Bimolecular Passivation‐Dipole Bridge for Highly Efficient Inverted Perovskite Solar Cells with Low Nonradiative Recombination Loss

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Abstract Constructing charge‐selective heterointerface with minimized defect state and matched energy level alignment is essential to reduce nonradiative recombination for achieving high‐performance perovskite solar cells (PSCs). Herein, a bimolecular passivation‐dipole bridge comprised of sodium phenylmethanesulfonate (SPM) and 2‐phenylethylammonium iodide (PEAI) is carefully developed to regulate perovskite heterointerface. SPM passivates defect states and upshifts Fermi level ( E F ) of perovskite surface, and subsequent PEAI further induces additional negative dipole and causes the surface E F of perovskite pinning to negative polaron transport state of electron transport layer PCBM, which significantly promotes electron extraction at the perovskite electron‐selective contact. These advantages are confirmed by a remarkably improved efficiency from 21.74% for control to 25.12% for treated PSC with excellent stability. Moreover, corresponding nonradiative recombination loss impressively diminishes from 123 to 70 meV, and charge transport‐induced fill factor loss is only 3.00%. This work provides a promising approach via passivation‐energetic synergy for engineering perovskite heterointerface toward highly efficient and stable PSCs.

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