Publication date: 11th March 2026
Wide-bandgap (WBG) perovskites have attracted massive research interest for indoor and tandem photovoltaic applications. Although promising, large voltage deficits due to severe defect-assisted non-radiative recombination and misaligned energetic configuration between functional layers limit their acquisition of high efficiency.[1] These challenges are not effectively mitigated until the advent of self-assembled monolayer (SAM) molecules that can modulate the energy levels of the underlying hole-selective layers via a dipole effect and passivate the buried perovskite interfaces through their versatile functional moieties. Transcending the traditional scope of SAMs as interfacial modifiers, we herein propose an interface-bulk co-embedding (IBCE) technology that enables SAMs to simultaneously act on the buried interface and grain boundary of WBG perovskite films. Cross-sectional Kelvin probe force microscopy characterization reveals a unique p-type doping feature within the perovskite layer, originating from the electron-withdrawing effect of semi-penetrating SAMs distributed at grain-boundaries, which extends the depletion regions and reinforces its built-in potential. The IBCE strategy is also demonstrated to regulate crystallization kinetics, suppressing deep-level defects throughout the heterojunction and internal framework, and improve carrier transport and transfer dynamics. Meanwhile, Indene-C60 bisadduct, ICBA, is strategically employed to cater to the upward-shifted conduction band of perovskites. Consequently, a record-breaking VOC of 1.394 V (corresponding to a voltage loss of 0.376 V) and a champion PCE of 21.69% are achieved in 1.77 eV perovskite solar cells under AM 1.5G. Moreover, indoor photovoltaic performance realizes an efficiency of 42.07% with a maximum indoor VOC of ~ 1.2 V under 1000 lux warm LED illumination. Device simulation further confirms that the induced gradient p-type transition in WBG perovskites substantially broadens the quasi-Fermi level splitting throughout the entire device, leading to a solid physical basis for the significant enhancement of VOC and efficiency.
This work is supported by the Research Grants Council Hong Kong, China (Project No. 15306822) and the research Centre for Organic Electronics of the Hong Kong Polytechnic University, Hong Kong, China (1-CE0P).
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