the stability and efficiency of RPP solar cells, but research still lacks the systematical understanding of the interplay of binary spacer in the overall mixture range of 0–100% in RPPs on the precursor chemistry, film quality, and carrier behavior. Herein, a series of novel binary spacer RPP films of (PBA_{1− x} BA _x )₂MA₃Pb₄I₁₃ (BA = n‐butylammonium, PBA = 4‐phenylbutan‐1‐aminium, and MA = methylammonium) is successfully fabricated to reveal the interplay of binary spacers. The incorporation of 50% BA into the (PBA)₂MA₃Pb₄I₁₃ precursor solution increases the colloidal size and reduces nucleation sites, and therefore forms a very smooth film with much larger crystal grains and a higher degree of crystal preferential orientation, resulting in a significant reduction of trap states. The resulting combination of fast electron transfer and efficient electron extraction facilitates to effectively suppress the trap‐assisted charge recombination and remarkably decrease charge recombination losses. Consequently, the (PBA_0.5BA_0.5)₂MA₃Pb₄I₁₃ device achieves a champion efficiency of 16.0%, among the highest reported efficiencies for RPP devices. Furthermore, this device demonstrates good ambient, illumination, and thermal stabilities, retaining 60–93% of its initial efficiency after 30 days of various ageing.

The significant improvement of photovoltaic performances by synergetic effects of GeI₂ and methylammonium chloride (MACl) is described. The improved solubility of GeI₂ with the help of MACl in the precursor leads to high performance perovskite solar cells.

Abstract

Interfacial engineering, grain boundary, and surface passivation in organic–inorganic hybrid perovskite solar cells (HyPSCs) are effective in achieving high performance and enhanced durability. Organic additives and inorganic doping are generally used to chemically modify the surface contacting charge transport layers, and/or grain boundaries so as to reduce the defect density. Here, a simple but tricky one‐step method to dope organic–inorganic hybrid perovskite with Ge for the first time is reported. Unlike Ge doping to all‐inorganic perovskites, application of GeI₂ in organic–inorganic perovskite precursors is challenging due to the extremely poor solubility of GeI₂ in hybrid perovskite ink, leading to failure in the formation of uniform films. However, it is found that addition of methylammonium chloride (MACl) into the precursor remarkably increases the solubility of GeI₂. This MACl‐assisted Ge doping of hybrid perovskites produces high‐quality crystalline film with its surface passivated with nonvolatile GeI₂ (GeO₂) and the volatile MACl additive also improves the uniformity of GeO₂ distribution in the perovskite films. The resulting Ge‐doped mixed cation and mixed halide perovskite films with composition FA_0.83MA_0.17Ge_0.03Pb_0.97(I_0.9Br_0.1)₃ show superior photoluminescence lifetime, power conversion efficiency above 22%, and greater stability toward illumination and humidity, outperforming photovoltaic properties of HyPSCs prepared without the Ge doping.

A proper vertical phase separation and purer phases of donor and acceptor are finely controlled by sequential blade‐casting strategy in the PTB7‐Th:FOIC‐based organic solar cell, resulting in simultaneous enhancement of efficiency, stability, and mechanical properties.

Abstract

As a predominant fabrication method of organic solar cells (OSCs), casting of a bulk heterojunction (BHJ) structure presents overwhelming advantages for achieving higher power conversion efficiency (PCE). However, long‐term stability and mechanical strength are significantly crucial to realize large‐area and flexible devices. Here, controlling blend film morphology is considered as an effective way toward co‐optimizing device performance, stability, and mechanical properties. A PCE of 12.27% for a P‐i‐N‐structured OSC processed by sequential blade casting (SBC) is reported. The device not only outperforms the as‐cast BHJ devices (11.01%), but also shows impressive stability and mechanical properties. The authors corroborate such enhancements with improved vertical phase separation and purer phases toward more efficient transport and collection of charges. Moreover, adaptation of SBC strategy here will result in thermodynamically favorable nanostructures toward more stable film morphology, and thus improving the stability and mechanical properties of the devices. Such co‐optimization of OSCs will pave ways toward realizing the highly efficient, large‐area, flexible devices for future endeavors.

A novel in‐situ tin(II) complex antisolvent process is employed to simultaneously form quasi‐core–shell structure and heterojunction in mixed Pb–Sn low‐bandgap perovskite solar cells. This quasi‐core–shell structure offers effective grain boundary trap passivation and the heterostructure significantly improves the carrier extraction, leading to highly improved electrical property and stability.

Abstract

Unlike Pb‐based perovskites, it is still a challenge for realizing the targets of high performance and stability in mixed Pb–Sn perovskite solar cells owing to grain boundary traps and chemical changes in the perovskites. In this work, proposed is the approach of in‐situ tin(II) inorganic complex antisolvent process for specifically tuning the perovskite nucleation and crystal growth process. Interestingly, uniquely formed is the quasi‐core–shell structure of Pb–Sn perovskite–tin(II) complex as well as heterojunction perovskite structure at the same time for achieving the targets. The core–shell structure of Pb–Sn perovskite crystals covered by a tin(II) complex at the grain boundaries effectively passivates the trap states and suppresses the nonradiative recombination, leading to longer carrier lifetime. Equally important, the perovskite heterostructure is intentionally formed at the perovskite top region for enhancing the carrier extraction. As a result, the mixed Pb–Sn low‐bandgap perovskite device achieves a high power conversion efficiency up to 19.03% with fill factor over 0.8, which is among the highest fill factor in high‐performance Pb–Sn perovskite solar cells. Remarkably, the device fail time under continuous light illumination is extended by over 18.5‐folds from 30 to 560 h, benefitting from the protection of the quasi‐core–shell structure.

Two hydroxyl‐functionalized nonfullerene acceptors, IT‐OH and IT‐DOH, are synthesized, showing improved molecular arrangements and crystallinity compared to the parent ITIC molecule. This is attributed to intermolecular hydrogen bonds elongating conjugated planes and thus leading to long‐range‐ordered structures via π–π stacking. A best efficiency of 12.5% is achieved from the IT‐DOH‐based nonannealed solar cell with good device stability.

Abstract

Various substituents have been incorporated into nonfullerene acceptors (NFAs) to modulate absorption scopes and energy levels for boosting efficiencies of organic solar cells (OSCs). The manipulation of the NFAs' molecular order and crystallinity via those substitutions is equally crucial to OSC performances, which yet remains interesting and challenging. The hydroxyl group, which can potentially form strong intermolecular hydrogen bonds (H‐bonds) for improving molecular arrangements, has, however, never been considered. Herein, two hydroxyl‐functionalized NFAs, IT‐OH with one hydroxyl and IT‐DOH with two hydroxyls, are synthesized to tune the molecular packing and crystallinity. The ordered molecular arrangement and higher crystallinity are observed for the IT‐OH and IT‐DOH than the parent ITIC. This is assigned to the formation of intermolecular H‐bonds induced by the hydroxyls, which elongates molecular conjugated planes leading to long‐range‐ordered structures via π–π stacking. By the appropriate crystallinity and miscibility with donor polymer, an IT‐DOH‐based nonannealed OSC affords an efficiency of 12.5% with good device stability. This work provides a promising strategy to tune the molecular packing and crystallinity to design NFAs by introducing hydroxyl groups.

Interfaces provide reactive zones and interphases stabilize electronic device operation. Understanding and designing interfaces and interphases represent an effective and efficient way for developing high‐performance rechargeable batteries and perovskite solar cells.

Abstract

The ever‐increasing demand for clean sustainable energy has driven tremendous worldwide investment in the design and exploration of new active materials for energy conversion and energy‐storage devices. Tailoring the surfaces of and interfaces between different materials is one of the surest and best studied paths to enable high‐energy‐density batteries and high‐efficiency solar cells. Metal‐halide perovskite solar cells (PSCs) are one of the most promising photovoltaic materials due to their unprecedented development, with their record power conversion efficiency (PCE) rocketing beyond 25% in less than 10 years. Such progress is achieved largely through the control of crystallinity and surface/interface defects. Rechargeable batteries (RBs) reversibly convert electrical and chemical potential energy through redox reactions at the interfaces between the electrodes and electrolyte. The (electro)chemical and optoelectronic compatibility between active components are essential design considerations to optimize power conversion and energy storage performance. A focused discussion and critical analysis on the formation and functions of the interfaces and interphases of the active materials in these devices is provided, and prospective strategies used to overcome current challenges are described. These strategies revolve around manipulating the chemical compositions, defects, stability, and passivation of the various interfaces of RBs and PSCs.

Semi‐transparent perovskite solar cells (ST‐PSCs) have received great attention due to their promising applications in many areas, such as building integrated photovoltaics (BIPV), tandem devices, and wearable electronics. A general overview of recent advances in ST‐PSCs from materials and devices to applications is provided, and presented alongside some personal perspectives on their future development.

Abstract

Semitransparent solar cells (ST‐SCs) have received great attention due to their promising application in many areas, such as building integrated photovoltaics (BIPVs), tandem devices, and wearable electronics. In the past decade, perovskite solar cells (PSCs) have revolutionized the field of photovoltaics (PVs) with their high efficiencies and facile preparation processes. Due to their large absorption coefficient and bandgap tunability, perovskites offer new opportunities to ST‐SCs. Here, a general overview is provided on the recent advances in ST‐PSCs from materials and devices to applications and some personal perspectives on the future development of ST‐PSCs.

Integrated perovskite/bulk‐heterojunction (BHJ) organic solar cells have shown great potential to further improve their performance by combining the advantages of perovskite solar cells and near‐infrared (NIR) BHJ organic solar cells. Combining with the maintained high V _OC, higher efficiencies are expected by fully optimizing the perovskite layers and NIR BHJ layers through device engineering and materials innovations.

Abstract

The recently emerged integrated perovskite/bulk‐heterojunction (BHJ) organic solar cells (IPOSCs) without any recombination layers have generated wide attention. This type of device structure can take the advantages of tandem cells using both perovskite solar and near‐infrared (NIR) BHJ organic solar materials for wide‐range sunlight absorption and the simple fabrication of single junction cells, as the low bandgap BHJ layer can provide additional light harvesting in the NIR region and the high open‐circuit voltage can be maintained at the same time. This progress report highlights the recent developments in such IPOSCs and the possible challenges ahead. In addition, the recent development of perovskite solar cells and NIR organic solar cells is also covered to fully underline the importance and potential of IPOSCs.

The efficiency of photocurrent generation is studied in the high‐efficiency nonfullerene PM6:Y6 blend, using a combination of field‐ and temperature‐dependent optoelectronic measurements. These experiments reveal barrierless free charge generation, despite a small driving force. Theoretical modeling suggests the existence of a large electrostatic interfacial field, which pushes charges away from the donor–acceptor interface.

Abstract

Organic solar cells are currently experiencing a second golden age thanks to the development of novel non‐fullerene acceptors (NFAs). Surprisingly, some of these blends exhibit high efficiencies despite a low energy offset at the heterojunction. Herein, free charge generation in the high‐performance blend of the donor polymer PM6 with the NFA Y6 is thoroughly investigated as a function of internal field, temperature and excitation energy. Results show that photocurrent generation is essentially barrierless with near‐unity efficiency, regardless of excitation energy. Efficient charge separation is maintained over a wide temperature range, down to 100 K, despite the small driving force for charge generation. Studies on a blend with a low concentration of the NFA, measurements of the energetic disorder, and theoretical modeling suggest that CT state dissociation is assisted by the electrostatic interfacial field which for Y6 is large enough to compensate the Coulomb dissociation barrier.

Through a strategy of embedding cyclohexane‐1,4‐dione into the thieno[3,4‐b]thiophene unit, a highly electron‐deficient core (TTDO) is synthesized, and the corresponding donor polymer (PBTT‐F) is also developed. The nonfullerene photovoltaic device based on this new donor polymer exhibits an outstanding PCE of 16.1% with a very high fill factor of 77.1%, which demonstrates it a very promising donor for high‐performance solar cells.

Abstract

It is of great significance to develop efficient donor polymers during the rapid development of acceptor materials for nonfullerene bulk‐heterojunction (BHJ) polymer solar cells. Herein, a new donor polymer, named PBTT‐F, based on a strongly electron‐deficient core (5,7‐dibromo‐2,3‐bis(2‐ethylhexyl)benzo[1,2‐b:4,5‐c′]dithiophene‐4,8‐dione, TTDO), is developed through the design of cyclohexane‐1,4‐dione embedded into a thieno[3,4‐b]thiophene (TT) unit. When blended with the acceptor Y6, the PBTT‐F‐based photovoltaic device exhibits an outstanding power conversion efficiency (PCE) of 16.1% with a very high fill factor (FF) of 77.1%. This polymer also shows high efficiency for a thick‐film device, with a PCE of ≈14.2% being realized for an active layer thickness of 190 nm. In addition, the PBTT‐F‐based polymer solar cells also show good stability after storage for ≈700 h in a glove box, with a high PCE of ≈14.8%, which obviously shows that this kind of polymer is very promising for future commercial applications. This work provides a unique strategy for the molecular synthesis of donor polymers, and these results demonstrate that PBTT‐F is a very promising donor polymer for use in polymer solar cells, providing an alternative choice for a variety of fullerene‐free acceptor materials for the research community.

Nature Energy, Published online: 28 January 2020; doi:10.1038/s41560-020-0564-2