Abstract Modulating the surface charge transport behavior of hole transport materials (HTMs) would be as an potential approach to improve their hole mobility, while yet realized for fabricating efficient photovoltaic devices. Here, an oxygen bridged dimer‐based monoamine Fe III porphyrin supramolecule is prepared and doped in HTM film. Theoretical analyses reveal that the polaron distributed on dimer can be coupled with the parallel arranged polarons on adjacent dimers. This polaron coupling at the interface of supramolecule and HTM can resonates with hole flux to increase hole transport efficiency. Mobility tests reveal that the hole mobility of doped HTM film is improved by 8‐fold. Doped perovskite device exhibits an increased efficiency from 19.8 % to 23.2 %, and greatly improved stability. This work provides a new strategy to improve the mobility of HTMs by surface carrier modulation, therefore fabricating efficient photovoltaic devices. 

Porphyrin Supramolecule as Surface Carrier Modulator Imparts Hole Transporter with Enhanced Mobility for Perovskite Photovoltaics.

Porphyrin Supramolecule as Surface Carrier Modulator Imparts Hole Transporter with Enhanced Mobility for Perovskite Photovoltaics

Numerous defects exist at the buried interface between the perovskite and adjacent electron transport layers in perovskite solar cells, resulting in severe non-radiative recombination and excessive open-circuit voltage (VOC) loss. Herein, a dual defect passivation strategy utilizing guanidine sulfate (GUA2SO4) as an interface modifier is first reported. On the one hand, the SO4 2- preferentially interacts with Pb-related defects, generating water-insoluble lead oxysalts complexes. Additionally, GUA+ diffuses into the perovskite and induces the formation of low-dimensional perovskite. These reactions effectively suppress trap states at the buried interface and perovskite boundaries in printable mesoscopic perovskite solar cells (p-MPSCs), thus increasing the carrier lifetime. Meanwhile, GUA2SO4 optimizes the interface energy band alignment, thus accelerating the charge extraction and transfer at the buried interface. This synergistic effect of trap passivation and interface energy band alignment modulation is strongly demonstrated by an increase in average VOC of 70 mV and the power conversion efficiency improvement from 17.51% to 18.70%. This work provides a novel approach to efficiently improve the performance of p-MPSCs through dual-targeted defect passivation at the buried interface.

Dual Defect Passivation at the Buried Interface for Printable Mesoscopic Perovskite Solar Cells with Reduced Open-Circuit Voltage Loss.

Interface in perovskite solar cells (PSCs) is of vital importance because it dominates deep‐level defects and non‐radiative recombination, thus impacting both efficiency and stability further. Herein, a symmetrical acceptor–donor–acceptor (A–D–A) conjugated molecule with the core architecture of terthieno[3,2‐b hiophene and 2‐(3‐oxo‐2,3‐dihydro‐1 H‐inden‐1‐ylidene)malononitrile, named 6TIC, as a versatile buffer layer, is adopted to enhance photovoltaic performance and stability simultaneously. It is found that the conjugated molecule filling at grain boundaries and surface can not only chemically anchor with perovskite components to substantially eliminate interfacial defects and suppress detestable non‐radiative recombination, but also effectively improve the energy level alignment and facilitate charge transfer efficiency at the interface, resulting in an excellent power conversion efficiency of 24.81% with an admirable fill factor of 84.5%. Furthermore, benefiting from the unexceptionable surface protection effect of the hydrophobic buffer layer, greatly improved operational stability is delivered, with retaining 90% of initial efficiency for 960 h aging in a relative humidity of 60 ± 5% air and 1450 h aging under continuous 85 °C heating stress. This strategy may provide a new avenue for advancing high‐efficiency and stable PSCs.

An Acceptor–Donor–Acceptor Molecule Tailored Versatile Buffer Enabling Efficient and Stable Perovskite Solar Cells

Calix[n]arenes, a promising family of macrocyclic ligands, have been widely employed in the construction of polynuclear metal clusters. However, their utilization in titanium-oxo clusters (TOCs) is rare, especially in the...

Calix[6]arene-Functionalized Titanium-oxo clusters for Photocatalytic Cycloaddition of Carbon Dioxide to Epoxides

Typical wide-band gap cathode interlayer materials are difficulty in reducing interface recombination without limiting charge transport in perovskite solar cells (PSCs). Here, a lead-doped titanium-oxo cluster protected by S-containing ligands is introduced at the interface of perovskite and SnO2 . By in situ heating, the cluster is transformed into PbSO4 -PbTi3 O7 heterostructure. The oxygen atoms from sulfate ion in heterostructure connect with iodine from perovskite to boost interfacial electron extraction and reduce charge recombination. While the yielded metallic interface between PbSO4 and PbTi3 O7 promotes the electron transport across the interface. Finally, an efficiency as high as 24.2 % for the modified PSC is obtained. The heterostructure well-stabilize the interface of perovskite and SnO2 , to greatly improve the device stability. This work provides a novel strategy to prepare wide-band gap cathode interlayer by directional transformation of heterometallic oxo clusters. 

Directional Transformation of Heterometallic Oxo Clusters: A New Approach to Prepare Wide‐Bandgap Cathode Interlayers for Perovskite Solar Cells

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Directional Transformation of Heterometallic Oxo Clusters: A New Approach to Prepare Wide‐Bandgap Cathode Interlayers for Perovskite Solar Cells