Publication date: 11th March 2026
Buried perovskite interfaces critically dictate nucleation kinetics, crystallisation pathways, and interfacial energetics, while both buried and top interfaces govern defect chemistry, nonradiative recombination, and charge-transport dynamics, collectively limiting device efficiency and stability. Here, we report an in situ dual-interface engineering strategy enabled by a single multifunctional molecular additive, maleimido propionic acid hydrazide hydrochloride (MPAH.HCl), incorporated directly into the perovskite precursor. During film formation, MPAH.HCl undergoes spontaneous bidirectional segregation, wherein Cl⁻ anions preferentially migrate toward and accumulate at the buried interface, while MPAH⁺ cations enrich at the top surface. At the buried contact, interfacial Cl⁻ ions promote regulated crystallisation, enlarged grain growth, deep-trap passivation, and favourable modulation of interfacial energy alignment. Simultaneously, surface-segregated MPAH⁺ cations selectively passivate dominant vacancy (VI, VPb) and antisite (PbI, IPb) defects at the top perovskite interface. This synergistic dual-interface regulation substantially suppresses nonradiative recombination and enables more efficient charge extraction and transport. As a result, inverted perovskite solar cells achieve a markedly enhanced fill factor of 86.6% (from 80.6%), delivering a power conversion efficiency of 26.10% for small-area devices and 24.28% for 1 cm² devices. Furthermore, improved crystallinity and stabilised interfacial chemistry yield significantly enhanced operational stability under ambient storage, continuous illumination, and thermal stress. This work establishes bidirectional additive segregation as an effective design paradigm for simultaneously optimising buried and top perovskite interfaces toward high-efficiency, stable perovskite photovoltaics.
DST/TSG/PT/2009/23, DST/TMD/IC-MAP/2K20/03, and DST/CRG/2019/002164, Deity, India, no. 5(9)/2012-NANO (Vol. II), Max-Planck-Gesellschaft IGSTC/MPG/PG(PKI)/ 2011A/48 and MHRD, India, through SPARC project SPARC/2018-2019/P1097/SL, ANRF/ECRG/2024/000912/CS.
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