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Perovskite solar cells (PSCs) have demonstrated a high power conversion efficiency, however, the large energy loss due to non‐radiative recombination is the main challenge for further performance enhancement. Here, a surface treatment strategy is developed by heat‐induced decomposition of a thin interlayer 2,7‐Naphthaleneditriflate (NAP) to in situ reconstruct perovskite energetics. It is verified that the reconstructed perovskite surface energetics match better with the upper hole transport layer compared to the intrinsic condition. Spontaneous generation of n/n− homojunctions between the perovskite film bulk and the surface region promotes hole extraction, enhancing built‐in electric field, and thus significantly suppresses charge recombination at such perovskite hole‐selective heterojunctions. Moreover, the surface decomposed fluorine‐rich complexes passivate the defects and improve the crystallinity of the perovskite film. These advantages are confirmed by a remarkably improved efficiency from 20.52% for the control device to 23.37% for the treated one with excellent stability. The work provides a promising approach of in situ reconstructing perovskite surface and interface for the design of highly efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) suffer from significant nonradiative recombination at perovskite/charge transport layer heterojunction, seriously limiting their power conversion efficiencies. Herein, solution‐processed chromium multioxide (CrOx) is judiciously selected to construct a MAPbI3/CrOx/Spiro‐OMeTAD hole‐selective heterojunction. It is demonstrated that the inserted CrOx not only effectively reduces defect sites via redox shuttle at perovskite contact, but also decreases valence band maximum (VBM)‐HOMO offset between perovskite and Spiro‐OMeTAD. This will diminish thermionic losses for collecting holes and thus promote charge transport across the heterojunction, suppressing both defect‐assisted recombination and interface carrier recombination. As a result, a remarkable improvement of 21.21% efficiency with excellent device stability is achieved compared to 18.46% of the control device, which is among the highest efficiencies for polycrystalline MAPbI3 based n–i–p planar PSCs reported to date. These findings of this work provide new insights into novel charge‐selective heterojunctions for further enhancing efficiency and stability of PSCs. [ABSTRACT FROM AUTHOR]

Record power conversion efficiencies (PCEs) of perovskite solar cells (PSCs) have been obtained with the organic hole transporter 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl-amine)9,9′-spirobifluorene (spiro-OMeTAD). Conventional doping of spiro-OMeTAD with hygroscopic lithium salts and volatile 4-tert-butylpyridine is a time-consuming process and also leads to poor device stability. We developed a new doping strategy for spiro-OMeTAD that avoids post-oxidation by using stable organic radicals as the dopant and ionic salts as the doping modulator (referred to as ion-modulated radical doping). We achieved PCEs of >25% and much-improved device stability under harsh conditions. The radicals provide hole polarons that instantly increase the conductivity and work function (WF), and ionic salts further modulate the WF by affecting the energetics of the hole polarons. This organic semiconductor doping strategy, which decouples conductivity and WF tunability, could inspire further optimization in other optoelectronic devices. [ABSTRACT FROM AUTHOR]

Defect passivation via additive and energetic modification via interface engineering are two effective strategies for achieving high‐performance perovskite solar cells (PSCs). Here, the synergies of pentafluorophenyl acrylate when used as additive, in which it not only passivates surface defect states but also simultaneously modifies the energetics at the perovskite/Spiro‐OMeTAD interface to promote charge transport, are shown. The additive‐induced synergy effect significantly suppresses both defect‐assisted recombination and interface carrier recombination, resulting in a device efficiency of 22.42% and an open‐circuit voltage of 1.193 V with excellent device stability. The two photovoltaic parameters are among the highest values for polycrystalline CsFormamidinium/Methylammonium (FAMA)/FAMA based n‐i‐p structural PSCs using low‐cost silver electrodes reported to date. The findings provide a promising approach by choosing the dual functional additive to enhance efficiency and stability of PSCs. [ABSTRACT FROM AUTHOR]

Defect passivation via additive and energetic modification via interface engineering are two effective strategies for achieving high‐performance perovskite solar cells (PSCs). Here, the synergies of pentafluorophenyl acrylate when used as additive, in which it not only passivates surface defect states but also simultaneously modifies the energetics at the perovskite/Spiro‐OMeTAD interface to promote charge transport, are shown. The additive‐induced synergy effect significantly suppresses both defect‐assisted recombination and interface carrier recombination, resulting in a device efficiency of 22.42% and an open‐circuit voltage of 1.193 V with excellent device stability. The two photovoltaic parameters are among the highest values for polycrystalline CsFormamidinium/Methylammonium (FAMA)/FAMA based n‐i‐p structural PSCs using low‐cost silver electrodes reported to date. The findings provide a promising approach by choosing the dual functional additive to enhance efficiency and stability of PSCs. [ABSTRACT FROM AUTHOR]

The demonstration of an efficient nanostructure that provides acceptable photoelectrochemical water splitting properties using the sun visible radiation is an appealing issue. In this connection, a new ternary nanocomposite of Ag 2 S/MoS 2 /ZnO photoanode is subsequently fabricated via hydrothermal, solvothermal and SILAR methods. Different properties of the nanocomposite are characterized by XRD, SEM, EDX, XPS, UV–Vis-IR spectroscopy and electrochemical techniques. The post-grown annealed 8-Ag 2 S/MoS 2 /ZnO photoanode exhibits a good performance with a photocurrent density of 2 mA/cm2 at a bias potential 1.23 V vs. RHE. The photocurrent of the post-grown annealed 8-Ag 2 S/MoS 2 /ZnO photoanode is 71.42 times, 40 times and 2 times higher compares to the pure ZnO, post-grown annealed MoS 2 /ZnO, and post-grown annealed 8-Ag 2 S/ZnO photoanodes, respectively. The enhanced PEC performance may originate from the combination of different effects such as the expansion of light absorption and energy band alignment (type II heterostructures), [SO 4 ] acted as a charge-transfer medium, and electrode-electrolyte interface kinetic reactions. [Display omitted] • Ag 2 S/MoS 2 /ZnO ternary nanocomposite was successfully synthesized in three steps. • This ternary photoanode greatly improved the photocurrent of the PEC water splitting. • Ag 2 S components are utilized as light-absorption sensitizers. • The sacrificial reagent electrolyte is used to study the reactions. [ABSTRACT FROM AUTHOR]

[Display omitted] • The hybrid HTL consists of MoS 2 nanosheets and a PEDOT derivative, which results in an obvious improvement in organic solar cells' performance. • We identified that the synergy of exfoliated-MoS 2 nanosheets and DA-P result in better hole transport and extraction through systematic investigations. • By applying a comprehensive range of spectroscopies, we discovered that the dopant is derived from the oxidation products of MoS 2 nanosheets during ultrasonic exfoliation. We report an efficient hole transporting layer (HTL) for organic solar cell (OSC) based on solution-processed organic-inorganic hybrid composed of ultrasonic-exfoliated MoS 2 nanosheets and dopamine-copolymerized poly(3,4-ethylenedioxythiophene) (PEDOT) derivative (DA-P). The OSCs based on this new hybrid HTL show a marked performance improvement over those with single-component HTLs, and they retain up to 80% of their original power conversion efficiency after 35 days. Our investigations reveal that the boost in performance is due to a synergistic effect that improves both hole transport and extraction ability. This effect is mainly due to the doping of exfoliated-MoS 2 nanosheets on DA-P. We employ a comprehensive range of spectroscopies to uncover that the dopant is derived from the oxidation products of MoS 2 nanosheets during the ultrasonic exfoliation. Our work demonstrates an efficient hybrid HTL and offers new insights into the interaction of exfoliated-MoS 2 nanosheets and the PEDOT derivatives. [ABSTRACT FROM AUTHOR]